Continuum Model to Define the Chemistry and Mass Transfer in a Bicarbonate Electrolyzer

Lees, Eric W.; Bui, Justin C.; Song, Datong; Weber, Adam Z.; Berlinguette, Curtis P.

doi:10.1021/acsenergylett.1c02522

Title: Continuum Model to Define the Chemistry and Mass Transfer in a Bicarbonate Electrolyzer

Journal Article · 24 January 2022 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.1c02522 · OSTI ID:1877591

Lees, Eric W. ^[1];

^[2]; Song, Datong ^[3];

^[4];

^[5]

Univ. of British Columbia, Vancouver, BC (Canada); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
National Research Council Canada, Vancouver, BC (Canada)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of British Columbia, Vancouver, BC (Canada); Canadian Institute for Advanced Research (CIFAR), Toronto, ON (Canada)

Bicarbonate electrolyzers are devices designed to convert CO₂ captured from point sources or the atmosphere into chemicals and fuels without needing to first isolate pure CO₂ gas. In this work, we report here an experimentally validated model that quantifies the reaction chemistry and mass transfer processes within the catalyst layer and cation exchange membrane layer of a bicarbonate electrolyzer. Our results demonstrate that two distinct chemical microenvironments are key to forming CO at high rates: an acidic membrane layer that promotes in situ CO₂ formation and a basic catalyst layer that suppresses the hydrogen evolution reaction. We show that the rate of CO product formation can be increased by modulating the catalyst and membrane layer properties to increase the rate of in situ CO₂ generation and transport to the cathode. These insights serve to inform the design of bicarbonate and BPM-based CO₂ electrolyzers while demonstrating the value of modeling for resolving rate-determining processes in electrochemical systems.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Canadian Foundation for Innovation; Canadian Institute for Advanced Research (CIFAR); Canadian Natural Science and Engineering Research Council; National Research Council of Canada; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0021266

OSTI ID:: 1877591

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 2 Vol. 7; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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