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Nanomaterials 12 (21): 3905 (2022)
University of British Columbia. Nanomaterials and Polymer Nanocomposites Laboratory
Mousavi, Seyyed Mojtaba
Hashemi, Seyyed Alireza
Yari Kalashgrani, Masoomeh
Kurniawan, Darwin
Gholami, Ahmad
Chiang, Wei-Hung
The exponential increase in global energy demand in daily life prompts us to search for a bioresource for energy production and storage. Therefore, in developing countries with large populations, there is a need for alternative energy resources to compensate for the energy deficit in an environmentally friendly way and to be independent in their energy demands. The objective of this review article is to compile and evaluate the progress in the development of quantum dots (QDs) for energy generation and storage. Therefore, this article discusses the energy scenario by presenting the basic concepts and advances of various solar cells, providing an overview of energy storage systems (supercapacitors and batteries), and highlighting the research progress to date and future opportunities. This exploratory study will examine the systematic and sequential advances in all three generations of solar cells, namely perovskite solar cells, dye-sensitized solar cells, Si cells, and thin-film solar cells. The discussion will focus on the development of novel QDs that are economical, efficient, and stable. In addition, the current status of high-performance devices for each technology will be discussed in detail. Finally, the prospects, opportunities for improvement, and future trends in the development of cost-effective and efficient QDs for solar cells and storage from biological resources will be highlighted.
Citation: Mousavi, S.M.; Hashemi,S.A.; Yari Kalashgrani, M.;Kurniawan, D.; Gholami, A.; Chiang,W.-H. Bioresource-FunctionalizedQuantum Dots for EnergyGeneration and Storage: RecentAdvances and Feature Perspective.Nanomaterials 2022, 12, 3905. https://doi.org/10.3390/nano12213905Academic Editor: Hideya KawasakiReceived: 14 August 2022Accepted: 3 November 2022Published: 5 November 2022Publisher’s Note: MDPI stays neutralwith regard to jurisdictional claims inpublished maps and institutional affil-iations.Copyright: © 2022 by the authors.Licensee MDPI, Basel, Switzerland.This article is an open access articledistributed under the terms andconditions of the Creative CommonsAttribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).nanomaterialsReviewBioresource-Functionalized Quantum Dots for EnergyGeneration and Storage: Recent Advances andFeature PerspectiveSeyyed Mojtaba Mousavi 1 , Seyyed Alireza Hashemi 2, Masoomeh Yari Kalashgrani 3 , Darwin Kurniawan 1 ,Ahmad Gholami 3,* and Wei-Hung Chiang 1,*1 Department of Chemical Engineering, National Taiwan University of Science and Technology,Taipei City 106335, Taiwan2 Nanomaterials and Polymer Nanocomposites Laboratory, School of Engineering, University of BritishColumbia, Kelowna, BC V1V 1V7, Canada3 Biotechnology Research Center, Shiraz University of Medical Science, Shiraz 71468-64685, Iran* Correspondence: gholami@sums.ac.ir (A.G.); whchiang@mail.ntust.edu.tw (W.-H.C.)Abstract: The exponential increase in global energy demand in daily life prompts us to search fora bioresource for energy production and storage. Therefore, in developing countries with largepopulations, there is a need for alternative energy resources to compensate for the energy deficit inan environmentally friendly way and to be independent in their energy demands. The objective ofthis review article is to compile and evaluate the progress in the development of quantum dots (QDs)for energy generation and storage. Therefore, this article discusses the energy scenario by presentingthe basic concepts and advances of various solar cells, providing an overview of energy storagesystems (supercapacitors and batteries), and highlighting the research progress to date and futureopportunities. This exploratory study will examine the systematic and sequential advances in allthree generations of solar cells, namely perovskite solar cells, dye-sensitized solar cells, Si cells, andthin-film solar cells. The discussion will focus on the development of novel QDs that are economical,efficient, and stable. In addition, the current status of high-performance devices for each technologywill be discussed in detail. Finally, the prospects, opportunities for improvement, and future trendsin the development of cost-effective and efficient QDs for solar cells and storage from biologicalresources will be highlighted.Keywords: bioresource; quantum dots; energy generation; energy storage1. IntroductionIn the coming years, as fossil fuel consumption increases, so will energy demand. Thisproblem puts a lot of pressure on renewable energy sources. At the same time, the reduc-tion in renewable energy sources leads to environmental pollution, reduction in naturalresources, and global warming [1–3]. Therefore, it is necessary to develop new methodsof energy generation and storage for the times when they are needed. Lithium batteriesand supercapacitors will be among the energy storage devices of the future [4–7]. In recentdecades, a new type of capacitor, supercapacitors/microcapacitors (SCs/MSCs), has beendeveloped. Supercapacitors are among the energy storage devices used in a variety ofapplications, such as hybrid vehicles, personal electronic devices, digital telecommunica-tion systems, energy storage in conjunction with other energy systems, such as solar cells,backup power in computers, and in the electrical industry [8–10]. One way to optimizethe properties of energy storage systems is to develop new materials for use as electrodematerials in supercapacitors, batteries, and solar cells [11–14]. Quantum materials, such ascarbon quantum dots (CQDs) and graphene quantum dots (GQDs), play an important rolein supercapacitors, batteries, and solar cells due to their good electrical conductivity, lowNanomaterials 2022, 12, 3905. https://doi.org/10.3390/nano12213905 https://www.mdpi.com/journal/nanomaterialsNanomaterials 2022, 12, 3905 2 of 28cost and availability, biocompatibility, and good chemical stability, and one of the latestmethods is to obtain QDs from bioresources. Another important feature of CQDs/GQDs forsolar cell applications is their excellent photoreaction [15–19]. Due to the synthesis of GQDsby micro-organisms, such as bacteria [20], fungi, and yeasts [21], they are a very suitableoption for the development of the next generations of electronic and optical components,fuel cells, solar cells, lithium batteries, and bioresources [22–24]. It is worth noting thatresearch on quantum dots from biological sources for energy generation and storage islimited. Therefore, we tried to study a large part of the applications of quantum dots inenergy generation and storage, the applications of biological resources in energy genera-tion and storage separately, and a combination of quantum dots derived from biologicalresources in energy generation and storage. This review article will enable researchersto use quantum dots from biological sources for energy-related applications in the nearfuture. Therefore, this review provides an overview of recent progress and prospectsfor the characterization of bioresource-derived QDs for energy generation and storage.The synthesis of QDs using bioresources, e.g., micro-organisms, such as fungi, bacteria,and yeasts, is being extensively studied. This review shows the versatile applications ofQDs derived from biological sources for energy generation and storage, which are verypromising, such as supercapacitors/microcapacitors, batteries, and solar cells (perovskitesolar cells and organic and inorganic hybrid solar cells).2. Bioresource-Derived QDsBioresources include both plant and animal materials, and each of these materials can beconverted into renewable energy through the use of bioresources. In general, bioresourcescan be divided into three types: micromolecules derived from bioresources (e.g., citric acidand glucose), components of bioresources (e.g., cellulose, hemicellulose, lignin, etc.), andnatural bioresources (e.g., straw and crab shells) [25]. Various types of bioresources can beused as carbon sources in QDs, e.g., waste streams. In addition, products that do not fallinto the category of waste streams can also be used as carbon sources. Waste bioresources,such as leaves or food waste, are considered the most environmentally friendly, facilitatewaste management, and are often less expensive. Although these bioresources cannot beconsidered waste, they are still environmentally friendly because they do not contribute towaste management. However, they are less environmentally friendly than those whosewaste they can dispose of. Compared to waste bioresources, this type of bioresource isoften more expensive, but can be better purified, so its synthesis can be simplified. In thissection, we will describe the advantages of using bioresources to produce quantum dotswith minimal environmental impact. In terms of their photoluminescence (PL) emission,optical properties, excellent conductivity, and broad spectral absorption, these dots sharesome similarities with chemical QDs, especially in terms of their chemical stability andbroad optical absorption spectrum. Their properties include nonblinking, resistance tophotobleaching, broad excitation wavelengths, and the ability to tune synthesis parameters,including size, shape, composition, internal structure, and surface chemistry, to emit ata specific wavelength [26,27]. These materials are not only more environmentally friendly,but they are also potentially less toxic and biocompatible.3. Synthesis of Bioresource-Derived QDsSynthesis for obtaining QDs from bioresources with good electronic and optical prop-erties is possible by a variety of precursors and methods. The properties, advantages,and disadvantages of each method are listed in Table 1. In addition to these methods,microwave hydrothermal, oxidation, solvent thermal, and reflux methods are less commonsynthesis methods. Chemical oxidation is one of the least colorful methods because strongacids are used to quantify the quantum resource, while the bioresource extraction methodwithout heat or chemicals is one of the most environmentally friendly methods. The lackof control over the properties of the extracted points is one of the major drawbacks of theNanomaterials 2022, 12, 3905 3 of 28extraction method. From the analysis, microwave and hydrothermal methods are widelyused for QD synthesis [28–31].Table 1. The properties, advantages, and disadvantages of each method.Method Advantages Disadvantages Properties Ref.microwavemost effective and leasttime-consuming methods;high efficiency andhomogeneous heatingpoor control over size,microwave radiation isharmful to human beingscasein dots had high QY of18.7% and size of 7 nm [32–36]hydrothermal simple to operate,controllable and nontoxicpoor control over size andpresence of impurities.papaya carbon sourceproduced blue colored CDswith a 2−6 nm size and QY of18.98%; peach extractproduced blue nitrogen dopedwith particle size of 8 nm anda QY of 15%[37–42]ultrasonic synthesisprocess is simple, easy tocontrol, and promotescrystal structurestransformations of the dots,poor size control, and a longreaction timefood waste dots showed a highdegree of solubility in water,a narrow band of PL emission(400−470 nm), a size of 4 nmand excellent photostability[43–46]chemical oxidationvery hydrophilic andvariable emission, andeffective and facilemethod suitable for largescale; process is easilymodified, and surfacestate is tunableharsh chemical may be usedand biotoxicity of theproducts is increasedbiowaste synthesized dots hadan average particle size of5−6 nm and the QY < 2%[47–49]3.1. Hydrothermal MethodThe hydrothermal method is one of the most popular methods for producing QDsquickly, cheaply, conveniently, and in an environmentally friendly manner, producingquantum dots at a high rate under aqueous conditions of high temperature and pressure.There are a number of reasons why this method is so popular, including ease of use,control, nontoxicity, and the fact that the polymer does not need to be passivated beforeuse. Nevertheless, this method does not allow for precise control of size, and impuritiesmay already be present at the time of the process [37–42].A 2016 paper by Wang et al. reported that the authors developed a new environmen-tally friendly method for hydrothermal carbonization of papaya to synthesize CDs.Papaya was heated at 200 ◦C for 5 h, filtered, and dialyzed for 72 h, after whichan extraction procedure was carried out at 2–6 nm with a high quantum yield of 18.3%.The result was a blue CD PL with a size of 2–6 nm and a quantum yield of 18.3%. Theresearchers performed a series of experiments to show that the dots were suitable forimaging HeLa cells as well as for measuring the fluorescence of E. coli bacterial strains.However, it should be emphasized that no percentage yield was reported in the otherresearch cited; therefore, it is impossible to draw a conclusion as to whether or not thisreaction is effective with further magnification [38].3.2. Microwave SynthesisIn microwave synthesis, it is possible to quantify organic substances using microwavesto produce QDs. The yield and quality of quantum dots increase with a short heatingtime, as this increases the quantum yield. It has the added advantage of being veryefficient, saving time, and distributing heat evenly. However, it is also characterized bypoor size control and microwave radiation, which can be harmful to human health ona large scale [32–36].Bajpai et al. used milk powder containing casein as a carbon source in their study.A microwave oven can be used to heat a casein solution until it becomes semisolid, so thata semisolid solution is formed by the heating process. The residue from this process isNanomaterials 2022, 12, 3905 4 of 28then diluted with distilled water and centrifuged to remove all residues. The supernatantis collected and analyzed. The environmental friendliness and the fact that no harshchemicals are used in this process make it an ideal alternative for those who want to protectthe environment. Only a few steps are required to complete the process. Since this methoddoes not use waste biomass to make the synthesis, but instead buys the biomass to makeit in a lab, it is less environmentally friendly than the others. To determine if the caseinpoints described in the paper are more economical than those created from dairy waste,both the casein points described in the paper and those created from dairy waste must becompared. To determine whether casein points are more economically advantageous, thecasein points described in the paper must be compared. Note that these points have a highyield of 18.7%, which means they fall in the blue range [32].4. Limiting Factors of Using Bioresources for the Synthesis of Quantum DotsThere are a limited number of applications for QDs compared to SCQDs due to theirlow quantum yield [50]. Quantum yields between 40% and 90% [51] can be achievedwith SCQDs, while QDs usually achieve quantum yields of 30%. According to Yang et al.,microwaves were used to generate quantum dots using resorcinol, OPD, and hydrochloricacid, and a quantum yield of 62.8% was achieved. This was because the QDs had beendoped with nitrogen, so there were many nitrogen atoms in the QDs. In addition, the dotscontained few vacancies in the carbon skeleton, and the core consisted mainly of the sp2domain. It was found that the reaction was positively affected by the presence of HClas a “promoter”, resulting in bright fluorescence and a high yield of reaction products.Consequently, if this method is applied to waste biomass instead of chemical feedstockas a power plant raw material, it might be possible to reduce the ecological impact of itsuse [52].5. Modification of QDs with BioresourceBioresources can be defined as organically produced raw materials that have beencreated by the activities of humans and animals and can, therefore, be used as natural,renewable resources that are derived from the material itself. Bioresources can be laboratoryanimals, plants, cells, genes, and micro-organisms used for research [53]. In additionto agricultural waste, carbonaceous solid waste is also a bioresource. There are variousmethods to dispose of agricultural wastes that are continuously generated from agriculturalactivities. Various industries, including mills, can use this waste as a fuel source forheating, power generation, and chemical processes. From these wastes, various industries,such as mills, can generate electricity, heat, and chemicals. GQDs derived from plantleaves do not require oxidizing or reducing agents or organic solvents, and the structuresof these bioresources contain various functional groups [54]. Bioresources are used forvarious purposes and applications, as shown by agroforestry and aquaculture. The useof important bioresources for energy production is problematic due to the ineffectivenessof GQD. Synthesis received much attention due to their low cost, availability, and highcarbon content as potential feedstocks for the synthesis of GQDs. Functionalization ofGQDs, even when they are in pure form, occurs because of the constraints on their use.Functionalization is achieved either by forming composites with polymers [55], inorganicmaterials [56], organic molecules [57], etc., or through doping with heteroatoms [58]. Thefunctionalized GQDs have enormous applications, such as drug delivery, bioimaging,batteries, sensors, etc. [59–61]. Recently, the synthesis of QDs from various bioresources hasbeen influenced by the development of green and sustainable chemistry [62–64]. This ismainly because conventional synthesis methods involve lengthy synthesis processes underextreme temperature and pressure conditions. In addition, these synthesis methods usetoxic reagents and require extensive purification procedures. In the synthesis of QDs, theuse of bioresources led to inexpensive and simple methods. Therefore, the present studyfocuses on the synthesis of QDs from various bioresources, including micro-organisms,such as bacteria, fungi, yeast, and algae [62,65–67].Nanomaterials 2022, 12, 3905 5 of 285.1. Microorganisms Derived QDsAs properties, such as biocompatibility, environmental friendliness, and feasibility, areconsidered in the implementation of synthesis methods, it is possible to propose the synthe-sis of QDs via biological pathways that are environmentally friendly, inexpensive, and lowin toxicity, rather than using chemical synthesis methods for QDs. Micro-organisms are alsoexcellent biological nanofactories for the synthesis of QDs. The biosynthesis of QDs hasseveral major advantages that can be exploited, especially in energy production and storage.Micro-organisms have tremendous diversity, which gives them an inherent potential tomediate QDs. Bacteria, yeasts, and fungi are among the micro-organisms suggested tosynthesize QDs. This is due to various factors, such as pH and temperature, their abilityto grow under stressful environmental conditions, and their ease of cultivation [68,69].Due to their high tolerance and self-compatibility in environments containing toxic metals,micro-organisms have the unique ability to promote QD synthesis by utilizing energyproduction and storage [70,71]. Microbial enzymes play a key role in the conversion ofprecursor metal ions into nanoparticles. Various biological sources are used for the biosyn-thesis of QDs, such as viruses [72], bacteria [73], fungi [74], agricultural and industrialwastes [75], plant extracts [76], and algae [77]. Figure 1 shows micro-organisms such asbacteria, fungi, yeasts, and algae that produce QD. Currently, the biological productionof QDs by micro-organisms, such as yeasts, bacteria, and fungi, has attracted particularattention due to their ability to bioaccumulate and biotransform QDs, as shown in Table 2.The synthesis of QDs by fungi was also given attention because they were effective secretorsof various biomolecules among the micro-organisms studied. The advantages of usingfungi also include their cost-effectiveness and ease of biomass processing. However, thesynthesis of QDs by bacteria offers advantages, since bacteria can be genetically engineeredto express specific enzymes involved in the synthesis of QDs [78,79].Nanomaterials 2022, 12, 3905 6 of 29 Carboxylated graphene quantum dots (CGQDs) Concentrations E. coli [88] CdTe–Rocephin QD complex - E. coli [89] CQDs - E. coli [90] CdS pH Acidithiobacillus ferrooxidans, A. thiooxidans and A. caldus [91] GQDs-M - Shewan lla decolorati nis S12 [92] CdSe - Pseudomonas aeruginosa [93] MoS2 - E. coli, S. aureus [94] CdTe - E. coli [95] Yeast CdS - Saccharomyces cerevisiae [96] CdSe Different concentrations of Na2SeO3 and CdCl2 and pH Rhodotorula m cilaginosa [97] GQDs Do e-depe dent S. cerevisiae and H9c2 c ll line [98] CdSe Effect of S. cerevisiae growth phase, sele-nite concentration, cadmium concentra-tion, effects of sele ite and cadmium incu-bating time S. cerevisiae [99] CQDs - Saccharomyces cerevisiae [100,101] ZnS Reaction time and different concentrations of yeast biomass and ZnSO4 S. cerevisiae MTCC 2918 [102] Figure 1. Micro-organisms derived QDs, such as bacteria, fungi, yeast, and algae. 5.1.1. Bacteria Bacteria have great potential in energy-related fields because they can be produced on a large scale, have a diverse morphology, are biomineralizable, have unique electro-chemical activity, and are inexpensive. In addition, they are considered to be the most widely distributed living organisms and provide the largest contribution to the material Figure 1. icro-organisms derived QDs, such as bacteria, fungi, yeast, and algae.Nanomaterials 2022, 12, 3905 6 of 28Table 2. List of micro-organisms (bacteria, yeast, and fungi) through the production of QD andvarious types of microbial QDs.QDs Optimization of Factors Microorganisms Ref.FungiZnS - Penicillium sp. [80]CdTe - Fusarium oxysporum [81]CQD Concentration P. chrysogenum [82]CdS Reaction time F. oxysporum f. sp. lycopersici [83]PbSe - Aspergillus terreus [84]MoS2 Concentration Trichoderma viride [85]ZnS Reaction time, temperature, pH Aspergillus sp. [86]BacteriaCdS CdSO4 concentration,temperature, time and pH P. chlororaphis CHR05 [87]Carboxylated graphene quantumdots (CGQDs) Concentrations E. coli [88]CdTe–Rocephin QD complex - E. coli [89]CQDs - E. coli [90]CdS pH Acidithiobacillus ferrooxidans,A. thiooxidans and A. caldus [91]GQDs-M - Shewanella decolorationis S12 [92]CdSe - Pseudomonas aeruginosa [93]MoS2 - E. coli, S. aureus [94]CdTe - E. coli [95]YeastCdS - Saccharomyces cerevisiae [96]CdSe Different concentrations ofNa2SeO3 and CdCl2 and pHRhodotorula mucilaginosa [97]GQDs Dose-dependent S. cerevisiae and H9c2 cell line [98]CdSeEffect of S. cerevisiae growthphase, selenite concentration,cadmium concentration, effectsof selenite and cadmiumincubating timeS. cerevisiae [99]CQDs - Saccharomyces cerevisiae [100,101]ZnSReaction time and differentconcentrations of yeast biomassand ZnSO4S. cerevisiae MTCC 2918 [102]5.1.1. BacteriaBacteria have great potential in energy-related fields because they can be produced ona large scale, have a diverse morphology, are biomineralizable, have unique electrochemicalactivity, and are inexpensive. In addition, they are considered to be the most widelydistributed living organisms and provide the largest contribution to the material cycle inthe natural environment [103–105]. Economic production, stability, water solubility, anda stable structure are among the advantages of using bacteria for the biosynthesis of QDscompared to conventional methods. Another advantage of using bacteria for biosynthesisis the relatively low cytotoxicity of QDs. For the production of QDs of uniform size withpotential antibacterial properties, the use of bacteria is suitable as an environmentallyfriendly, cost-effective, and simple method. The QDs prepared using bacteria showedexcellent salt stability due to the morphological changes in the QDs caused by the bacteria.There is no doubt that QDs offer many exciting and indispensable prospects in the field ofNanomaterials 2022, 12, 3905 7 of 28energy conversion. This is due to their diverse and strong physicochemical properties andadvantageous features, such as quantum confinement effects and an abundance of surfacedefects. Doping with different heteroatoms cannot only enhance the electronic conductivity,but also introduce multiple active sites, increase the number of defects, and improve thechemical adsorption ability, which can improve the reaction activities and electrochemicalkinetics in energy storage and conversion devices [10,106,107]. The bioinspired synthesisof ZnS QDs from Aspergillus sp. was investigated by Jacob et al. The results showedthat biogenic ZnS QDs exhibited significant antimicrobial activity comparable to that ofstandard antibiotics after screening their antibacterial activity against common pathogenicbacteria. Factors responsible for the excellent bioactivity include the ability of ZnS QDs todisrupt the bacterial cell membrane, oxidative damage caused by ROS leading to bacterialcell lysis, and leakage of cytoplasmic contents (Figure 2) [108]. Table 3 shows the propertiesof QDs and the characterization tools for QDs biosynthesized from bacteria.Nanomaterials 2022, 12, 3905 7 of 29 cycle in the natural environment [103–105]. Economic production, stability, water solubil-ity, and a stable structure are among the advantages of using bacteria for the biosynthesis of QDs compared to conventional methods. Another advantage of using bacteria for bio-synthesis is the relatively low cytotoxicity of QDs. For the production of QDs of uniform size with potential antibacterial properties, the use of bacteria is suitable as an environ-mentally friendly, cost-effective, and simple method. The QDs prepared using bacteria showed excellent salt stability due to the morphological changes in the QDs caused by the bacteria. There is no doubt that QDs offer many exciting and indispensable prospects in the field of energy conversion. This is due to their diverse and strong physicochemical properties and advantageous features, such as quantum confinement effects and an abun-dance of surface defects. Doping with different heteroatoms cannot only enhance the elec-tronic conductivity, but also introduce multiple active sites, increase the number of de-fects, and improve the chemical adsorption ability, which can improve the reaction activ-ities and electrochemical kinetics in energy storage and conversion devices [10,106,107]. The bioinspired synthesis of ZnS QDs from Aspergillus sp. was investigated by Jacob et al. The results showed that biogenic ZnS QDs exhibited significant antimicrobial activity comparable to that of standard antibiotics after screening their antibacterial activity against common pathogenic bacteria. Factors responsible for the excellent bioactivity in-clude the ability of ZnS QDs to disrupt the bacterial cell membrane, oxidative damage caused by ROS leading to bacterial cell lysis, and leakage of cytoplasmic contents (Figure 2) [108]. Table 3 shows the properties of QDs and the characterization tools for QDs bio-synthesized from bacteria. Figure 2. Cytotoxic effect of ZnS QDs on bacterial cells. Reprinted with permission from Ref. [108]. Copyright 2019 Elsevier. Table 3. Characteristics of QDs and the characterization tools of QDs biosynthesized from bacte-ria. QDs Organism Characterization Tools Characteristics of QDs Ref. Size Shape CdS CdS/CdSe E. coli UV-vis, DLS, HR-STEM, TEM, EDX, FTIR, and fluorescence spectroscopy 12 nm 17 nm Spherical Spherical [109] Graphene E. coli AFM, HRTEM, UVvis absorption, FT-IR, XPS 3–8 nm - [110] ZnS Clostridiaceae sp. XRD, EDX, TEM, FTIR, PL and UV 3.34 ± 0.65 nm Spherical [111] Figure 2. Cytotoxic e fect of ZnS QDs on bacterial ce ls. Reprinted with permi sion from Ref. [108].Copyright 2019 Elsevier.Table 3. Characteristics of QDs and the characterization tools of QDs biosynthesized from bacteria.QDs Organism Characterization ToolsCharacteristics of QDsRef.Size ShapeCdSCdS/CdSe E. coliUV-vis, DLS, HR-STEM,TEM, EDX, FTIR, andfluorescence spectroscopy12 nm17 nmSphericalSpherical [109]Graphene E. coli AFM, HRTEM, UVvis absorption,FT-IR, XPS 3–8 nm - [110]ZnS Clostridiaceae sp. XRD, EDX, TEM, FTIR, PL and UV 3.34 ± 0.65 nm Spherical [111]Zn/rifampicin/Tf MycobacteriumsmegmatisUV/Vis-spectroscopy, TEM, FTIR,photoluminescence, XRD, XPSand NMR10 nm Spherical [112]CdTe E. coliRaman, mass spectrometry,absorption,and fluorescence spectroscopy andfluorescence microscopy- - [113]Ag/In/S Candida albicans TEM, XRD, UV-Vis 9.5–10 nm Spherical [114]CdSe Providencia vermicola UV-vis, FTIR XRD, TEM, and EDX 2–4 nm Cubic [115]ZnO E. coli X-ray, FTIR, MIC 3–7 nm Spherical [116]CdS Pseudomonas fragiDSL, AFM, TEM, XRD, XPS, UV-visand fluorescence emissionspectroscopy2–16 nm Spherical [117]Nanomaterials 2022, 12, 3905 8 of 285.1.2. FungiHeterotrophic micro-organisms with a nucleus and a cell wall are called fungi. Inrecent decades, fungi have attracted much attention in energy−related fields due totheir high production, diversity, and rapid reproduction [118,119]. Fungi include micro-organisms, such as yeasts [120], and multicellular organisms, such as molds [121,122].Since nano−dimensional particles with better monodispersity can be obtained by usingfungi, fungal-mediated synthesis is more advantageous than bacterial synthesis. Therefore,the use of fungi is one of the most stable and effective methods for the synthesis of CdSQDs with high biocompatibility and excellent optical properties for the generation andstorage of light. The use of fungi in the preparation of QDs also increases their fluorescenceproperties. In addition, the production of QDs with fungi has increased photocatalyticactivity, which has led to greater degradation of pollutants and the degradation of biosen-sors used in the generation and storage of energy. Fungi and QDs can demonstrate theirpotential in energy-related fields, such as supercapacitors, lithium-ion batteries, and solarcells [123,124]. A fundamental mechanistic aspect of the biosynthesis of QDs from fungiwas investigated by Jacob et al. As shown in Figure 3, the possible mechanism of biosyn-thesis of PbSe QDs from Aspergillus tereus was revealed by them. Detoxification of metalsby biological molecules occurs through a series of events, such as the induction of highcirculation of organic acids, the induction of proteins, and the stimulation of antioxidantenzymes, including the mechanism of fungal biosynthesis that emerged from their study.This process includes the following steps: (i) First, in the production medium of metalions (Pb2+ and Se2−), the precursors (Pb(NO3)2 and Na2SeSO3) undergo redox reactions.(ii) Detoxification is initiated by several processes: (a) reversible combination of levelfunctional groups (e.g., thiols, oxalic acids) with metal ions; (b) conversion of glutathioneto phytochelatins (PC) due to activation of phytochelatin synthase (PS) and also bindingwith metal ions, eventually leading to their transport by ATP-binding cassette membranetransfer proteins into the cell vacuole is due to metal stress; (c) binding of metallothioneinsto metal ions occurs in a similar manner; (d) redox reactions occur by tautomerization ofquinine; microscopic PbSe is formed by the activity of superoxide dismutase (SOD); and(f) stimulation of other oxidoreductases to generate a redox environment. (iii) The manu-facturing process of PbSe QDs occurs through the creation of a redox atmosphere and theinvolvement of glutathione/metallothionein. (iv) Thermal shock increases the permeabilityof the cell walls so that their contents are released into the environment. (v) Finally, nucleiform the QD−capped protein culture medium due to Ostwald maturation [125,126].5.1.3. YeastYeast is a unicellular fungus that belongs to the facultative anaerobes and can live inaerobic and anaerobic environments [118,127,128]. Yeast cell colonies are much thicker andlarger than bacteria [129–131]. In addition, yeasts are widely used in industry for energyproduction and storage. CdTe QDs are among the most important QDs considered forenergy storage applications due to their unique properties, which include high quantumefficiency, control, and narrow emission spectra. Bao et al. investigated CdTe QDs biosyn-thesized with yeast cells with tunable fluorescence emission spectra. They showed thesize-dependent emission spectra of the as-prepared CdTe QDs at 490–560 nm, as shown inFigure 4a. They also identified the dispersion of CdTe QDs with a diameter of 2.0–3.6 nm atTEM, as shown in Figure 4b. In the XRD pattern at 2θ ~ 26.7 ◦C, the diffraction peak of thebiosynthesized CdTe QDs is cubic and corresponds to the (200) reflection in Figure 4c. ByFTIR spectroscopy, it is possible to identify the possible ligands coating the fabricated CdTeQDs. Two absorption peaks corresponding to the amide I and II functional groups werefound at 1650 and 1566 cm−1, respectively, as shown in Figure 4d. The results show thatthe microbially prepared CdTe QDs exhibit exceptional biocompatibility and stability, andalso have a high quantum efficiency of ~33% [132].Nanomaterials 2022, 12, 3905 9 of 28Nanomaterials 2022, 12, 3905 9 of 29 Figure 3. Mechanistic pathway of PbSe QDs biosynthesis from fungus. Reprinted with permission from Ref. [125]. Copyright 2017 Elsevier. 5.1.3. Yeast Yeast is a unicellular fungus that belongs to the facultative anaerobes and can live in aerobic and anaerobic environments [118,127,128]. Yeast cell colonies are much thicker and larger than bacteria [129–131]. In addition, yeasts are widely used in industry for en-ergy production and storage. CdTe QDs are among the most important QDs considered for energy storage applications due to their unique properties, which include high quan-tum efficiency, control, and narrow emission spectra. Bao et al. investigated CdTe QDs biosynthesized with yeast cells with tunable fluorescence emission spectra. They showed the size-dependent emission spectra of the as-prepared CdTe QDs at 490–560 nm, as shown in Figure 4a. They also identified the dispersion of CdTe QDs with a diameter of 2.0–3.6 nm at TEM, as shown in Figure 4b. In the XRD pattern at 2θ ~ 26.7 °C, the diffrac-tion peak of the biosynthesized CdTe QDs is cubic and corresponds to the (200) reflection in Figure 4c. By FTIR spectroscopy, it is possible to identify the possible ligands coating the fabricated CdTe QDs. Two absorption peaks corresponding to the amide I and II func-tional groups were found at 1650 and 1566 cm−1, respectively, as shown in Figure 4d. The results show that the microbially prepared CdTe QDs exhibit exceptional biocompatibility and stability, and also have a high quantum efficiency of ~33% [132]. Figure 3. Mechanistic pathway of PbSe QDs biosynthesis from fungus. Repri ted with permissionfrom Ref. [125]. Copyright 2017 Elsevier.Nanomaterials 2022, 12, 3905 10 of 29 (a) (b) (c) (d) Figure 4. (a) Spectra of the biosynthesized CdTe QDs, which were taken from the reaction flask and centrifuged to remove the yeast cells after incubation at 35 °C in the open air for 1 day (black line), 2 days (red line), 4 days (green line), and 8 days (blue line). The inset in (a) is a photograph of the as-biosynthesized CdTe QDs under ambient room light. (b) TEM image (c) XRD pattern of the CdTe QDs extracellularly bio-grown with the yeast cells at 35 °C for 8 days (d) The FT–IR spectrum of the biosynthesized CdTe QDs incubated with yeast cells at 35 °C for 8 days. Reprinted from Ref. [132]. 5.1.4. Algae Recently, algal-mediated synthesis of QDs for various energy generation and storage applications has attracted attention due to its importance in the development of biocom-patible and highly fluorescent QDs. Since one of the environmental problems is caused by algal biomass, the use of algae for the biosynthesis of QDs helps not only as a bioresource for synthesis but also for environmental remediation. The results of using algae as precur-sors include the remarkable properties of QDs, including excellent blue luminescence in UV light, ionic strength, commendable stability, pH, exceptional insensitivity to photo-bleaching, and high-water dispersion. Another result of using algae is excellent light transmission. QDs synthesized by this method showed efficient optical absorption and fluorescence. The bioresource of microalgae is a sustainable, renewable, and abundant source that provides a cost-effective and easy way to synthesize CQDs for energy gener-ation and storage [133,134]. A mesoscopic solar cell system was developed using CQDs synthesized from Gelidium amansii powder, a species of red algae, to serve as light col-lectors. According to Dou et al., the CQDs were able to harvest light effectively. A mesoscopic TiO2 photoanode, in which CQDs containing the dye N719 were used, served as the photocell. The counter electrode, created from FTO glass with a Pt carrier, was used as the redox electrolyte for the solar cell. In addition, CQDs, N719, and TiO2 with a FTO glass support were used for the counter electrode (Figure 5a). Since the HOMO edge of the CQDs agrees well with the value of the N719 dye, and as evidenced by the redox potential of the I*/I3* system, extraction of holes from the N719 dye into the electrolyte occurs, leading to an improvement in the separation of electrons and holes (Figure 5b) [135]. Figure 4. (a) Spectra of the biosynthesized CdTe QDs, which were taken from the reaction flask andcentrifuged to remove the yeast cells after incubation at 35 ◦C in the open air for 1 day (black line),2 days (red line), 4 days (green line), and 8 days (blue line). The inset in (a) is a photograph of theas-biosynthesized CdTe QDs under ambient room light. (b) TEM image (c) XRD pattern of the CdTeQDs extracellularly bio-grown with the yeast cells at 35 ◦C for 8 days (d) The FT–IR spectrum of thebiosynthesized CdTe QDs incubated with yeast cells at 35 ◦C for 8 days. Reprinted from Ref. [132].Nanomaterials 2022, 12, 3905 10 of 285.1.4. AlgaeRecently, algal-mediated synthesis of QDs for various energy generation and storageapplications has attracted attention due to its importance in the development of biocompati-ble and highly fluorescent QDs. Since one of the environmental problems is caused by algalbiomass, the use of algae for the biosynthesis of QDs helps not only as a bioresource forsynthesis but also for environmental remediation. The results of using algae as precursorsinclude the remarkable properties of QDs, including excellent blue luminescence in UVlight, ionic strength, commendable stability, pH, exceptional insensitivity to photobleach-ing, and high-water dispersion. Another result of using algae is excellent light transmission.QDs synthesized by this method showed efficient optical absorption and fluorescence. Thebioresource of microalgae is a sustainable, renewable, and abundant source that providesa cost-effective and easy way to synthesize CQDs for energy generation and storage [133,134].A mesoscopic solar cell system was developed using CQDs synthesized from Gelidiumamansii powder, a species of red algae, to serve as light collectors. According to Dou et al.,the CQDs were able to harvest light effectively. A mesoscopic TiO2 photoanode, in whichCQDs containing the dye N719 were used, served as the photocell. The counter electrode,created from FTO glass with a Pt carrier, was used as the redox electrolyte for the solar cell.In addition, CQDs, N719, and TiO2 with a FTO glass support were used for the counterelectrode (Figure 5a). Since the HOMO edge of the CQDs agrees well with the value of theN719 dye, and as evidenced by the redox potential of the I*/I3* system, extraction of holesfrom the N719 dye into the electrolyte occurs, leading to an improvement in the separationof electrons and holes (Figure 5b) [135].Nanomaterials 2022, 12, 3905 11 of 29 Figure 5. (a) Schematic of solar cell structure with the help of CQDs as light harvester (b) charge transfer and energy level distribution of solar cell photoanode. Reprinted with permission from Ref. [135]. Copyright 2019 Elsevier. 5.2. Bio-Wastes Derived QDs Animals and plants engage in a variety of activities that result in the generation of biowaste, which can be divided into several categories. As a renewable energy resource, biowaste is converted into GQDs without the addition of chemicals [136]. Tade et al. con-verted industrial waste and biowaste into GQDs without adding chemicals. A study on carbonaceous bioprecursors, such as amino acids and carbohydrates, was carried out to understand their processes [137]. Based on the work of Mohan et al., it was found that the synthesis of GQDs can be successfully carried out using sugarcane bagasse (SB) as the feedstock for the process. This experiment was carried out at room temperature, and the starting material was carbonized during the experiment. To perform the synthesis of sug-arcane bagasse, 2 g of bagasse was mixed with 2 g of NaNO3 and 26 mL of H2SO4. This product was then mixed with 6 g KMnO4 and oxidized for 48 h with constant stirring. It was then mixed again with 6 g KMnO4. After the reaction was complete, I added 500 mL of distilled water and 5 mL of H2O2 to the mixture. The resulting sample was then diluted to ensure that no traces of acid remained in the sample [138]. 5.2.1. Lignin Lignin-based QDs materials are usually environmentally friendly and low cost, and are widely used in energy storage, the environment, electronic devices, and other fields [139,140]. It should be noted that lignin is attractive for the fabrication of CQDs due to its high graphene content and aromatic phenylpropane structure, which has the great ad-vantage of resembling the graphene framework of CQDs. To obtain very bright CQDs with stable fluorescence emission and water solubility, simple hydrothermal processing of LPC can also be used. Transmission electron microscopy (TEM) can be used to deter-mine the morphology of lignin-based CQDs (see Figure 6a). The TEM image also shows good dispersion of the quasi-spherical CQDs with no obvious aggregation. One of the reasons for the particles having a highly crystalline graphene structure is the presence of (100) graphitic carbon layers (0.21 nm lattice spacing) in the high-resolution TEM image, the TEM image shows stripes with a spacing of 0.21 nm [141]. The uniform distribution responsible for the photoluminescence and confinement of CQDs can be confirmed by the distribution of CQDs in the range of 2 to 9 nm with an average diameter of 4.18 nm (Figure 6b) [142]. Figure 6c shows the location of the strong absorption peak at approximately 265 nm in the sp2-hybridized graphene core, which is due to the π-π* transition of the conju-gated C=C/C=O bonds [143,144]. The color change of the lignin-based CQD solution under a UV lamp with a wavelength of 360 nm from pale yellow in natural light to light blue fluorescence is shown in the inset photograph in Figure 6c. Additionally, in Figure 6d, the Figure 5. (a) Schematic of solar cell structure with the h lp of CQDs as light harvester (b) chargetransfer and energy level istribution of solar cell photoanode. Reprinted with permission fromRef. [135]. Copyright 2019 Elsevier.5.2. Bio-Wastes Derived QDsAnimals and plants engage in a variety of activities that result in the generation ofbiowaste, which can be divided into several categories. As a renewable energy resource,biowaste is converted into GQDs without the addition of chemicals [136]. Tade et al.converted industrial waste and biowaste into GQDs without adding chemicals. A studyon carbonaceous bioprecursors, such as amino acids and carbohydrates, was carried outto understand their processes [137]. Based on the work of Mohan et al., it was found thatthe synthesis of GQDs can be successfully carried out using sugarcane bagasse (SB) asthe feedstock for the process. Thi experiment was carried out at ro m temperature, andthe starting material w s carbonized during the e periment. To perform the synthesis ofsugarcane bagasse, 2 g of bagasse was mixed with 2 g of NaNO3 and 26 mL of H2SO4. Thisproduct was then mixed with 6 g KMnO4 and oxidized for 48 h with constant stirring. Itwas then mixed again with 6 g KMnO4. After the reaction was complete, I added 500 mLof distilled water and 5 mL of H2O2 to the mixture. The resulting sample was then dilutedto ensure that no traces of acid remained in the sample [138].Nanomaterials 2022, 12, 3905 11 of 285.2.1. LigninLignin-based QDs materials are usually environmentally friendly and low cost, and arewidely used in energy storage, the environment, electronic devices, and other fields [139,140].It should be noted that lignin is attractive for the fabrication of CQDs due to its highgraphene content and aromatic phenylpropane structure, which has the great advantageof resembling the graphene framework of CQDs. To obtain very bright CQDs with stablefluorescence emission and water solubility, simple hydrothermal processing of LPC canalso be used. Transmission electron microscopy (TEM) can be used to determine themorphology of lignin-based CQDs (see Figure 6a). The TEM image also shows gooddispersion of the quasi-spherical CQDs with no obvious aggregation. One of the reasons forthe particles having a highly crystalline graphene structure is the presence of (100) graphiticcarbon layers (0.21 nm lattice spacing) in the high-resolution TEM image, the TEM imageshows stripes with a spacing of 0.21 nm [141]. The uniform distribution responsible forthe photoluminescence and confinement of CQDs can be confirmed by the distributionof CQDs in the range of 2 to 9 nm with an average diameter of 4.18 nm (Figure 6b) [142].Figure 6c shows the location of the strong absorption peak at approximately 265 nm inthe sp2-hybridized graphene core, which is due to the pi-pi* transition of the conjugatedC=C/C=O bonds [143,144]. The color change of the lignin-based CQD solution undera UV lamp with a wavelength of 360 nm from pale yellow in natural light to light bluefluorescence is shown in the inset photograph in Figure 6c. Additionally, in Figure 6d, thestrongest absorption of CQDs by PL excitation, which is similar to the documented PLexcitation analysis of carbon dots (Cdots), was shown in the range of 400–460 nm [144].The CQDs showed an excitation peak approximately 449 nm, which could be due to thegraphene core, surface structure and specific diameter [145].Nanomaterials 2022, 12, 3905 12 of 29 strongest absorption of CQDs by PL excitation, which is similar to the documented PL excitation analysis of carbon dots (Cdots), was shown in the range of 400–460 nm [144]. The CQDs howed an excitation peak approximately 449 nm, which could be due to the graphene core, surface structure and specific diameter [145]. Figure 6. Structural profile and performance of CQD assay from lignin. (a) TEM images (scale bar 50 nm), (b) high-resolution XPS spectra of graphene, particle size distribution, (c) UV-vis absorption spectrum, emission spectrum under maximum excitation at 360 nm, and excitation spectrum ob-served at maximum emission wavelength of 440 nm. Reprinted with permission from Ref. [146]. Copyright 2021 Elsevier. (d) UV–Vis and PL excitation (PLE) spectra of C dots. Reprinted with per-mission from Ref. [144]. Copyright 2019 Elsevier. 5.2.2. Wood Charcoal There are many methods of making charcoal, but the most common is to heat wood at 400 degrees Celsius in an oxygen-deficient environment, since charcoal is a pure form of carbon. Pyrolysis is a method of converting wood into charcoal and is one of the most effective methods. As an abundant, highly flammable energy source, charcoal, a carbona-ceous substance, is readily available in large quantities and is an abundant carbon source [147]. GQDs were synthesized in a two-electrode system by electrochemical oxidation of charcoal as described by Nirala et al. In this experiment, a solution of 0.01 M ammonium persulfate was used as electrolyte and an electrode potential of 5 volts was used for oxi-dation, with a current of 100–200 mA/cm2 during oxidation. The free rotation that occurs during the anodic oxidation of water and giant graphene sheets allowed the giant gra-phene sheets to be oxidized to GQDs. The assembly was centrifuged in a centrifuge at 10,000 rpm for 20 min. E-GQDs were also prepared by dialyzing a mixture for a period of three days before analysis [148]. 5.2.3. Coffee Grounds It has been observed that as coffee consumption has increased, so has the production of ground coffee, which is rich in carbohydrates, proteins, caffeine, tannins, and pectins, all of which have been shown to be important for human health. In addition to the primary (c) (a) (d) Figure 6. Structural profile and performance of CQD assay from lignin. (a) TEM imag s (scale bar50 nm), (b) high-resolution XPS spectra of graphene, particle size distribution, (c) UV-vis absorptionspectrum, emission spectrum under maximum excitation at 360 nm, and excitation spectrum observedat maximum emission wavelength of 440 nm. Reprinted with permission from Ref. [146]. Copyright2021 Elsevier. (d) UV–Vis and PL excitation (PLE) spectra of C dots. Reprinted with permission fromRef. [144]. Copyright 2019 Elsevier.Nanomaterials 2022, 12, 3905 12 of 285.2.2. Wood CharcoalThere are many methods of making charcoal, but the most common is to heat wood at400 degrees Celsius in an oxygen-deficient environment, since charcoal is a pure form ofcarbon. Pyrolysis is a method of converting wood into charcoal and is one of the most effec-tive methods. As an abundant, highly flammable energy source, charcoal, a carbonaceoussubstance, is readily available in large quantities and is an abundant carbon source [147].GQDs were synthesized in a two-electrode system by electrochemical oxidation of charcoalas described by Nirala et al. In this experiment, a solution of 0.01 M ammonium persulfatewas used as electrolyte and an electrode potential of 5 volts was used for oxidation, witha current of 100–200 mA/cm2 during oxidation. The free rotation that occurs during theanodic oxidation of water and giant graphene sheets allowed the giant graphene sheetsto be oxidized to GQDs. The assembly was centrifuged in a centrifuge at 10,000 rpm for20 min. E-GQDs were also prepared by dialyzing a mixture for a period of three daysbefore analysis [148].5.2.3. Coffee GroundsIt has been observed that as coffee consumption has increased, so has the productionof ground coffee, which is rich in carbohydrates, proteins, caffeine, tannins, and pectins, allof which have been shown to be important for human health. In addition to the primarycomposition of ground coffee, carbon is also a component of its primary composition.Carbon can be used in a variety of applications, such as wastewater treatment, biomedicalwaste treatment, and other industrial processes [149].Recently, a study was published by Wang et al. using coffee grounds to synthesizeGQDs. For this purpose, 0.1 g of highly sterile and dried coffee grounds was mixed withone ml of hydrazine hydrate. It was sonicated with 10 mL of water and 0.1 gram of coffeegrounds for 30 min. The mixture was then kept at 150–200 ◦C for approximately six–tenhours. After filtering off the solution containing the water-soluble GQDs, small moleculeswere removed from the solution by dialysis for two days. The quantum yield was reportedto be 33%. By using these GQDs for bioimaging, ion detection, and environmental analysis,we can produce blue fluorescent GQDs that emit blue fluorescence at 470 nm [150].6. Applications of Energy Generation and Storage Devices by Bioresource-Derived QDs6.1. Integrated Devices for Energy Harvesting and StorageIntegrated energy harvesting and storage devices, such as SCs/MSCs, lithium-ionbatteries (LIBs), and solar cells, play an important role in daily life because they can replaceconventional fossil fuel energy (Figure 7). Nevertheless, these isolated devices cannotprovide enough energy for long-term operation and constantly changing work situations,and have limited power and/or exclusive use. This shows that the development of goodautomated systems is necessary to meet the increasing energy demand for long-term usein different environmental scenarios. An effective way to achieve an energy system withhigh density, small size, and high reliability is to develop an integrated energy packageand a combination of energy harvesting and storage [151]. One of the most importantenergy-related technologies that can replace the battery or at least extend its lifetime isenergy harvesting and storage devices [152]. The use of toxic chemical reagents, hightemperatures, high time consumption, and synthetic steps are among the drawbacks ofmany traditional methods of bioresource-derived QD synthesis that limit the applicationof these syntheses. Therefore, recently, new bioresource-based methods, such as thoseusing micro-organisms (bacteria, fungi, and yeasts), lignin, and cellulose, are being used asgraphene sources for the synthesis of bioresource-derived QDs. Considering the severaladvantages of bioresource-derived QDs, including good recyclability, convenient synthe-sis, colorful PL, excellent biocompatibility, and low cost, scientists have been inspired todevelop novel materials with low environmental impact and new applications, such assupercapacitors/microsupercapacitors, batteries, and solar cells [153–155]. In recent years,properties, such as enhanced absorption of UV light, ease of functionalization, and im-Nanomaterials 2022, 12, 3905 13 of 28proved efficiency of solar cells have been used to improve the performance of solar cellswith QDs [156]. A QD is a type of nanoparticle that can be used as a mobile material toimprove the performance of batteries by introducing it into their electrolytes to improvetheir electrical properties [157].Nanomaterials 2022, 12, 3905 14 of 29 Figure 7. Applications of energy generation and storage devices by bioresource-derived QDs. 6.2. Supercapacitors/Microsupercapacitors SCs/MSCs as energy storage devices have attracted more attention due to their unique advantages, such as short charge/discharge times, small size, long lifetimes, and high-power densities. SCs/MSCs can be divided into two types of capacitors based on different charge storage mechanisms: quasi-capacitors and electrochemical double-layer capacitors. In general, SCs/MSCs with GQDs, whose mechanism is charge absorption at the electrode level as the electrode material, belong to the electrochemical double-layer type. Xue et al. investigated the electrochemical deposition of GQDs on a gold finger elec-trode. The results showed that the MSCs obtained after 5000 cycles have an operating speed of up to 1000 V/s, a specific capacitance of 534.7 mF/cm, and a specific capacitance of 97.8% compared to their initial specific capacitance [158]. A flexible, transparent MSC with highly bendable properties and a specific capacitance and high transmittance at 550 nm wavelength of 9.09 mF cm−2 and 92.97%, respectively, was developed by Lee et al. using chelated graphene and GQDs. It retains approximately 100% of its initial specific capacitance with respect to bending after 10,000 continuous cycles (long cycle stability can be maintained) [159]. Most lignin-based supercapacitors generally exhibit slow diffusion kinetics and lower electrochemical performance with low capacitance due to their low conductivity, uncontrolled morphology, and poor interfacial compatibility. Ding et al. in-vestigated the simultaneous rapid charging and increase in specific capacitance with GQDs and heterogeneous graphene sheets (GQD/Gr) prepared entirely from lignin. The in situ growth of GQDs on graphene is possible due to the conversion of lignin into GQDs and subsequent deposition on graphene, which provides good surface compatibility with GQD/Gr heterogeneity. They found that the GQD/Gr heterojunction has a high specific capacitance of 404.6 F g−1 and a short charge time constant (τ0) of 0.3 s, which is 2.5 times longer and 7.5 times faster than the unmodified lignin electrode with 162 and 2.3 s, re-spectively. The results show that it is possible to overcome the critical barriers for a lignin-based supercapacitor with superior electrochemical performance by creating a discontin-Figure 7. Applications of energy generation and storage devices by bioresource-derived QDs.6.2. Supercapacitors/MicrosupercapacitorsSCs/MSCs as energy storage devices have attracted more attention due to their uniqueadvantages, such as short charge/discharge times, small size, long lifetimes, and high-power de sities. SCs/MSCs can be divided into two types of capacit rs based on differentcharge storage mechanisms: quasi-capacitors and electrochemical double-layer capacitors.In gener l, SCs/MSCs wit GQD , whose mechani m is charge absorption at th elect odelevel as the lectrode material, belong to the electrochemical double-layer type. Xue et al.investigated the electrochemical deposition of GQDs on a gold finger electrode. Theresults showed that the MSCs obtained fter 5000 cycles have an operating sp ed ofup to 1000 V/ , a specific capacitance of 534.7 mF/cm, and a specific capacita ce of97.8% compared to their initial s ecific capacitance [158]. A flexible, transparent MSCwith highly bendabl properties and a specific capacitance and high transmittance at550 nm wavelength of 9.09 mF cm−2 and 92.97%, respectively, was developed by Lee et al.using chelated graphene and GQDs. It retains approximately 100% of its initial specificcapacit nce with r spect to bending after 10,000 c ntinuous cycles (long cycle stability canbe maintained) [159]. Most lignin-based supercapacitors generally exhibit slow diffusionkinetics and lower electrochemical performance with low capacitance due to their lowconductivity, uncontrolled mor hology, and poor interfacial compatibility. Ding et al.investigated the simultaneous rapid charging and increase in specific capacitance withGQDs and heterogeneous graphene sheets (GQD/Gr) prepared entirely from lignin. Thein situ growth of GQDs on graphene is possible due to the conversion of lignin intoGQDs and subsequent deposition on graphene, which provides good surface compatibilitywith GQD/Gr heterogeneity. They found that the GQD/Gr heterojunction has a highspecific capacitance of 404.6 F g−1 and a short charge time constant (τ0) of 0.3 s, which is2.5 times longer and 7.5 times faster than the unmodified lignin electrode with 162 andNanomaterials 2022, 12, 3905 14 of 282.3 s, respectively. The results show that it is possible to overcome the critical barriersfor a lignin-based supercapacitor with superior electrochemical performance by creatinga discontinuous 0D/2D GQD/Gr system. It also paves the way for the conversion of high-quality industrial lignin into highly efficient, scalable, and cost-effective electrochemicalenergy devices (Figure 8) [160]. The various features and functions of GQDs in MSCs andSCs are shown in Table 4.Nanomaterials 2022, 12, 3905 15 of 29 uous 0D/2D GQD/Gr system. It also paves the way for the conversion of high-quality in-dustrial lignin into highly efficient, scalable, and cost-effective electrochemical energy de-vices (Figure 8) [160]. The various features and functions of GQDs in MSCs and SCs are shown in Table 4. Figure 8. (a) Design of a 0D/2D GQD/Gr-converted all-lignin heterogeneous graft by a low-cost, facile, and scalable alkaline-activated hydrothermal method for high-speed, specially enhanced su-percapacitors. (b) Schematic illustration of more electron storage and efficient emission towards the GQD/Gr electrode through the GQD/Gr lignin electrode and alkali. Reprinted from Ref. [160]. Table 4. GQDs applied to MSCs and SCs. Electrode Substance Cycle Stability Electrolyte Operating Voltage (V) Ref. MSCs GQD//MnO2 - 0.5 M Na2SO4 1 [161] GQD//GQD 97.8%, 5000 cycles 0.5 M Na2SO4 1 [158] GQD//PANI 97.3%, 1500 cycles 0.5 M Na2SO4 0.9 [162] SCs GQD-3DG//GQD-3DG 90%, 5000 cycles 1 M H2SO4 0.8 [163] GEAC//GEAC 100%, 10,000 cycles Alkaline electrolyte 1 [164] CoDC-0.5//CoDC-0.5 90%, 10,000 cycles 6 M KOH 1 [165] 6.3. Batteries The use of LIB as a power source and in electric and hybrid vehicles as an intelligent energy storage system is becoming increasingly popular. Due to their lightweight design, cost-effectiveness, energy efficiency, and long life, the commercial demand for these bat-teries is increasing significantly. The charge-discharge process can rapidly degrade the capacity of many LIB electrode materials, but many of them also exhibit poor rate perfor-mance due to self-aggregation, uncontrolled volume expansion, dissolution, formation of solid electrolyte interfaces across the electrodes, and a rapid increase in charge transfer resistance during cycling [166–168]. Although electrode materials for LIBs are widely used, they have a number of drawbacks. These include the fact that the electrode materials (a) (b) Figure 8. (a) of a 0D/2D GQD/Gr-converted all- ignin heterogeneous graft by a low-cost,facile, and scalable alkaline-acti t er al method for high-speed, specially enhancedsupercapacitors. (b) Schemat c illustration of more electr d efficient emission towardsthe GQD/Gr electrode through the GQD/Gr lignin electrode and alkali. Repri Ref. [160].Table 4. GQDs applied to MSCs and SCs.Electrode Substance Cycle Stab lity Electrolyte Operating Volta e (V) Ref.MSCs GQD//MnO2 - 0.5 M Na2SO4 1 [161]GQD//GQD 97.8%, 5000 cycles 0.5 M Na2SO4 1 [158]GQD//PANI 97.3%, 1500 cycles 0.5 M Na2SO4 0.9 [162]SCsGQD-3DG//GQD-3DG 90%, 5000 cycles 1 M H2SO4 0.8 [163]GEAC//GEAC 100%, 10,000 cycles Alkaline electrolyte 1 [164]CoDC-0.5//CoDC-0.5 90%, 10,000 cycles 6 M KOH 1 [165]6.3. BatteriesThe use of LIB as a power source and in electric and hybrid vehicles as an intelligentenergy storage system is becoming increasingly popular. Due to their lightweight design,cost-effectiveness, energy efficiency, and long life, the commercial demand for these bat-Nanomaterials 2022, 12, 3905 15 of 28teries is increasing significantly. The charge-discharge process can rapidly degrade thecapacity of many LIB electrode materials, but many of them also exhibit poor rate perfor-mance due to self-aggregation, uncontrolled volume expansion, dissolution, formation ofsolid electrolyte interfaces across the electrodes, and a rapid increase in charge transferresistance during cycling [166–168]. Although electrode materials for LIBs are widely used,they have a number of drawbacks. These include the fact that the electrode materials arenot coulombically efficient, electrolyte depletion, and safety concerns. Recently, the useof QDs incorporated into LIB electrode materials has proliferated to address the issuesassociated with these materials. In order to improve the efficiency of the next generationof LIBs, changes are being made to the electrode materials in terms of surface finish andinternal structures. Compared to other types of electrode materials, QDs possess a numberof advantages, including increased conductivity, an increased number of active surfaces onthe electrodes, and improved electrode surfaces and wettability, all of which are importantaspects of electrode material performance. In addition, they could also help control thevolume expansion of electrode materials and control the voltage drop during chargingand discharging. In addition, anode materials with a large surface area, morphology, andhigh dimensional stability have also been explored as anode materials because they havea variety of properties that make them suitable for use in anode applications, such asgraphene and carbon nanotubes. By weakening the lattice disorder in these materials,they cannot only be strengthened but can be used more effectively as anodes in LIBs byenlarging the defects, improving the order in the lattice, and creating pores. Graphene andcarbon nanotubes (CNTs) accumulate defects over time as a result of interactions betweenvan der Waals forces and high surface energies. To understand the extent of the problemof accumulated defects over time, it is particularly important to understand how thesedefects accumulate over a short period of time. Due to the high conductivity of grapheneand carbon nanotubes, composites can be created that combine these highly conductivegraphene and carbon nanotubes by duplicating graphene and carbon nanotubes and thencombining them. The functional groups (-OH and COO-) on graphene quantum dots createa negative charge on the surface of the CNTs. This prevents the CNTs from clusteringtogether, as molecules with the same charge repel each other. In addition, these functional-ized CNTs improve the storage capacity of Li-ion batteries. The combined performanceof these hybrid graphenes and carbon nanotubes was greater than the performance of theindividual elements. The addition of these active sites and the reduction in mechanicalstress also led to an increase in the number of active sites. In addition, a reduction in me-chanical stress is also caused by the volume changes associated with the charge/dischargeprocesses [169–171].GQDs are used in lithium-ion batteries due to their unique structure and high con-ductivity, low density, high hardness, and high tensile strength [172–174]. The bioresource-derived GQDs improve the electrochemical performance in Li+ or Na+ batteries, increasethe electron transfer and Li+/Na+ diffusion rates, and decrease the volume expansion.Electrochemical performance can be improved by mixing bioresource-derived GQDs withan active material as an auxiliary material or by using bioresource-derived GQDs asan anode material. VOx is considered a promising electrode material for Li-ion batteriesbecause it offers high capacity, low cost, and abundant resources. They have fabricateda number of VOX nanostructures to use as LIB cathodes, and so far, we have been able toreport on their fabrication. Nevertheless, most of these materials tend to drop capacitancerapidly and perform poorly at high speeds, while resistance increases rapidly during cy-cling, suggesting that they are not suitable for use in extreme conditions [157,175]. A newLTO/N-GQD/superhierarchical anode material was investigated for LIB by Khan et al.The results showed that LTO with N-GQD not only has better electrical properties, but alsoincreases the specific capacitance by 23% compared to pure LTO (Li4Ti5O12); therefore, thedischarge capacity for more than 200 cycles is approximately 170 mAh·g−1 at 20 ◦C, asshown in Figure 9 [176].Nanomaterials 2022, 12, 3905 16 of 28Nanomaterials 2022, 12, 3905 17 of 29 Figure 9. The electrochemical performance of LTO-NGQ20 with rate capability from 0.2 °C to 50 °C and long cycling performance electrodes. Reprinted with permission from Ref. [176]. Copyright 2019 Elsevier. 6.4. Solar Cells A solar cell or photovoltaic cell is a solid-state electronic element that converts a por-tion of received solar energy directly into electricity. The operating mechanism of the solar cell is that by generating a photon and absorbing it, an electron-hole pair is created. By connecting two p-type and n-type semiconductors, electrons are transferred from the n-type region to the p-type region, and holes are transferred from the p-type region to the n-type region. The positive and negative ions created by the electron-hole transfer gener-ate an electric field that becomes stronger as more electrons and holes are transferred until the formal levels of the two regions equalize and an electric field is created. Upon solar irradiation and photon absorption (light packets whose energy is higher than the energy of the semiconductor gap), the generated electron-hole pair penetrates the electron donor-acceptor interface. Then the electron-hole pair is separated at the interface and generates electrons and holes. The electric field drives the electrons into the n-region and the holes into the p-region. In this way, a potential difference is created due to the negative charge density in the n-region and the positive charge density in the p-region. Then the charge transfer to the cathode and anode takes place. When the cathode and anode are connected with a wire, the excess electrons in the n-region migrate through the wire to the p-region, and a short-circuit current is generated. Figure 10a shows a schematic diagram of a solar cell. Nowadays, silicon solar cells are used on an experimental scale, but since the silicon wafers must have a high degree of purity, the manufacturing cost is very high, which makes it difficult to use this type of solar cell. Different types of polymers, pigments, and perovskite solar cells have been produced, which have reasonable energy conversion ef-ficiencies and lower weight and cost. A solar cell consists of three parts: photoanode, cath-ode (usually metals, such as aluminum, silver, and calcium), and active layer. Generally, indium oxide is used as a photoanode. This compound has a suitable bandgap, high trans-parency and electrical conductivity, and has a suitable working function. Due to the lim-ited indium sources, expensive fabrication methods, instability in acidic environments, and brittleness of electrodes, the attention of scientists has been drawn to the use of mate-rials with better performance, such as photoanodes or electrodes [177–180]. Bioresource-derived QDs have other advantages due to their special properties, such as lightweight and low density, high electrical conductivity (with zero bandgap and good mobility for electrons and holes), and flexibility, which include availability, affordability, sustainabil-ity, and an ecofriendly nature; they also have disadvantages, including scaling problems due to uneven heating and a wide size distribution of solar cells [181–183]. Since the mass production of bioresource-derived QDs, intensive research on bioresource-derived QDs Figure 9. The electrochemical performance of LTO-NGQ20 with rate capability from 0.2 ◦C to 50 ◦C andlong cycling performance electrodes. Reprinted with permission from Ref. [176]. Copyright 2019 Elsevier.6.4. Solar CellsA solar cell or photovoltaic cell is a solid-state electronic element that convertsa portion of received s lar energy direct y into electricity. The oper ing mech nismof the solar cell is that by genera ing a photon and abs rbing it, an electron-hole pair isreated. By connecting two p-type n-type semiconducto s, electrons are t ansferredfrom the n-type region to the p-ty e r gion, and h les are a sferred from th p-type regiono the n-type region. Th pos tive and negative ions created by the electron-hole transfergenerate an electric field that becomes stronger as more electrons and holes are transf rreduntil the formal levels of the two egions equaliz and an electric field is created. Uponsolar irradiation and phot n absorption (light packets whose energy is higher than theenergy of the semiconductor gap), the generat d electron-hole pair pen trates the elect ondonor-acceptor interface. Then the electron-hole pair is separated at th interface andgenerates electrons and holes. The electric field drives the electrons into the -region andthe holes into the p-region. In this way, a potential difference is created due to the negativecharge density in the n-region and the positive charge density in the p-region. Then thecharge transfer to the cathode and anode takes place. When the cathode and anode areconnected with a wire, the excess electrons in the n-region migrate through the wire to thep-region, and a short-circuit current is generated. Figure 10a shows a schematic diagramof a solar cell. Nowadays, silicon solar cells are used on an experimental scale, but sincethe silicon wafers must have a high degree of purity, the manufacturing cost is very high,which makes it difficult to use this type of solar cell. Different types of polymers, pigments,and perovskite solar cells have been produced, which have reasonable energy conversionefficiencies and lower weight and cost. A solar cell consists of three parts: photoanode,cathode (usually metals, such as aluminum, silver, and calcium), and active layer. Generally,indium oxide is used as a photoanode. This compound has a suitable bandgap, high trans-parency and electrical conductivity, and has a suitable working function. Due to the limitedindium sources, expensive fabrication methods, instability in acidic environments, andbrittleness of electrodes, the attention of scientists has been drawn to the use of materialswith better performance, such as photoanodes or electrodes [177–180]. Bioresource-derivedQDs have other advantages due to their special properties, such as lightweight and lowdensity, high electrical conductivity (with zero bandgap and good mobility for electronsand holes), and flexibility, which include availability, affordability, sustainability, andan ecofriendly nature; they also have disadvantages, including scaling problems due touneven heating and a wide size distribution of solar cells [181–183]. Since the mass produc-tion of bioresource-derived QDs, intensive research on bioresource-derived QDs has beencarried out in various industrial fields, especially in solar cells [184]. Bioresource-derivedNanomaterials 2022, 12, 3905 17 of 28QDs solar cells are developed based on Gratzel or pigment-sensitive solar cells, but they uselow-bandgap semiconductor compounds that can be used to fabricate bioresource-derivedQDs, such as PbS, Sb2S3, CdSe, and CdS. In these devices, QDs derived from bioresourcesare used instead of light-absorbing organic or metal-organic pigments. Changes in thesize of QDs derived from bioresources lead to changes in the intensity of the wavelengthof light absorbed in these cells [185]. In solar cells sensitized with bioresource-derivedQDs, the mesoporous TiO2 layer forms the main skeleton of the cell, just as it does incells sensitized with pigments, and the deposition of bioresource-derived QDs on the TiO2layer leads to light sensitivity in these structures. The quantum particles can be depositedon the TiO2 layer by various methods, such as chemical bath deposition, electrophoreticdeposition, or successive ionic layer adsorption and reaction (SILAR). Finally, the cycleis closed with a reducing/oxidizing (redox) couple, either solid or liquid. The efficiencyof solar cells sensitized with GQDs in liquid crystal cells and solid-state cells has reachedmore than 5% [186–188]. Bioresource-derived GQDs are widely used in high-performancephotovoltaic devices, including organic-inorganic hybrid solar cells [189] and perovskitesolar cells [190,191]. Figure 10b shows a schematic representation of the structure of a solarcell sensitized with bioresource-derived QDs.Nanomaterials 2022, 12, 3905 18 of 29 has been carried out in various industrial fields, especially in solar cells [184]. Bioresource-derived QDs solar cells are developed based on Gratzel or pigment-sensitive solar cells, but they use low-bandgap semiconductor compounds that can be used to fabricate biore-source-derived QDs, such as PbS, Sb2S3, CdSe, and CdS. In these devices, QDs derived from bioresources are used instead of light-absorbing organic or metal-organic pigments. Changes in the size of QDs derived from bioresources lead to changes in the intensity of the wavelength of light absorbed in these cells [185]. In solar cells sensitized with biore-source-derived QDs, the mesoporous TiO2 layer forms the main skeleton of the cell, just as it does in cells sensitized with pigments, and the deposition of bioresource-derived QDs on the TiO2 layer leads to light sensitivity in these structures. The quantum particles can be deposited on the TiO2 layer by various methods, such as chemical bath deposition, electrophoretic deposition, or successive ionic layer adsorption and reaction (SILAR). Fi-nally, the cycle is closed with a reducing/oxidizing (redox) couple, either solid or liquid. The efficiency of solar cells sensitized with GQDs in liquid crystal cells and solid-state cells has reached more than 5% [186–188]. Bioresource-derived GQDs are widely used in high-performance photovoltaic devices, including organic-inorganic hybrid solar cells [189] and perovskite solar cells [190,191]. Figure 10b shows a schematic representation of the structure of a solar cell sensitized with bioresource-derived QDs. Figure 10. (a) Schematic diagram of a solar cell. Reprinted from [192]. (b) Schematic design of a solar cell sensitized to QDs. Reprinted from Ref. [193]. 6.4.1. Organic and Inorganic Hybrid Solar Cells Silicon crystal cells are the first generation of solar cells. This type of solar cell, with an efficiency of approximately 22%, dominates the world market. However, despite the high efficiency and nontoxicity of the materials, there are limitations in the production of inorganic cells, namely: high production costs, inflexibility, and fragility of this type of cell. Inorganic silicon cells consist of two semiconductors (n) and an acceptor (p). When sunlight shines on the p-n junction (junction between two semiconducting and accepting materials), photons with energy greater than the bandgap energy of the semiconductor create electron-hole pairs, and the pairs formed in the zero region have a high chance of being separated by the internal field before recombination (Figure 11) [194,195]. Organic solar cells consist of conducting polymers or other organic conductors as electron transfer materials. The basis of their work is similar to that of the inorganic solar cell. Polymers with different LUMO (lowest unoccupied molecular orbital) and HUMO (highest occu-pied molecular orbital) levels are bonded together. In general, the process of energy gen-eration in an organic solar cell is divided into several stages, including the absorption of light and formation of excitons, emission of excitons in the direction of transition, dissoci-ation of excitons into charge carriers, and transfer of charge carriers to the electrodes and their collection [196]. Therefore, organic/inorganic hybrid solar cells are of increasing in-terest in fabricating low-cost organic photovoltaics (OPVs) and to achieve other ad-vantages, such as tuning of the absorption spectrum, with inorganic components. This is because hybrid solar cells have the potential to achieve high power conversion efficiency (a) (b) Figure 10. (a) Schematic diagram of a solar cell. Reprinted from [192]. (b) Schematic design of a solarcell sensitized to QDs. Reprinted from Ref. [193].6.4.1. Organic and Inorganic Hybrid Solar CellsSilicon crystal cells are the first generation of solar cells. This type of solar cell, withan efficiency of approximately 22%, dominates the world market. However, despite thehigh efficiency and nontoxicity of the materials, there are limitations in the production ofinorganic cells, namely: high production costs, inflexibility, and fragility of this type ofcell. Inorganic silicon cells consist of two semiconductors (n) and an acceptor (p). Whensunlight shines on the p-n junction (junction between two semiconducting and acceptingmaterials), photons with energy greater than the bandgap energy of the semiconductorcreate electron-hole pairs, and the pairs formed in the zero region have a high chance ofbeing separated by the internal field before recombination (Figure 11) [194,195]. Organicsolar cells consist of conducting polymers or other organic conductors as electron transfermaterials. The basis of their work is similar to that of the inorganic solar cell. Polymerswith different LUMO (lowest unoccupied molecular orbital) and HUMO (highest occupiedmolecular orbital) levels are bonded together. In general, the process of energy generationin an organic solar cell is divided into several stages, including the absorption of light andformation of excitons, emission of excitons in the direction of transition, dissociation ofexcitons into charge carriers, and transfer of charge carriers to the electrodes and theircollection [196]. Therefore, organic/inorganic hybrid solar cells are of increasing interest infabricating low-cost organic photovoltaics (OPVs) and to achieve other advantages, such astuning of the absorption spectrum, with inorganic components. This is because hybridsolar cells have the potential to achieve high power conversion efficiency (PCE), but itis currently low. To increase the power conversion efficiency, mineral materials are usedas electron acceptors in hybrid solar cells. In particular, the electronic structure is veryNanomaterials 2022, 12, 3905 18 of 28important for the device’s performance [197]. Photon down-conversion is a property ofbioresource-derived GQDs that enables the absorption of photons in shorter wavelengthranges for optical applications. Tsai et al. used and investigated GQDs as down-conversionmaterials for heterogeneous silicon solar cells. The short-circuit current in different layersof solar cells increased from 35.31 to 37.47 mA·cm2 by adding GQDs in an amount of0.3 wt% [198]. Additionally, for hybrid solar cells, a yield of 13.22% was obtained usingGQDs [199]. A high detection rate of 8 × 1011 Jones without applying bias voltage can beachieved by introducing GQD as an additive for photon down-conversion in PEDOT:PSSthrough the hybrid device [200].Nanomaterials 2022, 12, 3905 19 of 29 (PCE), but it is currently low. To increase the power conversion efficiency, mineral mate-rials are used as electron acceptors in hybrid solar cells. In particular, the electronic struc-ture is very important for the device’s performance [197]. Photon down-conversion is a property of bioresource-derived GQDs that enables the absorption of photons in shorter wavelength ranges for optical applications. Tsai et al. used and investigated GQDs as down-conversion materials for heterogeneous silicon solar cells. The short-circuit current in diff rent layers of solar cells increased from 35.31 to 37.47 mA·cm2 by adding GQDs in an amount of 0.3 wt% [198]. Additionally, for hybrid solar cells, a yield of 13.22% was obtained using GQDs [199]. A high detection rate of 8 × 1011 Jones without applying bias v ltage can be achieved by introducing GQD as an additive for photon down-conversion in PEDOT:PSS through the hybrid device [200]. Figure 11. Mechanism diagram of the semiconductor physics-related content. 6.4.2. Perovskite Solar Cells The latest generation of solar cells that has attracted the attention of scientists around the world since 2014 is perovskite solar cells. This group of solar cells consists of perov-skite compounds, which are usually organic mineral-lead hybrids or tin halide-based ma-terials. Perovskite materials have two very important advantages: they are cheap to pro-duce and easy to process. The low manufacturing price and high efficiency of this group of solar cells will lead to a large market for these solar cells by 2017 [201–207]. Bioresource-derived GQDs and graphene microlayers are among the advanced nanomaterials that have good chemical stability and tunable band gaps. Moreover, bioresource-derived GQDs act as excellent electron acceptors and donors in photoextraction [208]. To obtain efficient planar perovskite solar cells, Zhang’s group investigated GQD-modified TiO2 films of different sizes in 2017. They also found that GQDs can decrease the effective elec-tron transport at the perovskite/TiO2 interface and the contact resistance. This reduces the series resistance and increases the combined resistance of the device, which in turn im-proves the fill factor and open circuit voltage (VOC). The results show that GQDs increase all PV parameters by 19.11% to achieve the best PCE [209]. To improve the performance of planar perovskite solar cells (PSCs) using GQDs, Yang et al. reported a powerful method, such as a planar phenyl-C61 butyric acid methyl ester electrotron transport layer (PCBM ETL) with additional forward PSCs, which dramatically increases the power con-version efficiency (PCE) of PSCs while improving the optical stability of the devices. While the PCBM GQD device maintained a maximum of 80% under continuous full-spectrum solar irradiation for 300 h, their study showed that the PCE increased from 14.68 to 17.56 (Figure 12). The results showed that the conductivity under GQD doping conditions is an order of magnitude higher compared to pure PCBM [210]. Therefore, the improvement of Figure 11. Mechanism diagram of the semiconductor physics-related content.6.4.2. Perovskite Solar CellsThe latest generation of solar cells that has attracted the attention of scientists aroundthe world since 2014 is perovskite solar cells. This group of solar cells consists of perovskitecompounds, which are usually organic mineral-lead hybrids or tin halide-based materials.Perovskite materials have two very important advantages: they are cheap to produce andeasy to process. The low manufacturing price and high efficiency of this roup of solarcells will lead t a large market for these solar cells by 2017 [201–207]. Bioresource-derivedGQDs and graphen microlayers are among the advanced n n ma erials that have g odchemical stability and tunable b nd gaps. Moreover, bioresource-deriv d GQDs act asexcellent electron acceptor and donors in photo x raction [208]. To obtain fficient planarperovskite solar cells, Zh g’s gr up investigat d GQD-modified TiO2 films of differentsizes in 2017. They also found that GQDs can decrease the effective electron t ansport atthe perovskite/TiO2 interface and the contact resistance. This reduces the s ries resistanceand increases the combined resistance of the device, which in tur improves the fill factorand open circuit voltage (VOC). The results show that GQDs increase all PV parameters by19.11% to achieve the best PCE [209]. To improve the performance of planar perovskite solarcells (PSCs) using GQDs, Yang et al. reported a powerful method, such as a planar phenyl-C61 butyric acid methyl ester electrotron transport layer (PCBM ETL) with additionalforward PSCs, which dramatically increases the power conversion efficiency (PCE) ofPSCs while improving the optical stability of the devices. While the PCBM GQD devicemaintained a maximum of 80% under continuous full-spectrum solar irradiation for 300 h,their study showed that the PCE increased from 14.68 to 17.56 (Figure 12). The resultsshowed that the conductivity under GQD doping conditions is an order of magnitudehigher compared to pure PCBM [210]. Therefore, the improvement of electron transfer inthe perovskite layer, the deactivation of large parts of the grain boundaries, the reductionin charge recombination, and the elimination of electron traps are among the advantages ofintroducing GQDs into the perovskite thin films.Nanomaterials 2022, 12, 3905 19 of 28Nanomaterials 2022, 12, 3905 20 of 29 electron transfer in the perovskite layer, the deactivation of large parts of the grain bound-aries, the reduction in charge recombination, and the elimination of electron traps are among the advantages of introducing GQDs into the perovskite thin films. Figure 12. PSCs with a GQD-doped PCBM electron transport layer. Reprinted with permission from Ref. [210]. Copyright 2017 Elsevier. 7. Conclusions and Outlook One of the biggest challenges of bioresource-functionalized QDs for energy genera-tion and storage is the low production yield (or unreported). While the analysis is per-formed in solution, the yield can be such that it is impossible to separate the dots in solid form. However, in addition to reporting yield or lack thereof, researchers should always provide a reason for low yield (even if the yield is so low that it is impossible to quantify). Knowing these challenges helps researchers who need more effort to improve the yield of solid-dot synthesis methods. Additionally, to increase the viability of QDs derived from bioresources in applications related to energy generation and storage, increasing yield plays a significant role. Quality is as important and necessary as quantity. Optimization for efficient and large-scale production methods is important for the synthesis of high-quality QDs with small, uniform sizes, and high quantum yields. Size uniformity means that the emission properties are uniform and have a narrower range; meanwhile, the high quantum efficiency increases the brightness of the dots. The smaller size increases the sur-face area for functionality and allows them to be used in a wider range of applications, especially in energy generation and storage. These properties are much better for applica-tions, especially in microcapacitors/supercapacitors, batteries, and solar cells. Not fully explaining the optical properties is another challenge that needs to be solved. Therefore, more research should be conducted to fully understand the mechanisms behind PL in different types of QD and how to control them, such as doping, effect size, and surface defects. Researchers should periodically sample during QD synthesis to report on the mechanisms. Finally, the analysis of these samples can be used to suggest the appropriate mechanism because it clarifies what happens during the synthesis. Additionally, more research is needed to describe the effect of changing the synthesis parameters on the phys-ical and optical properties of QDs. To further describe the relationship between physical and optical properties, reports on a wide range of dot properties with synthesis conditions can be used. The synthesis of dots that have better optical properties and that can be tai-lored to their specific applications is possible through a better understanding of the link Figure 12. PSCs with a GQD-doped PCBM electron transport layer. Reprinted with permission fromRef. [210]. Copyright 2017 Elsevier.7. Conclusions and OutlookOne of the biggest challenges of bioresource-functionalized QDs for energy generationand storage is the low production yield (or unreported). While the analysis is performedin solution, the yield can be such that it is impossible to separate the dots in solid form.However, in addition to reporting yield or lack thereof, researchers should always providea reason for low yield (even if the yield is so low that it is impossible to quantify). Knowingthese challenges helps researchers who need more effort to improve the yield of solid-dotsynthesis methods. Additionally, to increase the viability of QDs derived from bioresourcesin applications related to energy generation and storage, increasing yield plays a significantrole. Quality is as important and necessary as quantity. Optimization for efficient andlarge-scale production methods is important for the synthesis of high-quality QDs withsmall, uniform sizes, and high quantum yields. Size uniformity means that the emissionproperties are uniform and have a narrower range; meanwhile, the high quantum efficiencyincreases the brightness of the dots. The smaller size increases the surface area for func-tionality and allows them to be used in a wider range of applications, especially in energygeneration and storage. These properties are much better for applications, especially inmicrocapacitors/supercapacitors, batteries, and solar cells. Not fully explaining the opticalproperties is another challenge that needs to be solved. Therefore, more research shouldbe conducted to fully understand the mechanisms behind PL in different types of QD andhow to control them, such as doping, effect size, and surface defects. Researchers shouldperiodically sample during QD synthesis to report on the mechanisms. Finally, the analysisof these samples can be used to suggest the appropriate mechanism because it clarifies whathappens during the synthesis. Additionally, more research is needed to describe the effect ofchanging the synthesis parameters on the physical and optical properties of QDs. To furtherdescribe the relationship between physical and optical properties, reports on a wide rangeof dot properties with synthesis conditions can be used. The synthesis of dots that havebetter optical properties and that c be tail red to their specific applications is possiblethrough a better understanding of th link between hysical properties and optical prop-erties, as well as through a better und rstanding of PL mechanisms. Bioresource-derivedQDs are currently moving toward green synthesis consideration, and some syntheses arealready green-labeled. Therefore, it is expected that syntheses will use green principlesas much as possible in the future. Additionally, syntheses should be efficient in terms ofreducing reaction waste, energy, and atomic economy. This type of synthesis must includeNanomaterials 2022, 12, 3905 20 of 28the selection of bioresources from the waste stream and micro-organisms to prevent wastedisposal and prevent the creation of something new to use as a carbon or heteroatomsource in the synthesis. Therefore, it is expected that syntheses will use green principlesas much as possible in the future. Additionally, syntheses should be efficient in terms ofreducing reaction waste, energy, and atomic economy. This type of synthesis must includethe selection of bioresources from the waste stream and micro-organisms to prevent wastedisposal and prevent the creation of something new to use as a carbon or heteroatom sourcein the synthesis. The synthesis should use inherently benign and nonhazardous chemistry,which facilitates the prevention of accidents and product toxicity. Bioresource-derived QDshave become the best solution for many applications for a long period of time by ensuringthat the synthesis is forward-looking and as green as possible. Since bioresource-derivedQDs have been seen to work with microcapacitors/supercapacitors, both in batteries andin targeted solar cells, it stands to reason that bioresource-derived QDs are excellent can-didates in the field of energy generation and storage. Typically, bioresource-derived QDshelp maintain the cycling stability of electrode materials and shorten charge transfer pathsdue to their crystal structure and improved surface properties. Considering the advantagesand limitations mentioned in the text, it is expected that more research will be conductedto provide high energy density and stable electrodes for energy generation and storageapplications in a cost-effective and environmentally friendly design using bioresource-derived QDs. Although QDs play a role in energy generation and storage applications,several critical problems and obstacles have yet to be addressed to fully understand theunderlying mechanism, process, and important knowledge of bioresource-functionalizedQDs. First, it remains difficult to obtain bioresource-functionalized QDs with high quantumyields. Therefore, future research efforts should focus on chemical and photostability andenhancing high quantum yields. Second, applied research should simultaneously focus onthe selectivity, quality improvement, and robustness of QDs with bioresource functionalityfor energy-oriented platforms. We anticipate that simpler, more revolutionary, and cost-effective green methods, and promising energy applications will be developed in the nearfuture to better exploit the potential of these important quantum materials.Author Contributions: S.M.M. and A.G. developed the idea and structure of the review article. S.A.H.and M.Y.K. wrote the manuscript and collected materials from databases. D.K. and A.G. revised andimproved the manuscript. S.M.M., A.G. and W.-H.C. supervised the writing of the manuscript. Allauthors have read and agreed to the published version of the manuscript.Funding: This work is sponsored by the Ministry of Science and Technology, Taiwan (grant number:MOST 111-2811-E-011-018, 111-2223-E-011-002-MY3, 111-NU-E-011-001-NU, 111-2628-E-011-002-MY2,109-2923-E-011-003-MY3).Institutional Review Board Statement: Not applicable.Informed Consent Statement: Not applicable.Data Availability Statement: All data generated or analyzed during this study are included in thispublished article.Conflicts of Interest: The authors declare no conflict of interest.References1. Tian, X.; Zhu, S.; Peng, J.; Zuo, Y.; Wang, G.; Guo, X.; Zhao, N.; Ma, Y.; Ma, L. Synthesis of micro-and meso-porous carbon derivedfrom cellulose as an electrode material for supercapacitors. Electrochim. 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Bioresource-Functionalized Quantum Dots for Energy Generation and Storage: Recent Advances and Feature Perspective
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