Sustainedly High-Rate Electroreduction of CO2 to Multi-Carbon Products on Nickel Oxygenate/Copper Interfacial Catalysts

Mao, Xuejiao; Chang, Chun‐Wai; Li, Zhiguo; Han, Zishan; Gao, Jiachen; Lyons, Mason; Sterbinsky, George; Guo, Yong; Zhang, Bo; Wang, Yaogang; Wang, Xinyu; Han, Daliang; Yang, Quan‐Hong; Feng, Zhenxing; Weng, Zhe

doi:10.1002/aenm.202400827

Sustainedly High-Rate Electroreduction of CO₂ to Multi-Carbon Products on Nickel Oxygenate/Copper Interfacial Catalysts

Journal Article · Sat Apr 13 00:00:00 EDT 2024 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202400827· OSTI ID:2564994

Mao, Xuejiao ^[1]; Chang, Chun‐Wai ^[2]; Li, Zhiguo ^[1]; Han, Zishan ^[1]; Gao, Jiachen ^[1]; Lyons, Mason ^[2]; Sterbinsky, George ^[3]; Guo, Yong ^[1]; Zhang, Bo ^[1]; Wang, Yaogang ^[1]; Wang, Xinyu ^[1]; Han, Daliang ^[1]; Yang, Quan‐Hong ^[1]; Feng, Zhenxing ^[2]; Weng, Zhe ^[1]

Tianjin University (China); Haihe Laboratory of Sustainable Chemical Transformations, Tianjin (China)
Oregon State University, Corvallis, OR (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Copper (Cu) is the most attractive electrocatalyst for CO₂ reduction to multi-carbon (C₂₊) products with high economic value in considerable amounts. However, the rational design of a structurally stable Cu-based catalyst that can achieve high activity and stability towards C₂₊ products remain a grand challenge. Here, in this study, a highly stable nickel oxygenate/Cu electrocatalyst is developed with abundant NiOOH/Cu interfaces by in situ electrochemical reconstruction. The nickel oxygenate/Cu electrocatalyst achieves a superior Faradaic efficiency of 86.3 ± 3.0% and a record partial current density of 2085 A g^-1 for C₂₊ products with long-term stability. In situ experimental and theoretical studies demonstrates that the exceptional performance in generating C₂₊ products is attributed to the presence of the NiOOH/Cu interfaces which increase *CO coverage, lower energy barrier for *CO coupling and stabilize *OCCO simultaneously. This work provides new insights into the rational design of electrocatalysts to achieve stable and efficient electrocatalytic CO₂ reduction capabilities.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2564994

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 25 Vol. 14; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 reduction
copper
electrocatalysis
interface
reconstruction

Sustainedly High-Rate Electroreduction of CO2 to Multi-Carbon Products on Nickel Oxygenate/Copper Interfacial Catalysts

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Sustainedly High-Rate Electroreduction of CO₂ to Multi-Carbon Products on Nickel Oxygenate/Copper Interfacial Catalysts