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Electrochemical conversion of CO₂ into formate (HCOO⁻) represents a promising strategy for mitigating global warming while producing an industrially important chemical. Polyoxometalates (POMs), anionic molecular metal-oxo clusters, offer unique opportunities as catalysts and catalyst precursors for the electrochemical CO₂ reduction reaction (CO₂RR) owing to their structural diversity, compositional tunability, and flexibility in countercation selection. Despite these advantages, effective strategies for developing POM-based CO₂RR catalysts with high selectivity toward HCOO⁻ remain limited. In this study, we demonstrate countercation manipulation as a powerful approach to achieving selective HCOO⁻ production using a bismuth (Bi)-incorporated POM, [Bi₄O(γ-SiW₁₀O₃₆)₂(OAc)]⁷⁻ (Bi4). Under gas-diffusion CO₂RR conditions with a 2 M KHCO₃ aqueous electrolyte, the Ba²⁺ salt of Bi4 immobilized on carbon (Ba-Bi4/C) exhibited high HCOO⁻ selectivity with a Faradaic efficiency of 84.3% at −0.79 V_RHE, whereas the corresponding tetra-n-butylammonium (TBA⁺) salt (TBA-Bi4/C) exhibited substantially lower selectivity (26.6% at −0.79 V_RHE). Post-reaction analyses revealed that both catalysts transformed into highly dispersed Bi species protected by WO_x nanoaggregates. Control experiments and detailed characterizations indicated that the countercations, in conjunction with the POM-derived catalyst structure, play a crucial role in governing CO₂RR performance.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: bismuth, electrochemical CO2 reduction reaction, electrode catalysis, nanocatalysts, polyoxometalates

刊行年月日: 2026-10-27

出版者: Wiley

掲載誌:

• Chemistry – A European Journal (ISSN: 09476539) vol. 32 issue. 40 e71437

研究助成金:

• Japan Science and Technology Agency
• Japan Society for the Promotion of Science

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1002/chem.71437

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更新時刻: 2026-10-29 10:06:21 +0900

MDRでの公開時刻: 2026-10-29 12:27:40 +0900