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Open access publications by faculty, postdocs, and graduate students in the Department of Chemical and Biomolecular Engineering
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Browsing Open Access Publications by Subject "alloy"
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Item Cu Based Dilute Alloys for Tuning the C2+ Selectivity of Electrochemical CO2 Reduction(Small, 2024-07-12) Crandall, Bradie S.; Qi, Zhen; Foucher, Alexandre C.; Weitzner, Stephen E.; Akhade, Sneha A.; Liu, Xin; Kashi, Ajay R.; Buckley, Aya K.; Ma, Sichao; Stach, Eric A.; Varley, Joel B.; Jiao, Feng; Biener, JuergenElectrochemical CO2 reduction is a promising technology for replacing fossil fuel feedstocks in the chemical industry but further improvements in catalyst selectivity need to be made. So far, only copper-based catalysts have shown efficient conversion of CO2 into the desired multi-carbon (C2+) products. This work explores Cu-based dilute alloys to systematically tune the energy landscape of CO2 electrolysis toward C2+ products. Selection of the dilute alloy components is guided by grand canonical density functional theory simulations using the calculated binding energies of the reaction intermediates CO*, CHO*, and OCCO* dimer as descriptors for the selectivity toward C2+ products. A physical vapor deposition catalyst testing platform is employed to isolate the effect of alloy composition on the C2+/C1 product branching ratio without interference from catalyst morphology or catalyst integration. Six dilute alloy catalysts are prepared and tested with respect to their C2+/C1 product ratio using different electrolyzer environments including selected tests in a 100-cm2 electrolyzer. Consistent with theory, CuAl, CuB, CuGa and especially CuSc show increased selectivity toward C2+ products by making CO dimerization energetically more favorable on the dominant Cu facets, demonstrating the power of using the dilute alloy approach to tune the selectivity of CO2 electrolysis.