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pH‐Controlled Catalyst Reconstruction Switches CO2 Reduction Pathways Between Methane and Ethylene.

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Title: pH‐Controlled Catalyst Reconstruction Switches CO2 Reduction Pathways Between Methane and Ethylene.
Authors: Li, Yawen1 (AUTHOR), Zhu, Zifan1 (AUTHOR), Yu, Chuning1 (AUTHOR), Li, Jianhui2 (AUTHOR), Zhang, Lizhong3 (AUTHOR), Song, Yang4 (AUTHOR) songyang.ripp@sinopec.com, Alodhayb, Abdullah N.5 (AUTHOR), Yi, Xiaodong2 (AUTHOR) xdyi@xmu.edu.cn, Chen, Zhou1 (AUTHOR) zhouchen@xmu.edu.cn
Source: ChemCatChem. Jun2026, Vol. 18 Issue 11, p1-9. 9p.
Subjects: Carbon dioxide reduction, Catalyst selectivity, Hydrogen-ion concentration, Copper catalysts, Catalyst structure, Methane, Electrochemical analysis, Ethylene industry
Abstract: Controlling product selectivity in electrochemical CO2 reduction (CO2RR) on Cu‐based catalysts remains a major challenge due to the complex interplay between catalyst structure and local reaction environment. Herein, we report a pH‐controlled reconstruction strategy to regulate catalyst morphology and electronic structure, enabling selective CO2RR pathways toward either methane or ethylene. A maleic acid copper (MHCu) precursor is electrochemically reduced under different pH conditions, which modulates the Ostwald ripening process and results in Cu/CuxO catalysts with distinct particle sizes and surface roughness. Under acidic conditions, accelerated ripening produces larger and smoother particles, favoring CH4 formation with a Faradaic efficiency of up to 60.5%. In contrast, suppressed ripening under neutral and alkaline conditions generates roughened nanostructures that promote C–C coupling, delivering C2+ products with Faradaic efficiencies exceeding 50% and a maximum C2H4 selectivity of 34.0%. Notably, the product selectivity can be effectively switched between CH4 and C2H4, with CH4 reaching a Faradaic efficiency of 60.5% and the C2H4/CH4 ratio increasing up to 10.0 under optimized conditions. Electrochemical and spectroscopic analyses reveal that the enhanced C2+ production originates from the combined effects of increased surface roughness and optimized Cu valence states, which facilitate *CO accumulation and subsequent C–C coupling. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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Abstract:Controlling product selectivity in electrochemical CO2 reduction (CO2RR) on Cu‐based catalysts remains a major challenge due to the complex interplay between catalyst structure and local reaction environment. Herein, we report a pH‐controlled reconstruction strategy to regulate catalyst morphology and electronic structure, enabling selective CO2RR pathways toward either methane or ethylene. A maleic acid copper (MHCu) precursor is electrochemically reduced under different pH conditions, which modulates the Ostwald ripening process and results in Cu/CuxO catalysts with distinct particle sizes and surface roughness. Under acidic conditions, accelerated ripening produces larger and smoother particles, favoring CH4 formation with a Faradaic efficiency of up to 60.5%. In contrast, suppressed ripening under neutral and alkaline conditions generates roughened nanostructures that promote C–C coupling, delivering C2+ products with Faradaic efficiencies exceeding 50% and a maximum C2H4 selectivity of 34.0%. Notably, the product selectivity can be effectively switched between CH4 and C2H4, with CH4 reaching a Faradaic efficiency of 60.5% and the C2H4/CH4 ratio increasing up to 10.0 under optimized conditions. Electrochemical and spectroscopic analyses reveal that the enhanced C2+ production originates from the combined effects of increased surface roughness and optimized Cu valence states, which facilitate *CO accumulation and subsequent C–C coupling. [ABSTRACT FROM AUTHOR]
ISSN:18673880
DOI:10.1002/cctc.70825