Local ionic transport enables selective PGM-free bipolar membrane electrode assembly

Li, Mengran; Lees, Eric W.; Ju, Wen; Subramanian, Siddhartha; Yang, Kailun; Bui, Justin C.; Iglesias van Montfort, Hugo-Pieter; Abdinejad, Maryam; Middelkoop, Joost; Strasser, Peter; Weber, Adam Z.; Bell, Alexis T.; Burdyny, Thomas

doi:10.1038/s41467-024-52409-z

Title: Local ionic transport enables selective PGM-free bipolar membrane electrode assembly

Journal Article · 19 September 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-52409-z · OSTI ID:2454984

^[1]; Lees, Eric W. ^[2]; Ju, Wen ^[3];

^[4]; Yang, Kailun ^[4];

^[5];

^[4];

^[6]; Middelkoop, Joost ^[4];

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Delft Univ. of Technology (Netherlands); Univ. of Melbourne, VIC (Australia)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of British Columbia, Vancouver, BC (Canada)
Technical Univ. of Berlin (Germany); Leibniz Institute for Catalysis, Rostock (Germany)
Delft Univ. of Technology (Netherlands)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Delft Univ. of Technology (Netherlands); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Technical Univ. of Berlin (Germany)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Bipolar membranes in electrochemical CO₂ conversion cells enable different reaction environments in the CO₂-reduction and O₂-evolution compartments. Under ideal conditions, water-splitting in the bipolar membrane allows for platinum-group-metal-free anode materials and high CO₂ utilizations. In practice, however, even minor unwanted ion crossover limits stability to short time periods. Here we report the vital role of managing ionic species to improve CO₂ conversion efficiency while preventing acidification of the anodic compartment. Through transport modelling, we identify that an anion-exchange ionomer in the catalyst layer improves local bicarbonate availability and increasing the proton transference number in the bipolar membranes increases CO₂ regeneration and limits K⁺ concentration in the cathode region. Through experiments, we show that a uniform local distribution of bicarbonate ions increases the accessibility of reverted CO₂ to the catalyst surface, improving Faradaic efficiency and limiting current densities by twofold. Using these insights, we demonstrate a fully platinum-group-metal-free bipolar membrane electrode assembly CO₂ conversion system exhibiting <1% CO₂/cation crossover rates and 80-90% CO₂-to-CO utilization efficiency over 150 h operation at 100 mA cm^-2 without anolyte replenishment.

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Bioenergy Technologies Office (BETO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

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

OSTI ID:: 2454984

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Local ionic transport enables selective PGM-free bipolar membrane electrode assembly

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