Stable dual metal oxide matrix for tuning selectivity in acidic electrochemical carbon dioxide reduction

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dc.contributor.authorZhang, Z.
dc.contributor.authorTrần-Phú, T.
dc.contributor.authorYuwono, J.
dc.contributor.authorMa, Z.
dc.contributor.authorYang, Y.
dc.contributor.authorLeverett, J.
dc.contributor.authorHocking, R.K.
dc.contributor.authorJohannessen, B.
dc.contributor.authorKumar, P.
dc.contributor.authorAmal, R.
dc.contributor.authorDaiyan, R.
dc.date.issued2025
dc.description.abstractThe acidic electrochemical CO₂ reduction reaction (CO₂RR) holds promise for achieving a carbon-neutral future and can promote efficient CO₂ utilization by attenuating the carbonate/bicarbonate formation reaction. However, catalyst degradation in strong acids and the competing hydrogen evolution reaction (HER) often result in short catalyst lifetime and poor product selectivity. Herein, this study introduces a strategy to stabilize copper oxide (CuOₓ) catalysts for acidic CO₂ reduction (CO₂RR) by incorporating bismuth oxide (BiOₓ) and achieved a maximum formic acid Faradaic efficiency (FEHCOOH) of 97 ± 1 % at —2.7 V vs. RHE and maintaining over 90 % FE for more than 20 h. In situ XAS, SR-FTIR and density functional theory (DFT) calculations show that the catalyst can inhibit *H adsorption and promote selective CO₂ conversion to HCOOH via the HCOO* pathway. Further electrolyte anion modulation achieves ethanol and acetone production at Faradaic efficiencies of 17 % and 16 % in phosphoric and perchloric acid, respectively. In situ analyses reveal that distinct anion adsorption influence key intermediates, such as *CO, leading to shifts in C₂₊ product distributions. This work offers insights into designing acid-stable electrocatalysts for CO₂RR and highlights the potential of electrolyte modification to tailor product selectivity.
dc.description.statementofresponsibilityZiling Zhang, Thanh Trần-Phú, Jodie Yuwono, Zhipeng Ma, Yuwei Yang, Josh Leverett, Rosalie K. Hocking, Bernt Johannessen, Priyank Kumar, Rose Amal, Rahman Daiyan
dc.identifier.citationApplied Catalysis B: Environmental, 2025; 371:125203-1-125203-9
dc.identifier.doi10.1016/j.apcatb.2025.125203
dc.identifier.issn0926-3373
dc.identifier.issn1873-3883
dc.identifier.orcidYuwono, J. [0000-0002-0915-0756]
dc.identifier.urihttps://hdl.handle.net/2440/147758
dc.language.isoen
dc.publisherElsevier
dc.relation.grantARC
dc.rights© 2025 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
dc.source.urihttps://doi.org/10.1016/j.apcatb.2025.125203
dc.subjectCO₂ reduction; electrocatalysis; acid stable; In situ XAS
dc.titleStable dual metal oxide matrix for tuning selectivity in acidic electrochemical carbon dioxide reduction
dc.typeJournal article
pubs.publication-statusPublished

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