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Setiawan, Felix Arie

University of British Columbia

Bio-oil upgrading by electrocatalysis requires significant technical innovations so as to compete with thermocatalytic processes that have significantly higher catalytic activity. In the present study, the primary advantage of in-situ hydrogen supply from water electrolysis is combined with the development of non-noble metal catalysts for the bio-oil electrocatalytic hydrodeoxygenation (ECH-DO) reaction. Furthermore, the well-established technology of paired electrosynthesis is applied to bio-oil ECH-DO with anodic coupling electrosynthesis (ACE), utilizing the glycerol electrooxidation reaction, creating product intensification and increasing process energy efficiency. Firstly, the study assessed candidate anodic reactions using multi-objective optimization (MOO) based on six key elements: safety, environment, energy, economics, separation, and technology readiness level. Secondly, the selected ACE and bio-oil ECH-DO were optimized individually in different electrolyte pairs using noble metal catalysts in a divided stirred slurry electrocatalytic reactor (SSER). Thirdly, the paired electrosynthesis of guaiacol (as bio-oil model compound) electrocatalytic hydrodeoxygenation (GECH-DO) and the ACE was assessed to find the best operating conditions in terms of agitation speed, initial concentration, current density, temperature, and metal loading. Lastly, tailored binary (PtNi/C and PtCo/C) and ternary (PtNiCo/C) electrocatalysts were introduced and compared with the existing reference electrocatalyst (Pt/C). Glycerol electrooxidation (GEOR) to glyceraldehyde was the best candidate for the anodic electrosynthesis based on the MOO analysis. Results showed that 25% isopropanol (IPA) in the catholyte triggered the dehydration reaction of guaiacol towards cyclohexane. Furthermore, the Pt/C catalyst had the highest catalytic activity for GECH-DO and GEOR for glyceraldehyde production, compared to Ru/C and Pd/C. The paired electrosynthesis was favored in acid-acid electrolyte pairs. Compared with the half-cell, the paired cell electrosynthesis decreased the required energy and increased faradaic efficiency. The best operating condition of the paired cell (400 RPM, 100 mM guaiacol and 300 mM glycerol initial concentration, 66 mA cm⁻² (0.4 A), and 50 °C) with the Pt/C catalyst resulted in 93.7% guaiacol conversion. The tailored PtNi/C decreased the dependency on Pt by as much as 40% while maintaining performance of the paired synthesis.

Text

2025-05-01

Attribution-NonCommercial-NoDerivatives 4.0 International

http://hdl.handle.net/2429/90940

Chemical and Biological Engineering

University of British Columbia

UBCV

http://creativecommons.org/licenses/by-nc-nd/4.0/