Impact of Alkali Cation Identity on the Conversion of HCO3− to CO in Bicarbonate Electrolyzers

ChemElectroChem - Tập 8 Số 11 - Trang 2094-2100 - 2021
Arthur G. Fink1, Eric W. Lees2, Zishuai Zhang1, Shaoxuan Ren1, Roxanna S. Delima2,3, Curtis P. Berlinguette4,2,1,3
1Department of Chemistry, The University of British Columbia, 2036 Main Mall, Vancouver, British Columbia, V6T 1Z1, Canada
2Department of Chemical and Biological Engineering, The University of British Columbia, 2360 East Mall, Vancouver, British Columbia, V6T 1Z3, Canada
3Stewart Blusson Quantum Matter Institute, The University of British Columbia, 2355 East Mall, Vancouver, British Columbia V6T 1Z4, Canada
4Canadian Institute for Advanced Research (CIFAR), 661 University Avenue, Toronto, Ontario, M5G 1 M1 Canada

Tóm tắt

AbstractThe reduction of CO2 to CO from a bicarbonate feedstock offers an opportunity to directly use aqueous carbon capture solutions, while bypassing ex‐situ energy‐intensive gaseous CO2 regeneration. In this study, we resolved how the electrolyte cation identity (Li+, Na+, K+, Cs+) affects the two reactions that make bicarbonate electrolysis possible: (i) the production of in‐situ CO2 formed through reaction of HCO3− (from the catholyte) with H+ (sourced from the membrane); and (ii) the electroreduction of CO2 into CO. Our results show that cation identity does not change the rate of in‐situ CO2 formation, but it does enhance the rate of the CO2 reduction reaction (CO2RR). Electrolysis experiments performed with a constant [HCO3−] showed that CO selectivities progressively increased for the series Li+, Na+, K+, and Cs+, respectively. Optimization of the electrolyte composition yielded a CO selectivity of ∼80 % during electrolysis of 1.5 M CsHCO3 solutions at 100 mA cm−2, while saturated LiHCO3 solutions (0.84 M) yielded CO selectivities values of merely 30 % at the same current density. This study demonstrates a quantitative relationship between CO product selectivity and the cation radius, which provides a pathway to integrate bicarbonate electrolysis to carbon capture.

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ChemElectroChem

Tập 8 Số 11

2094-2100

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