Photoelectrochemical (PEC) CO 2 reduction (PEC CO 2 R) is a prospective approach for utilizing solar energy to synthesize a variety of carbon-containing chemicals and fuels, the most valuable of which are multicarbon (C 2+ ) products, such as ethylene and ethanol. While these products can be produced with high faradaic efficiency using Cu, this occurs over a relatively narrow potential range, which, in turn, imposes constraints on the design of a device for PEC CO 2 R. Herein, we used continuum-scale modeling to simulate the solar-to-C 2+ (STC 2+ ) efficiency of PEC CO 2 R devices fed with CO 2 -saturated, 0.1 M CsHCO 3 . We then explored how cell architecture and the use of single or dual photoelectrode(s) alters the optimal combination of photoelectrode bandgaps for high STC 2+ efficiency. Ultimately, this work provides guidance for the co-design of the device architecture and photoelectrode bandgaps required to achieve high STC 2+ efficiency. The insights gained are then used to identify systems that yield the highest amount of C 2+ products throughout the day and year. Photoelectrochemical CO 2 reduction to multicarbon products with high efficiency. Co-design of photoelectrochemical CO 2 reduction devices for multicarbon product generation. Optimal semiconductor bandgaps for high multicarbon product selectivity. Limitations in multicarbon product generation from photoelectrochemical CO 2 reduction. Optimizing photoelectrochemical CO 2 reduction systems for multicarbon product generation.
CITATION STYLE
Wei, W. J., King, A. J., Bui, J. C., Weber, A. Z., & Bell, A. T. (2023). Co-Design of Multijunction Photoelectrochemical Devices for Unassisted CO 2 Reduction to Multicarbon Products. Journal of The Electrochemical Society, 170(12), 126502. https://doi.org/10.1149/1945-7111/ad10e7
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