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Abstract

To combat climate change and the energy crisis, we are urged to turn to renewable energy sources such as solar, wind, and ocean power. However, these sources are intermittent, such as solar panels being ineffective at night and wind power being inconsistent in most regions. Thus, we need to develop a safe, affordable, durable chemistry of energy storage to achieve a reliable, resilient energy supply from renewables. The chemistry of aqueous Zn-ion batteries (AZIB) has gained attention in the realm of energy storage owing to their capability of realizing decent energy density from Zn metal on the premise of a non-flammable, cost-effective aqueous electrolyte chemistry. Nevertheless, the practicality of using AZIB in large-scale energy storage scenarios is questionable due to the inadequate reversibility of Zn stripping and plating and an unavoidable challenge of multiple parasitic reactions such as hydrogen evolution reaction (HER) on Zn. There is a pressing demand for a highly reversible, HER-free chemistry of anodic interface. In response to that, this Ph.D. study focuses on addressing the issue of anode interface instability, developing durable AZIB through interfacial engineering, and gaining a new understanding of the interplay between interfacial phenomenon and electrochemical performance. Practically, the weakly solvating electrolyte strategy makes a high-loading AZIB demonstrate decent cycling stability, in addition to the intrinsic safety characteristics of AZIB chemistry, exhibiting the great potential of AZIB in energy storage applications.