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journal article·2024-10Open access

Stabilization of Cuδ+ Sites Within MnO2 for Superior Urea Electro‐Synthesis

Yidong Yang, Guanzheng Wu, Jiadi Jiang, Wuyong Zhang, Sijia Liu, Rui Yu, Fukang Liu, Aijun Du, Lei Dai, Xin Mao, Qing Qin

Advanced Materials· Volume 36· Issue 41
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Source abstract

Abstract

Abstract Electrocatalytic C‐N coupling between NO3‐ and CO2 has emerged as a sustainable route for urea production. However, identifying catalytic active sites and designing efficient electrocatalysts remain significant challenges. Herein, the synthesis of Cu‐doped MnO2 nanotube (denoted as Cu‐MnO2) with stable Cuδ+‐oxygen vacancies (Ovs)‐Mn3+ dual sites is reported. Compared with pure MnO2, Cuδ+ doping can effectively enhance urea production performance in the co‐reduction of CO2 and NO3‐. Thus, Cu‐MnO2 catalyst exhibits a maximum Faradaic efficiency (FE) of 54.7% and the highest yield rate of 116.7 mmol h−1 gcat.−1 in a flow cell. Remarkably, the urea yield rate remains over 78 mmol h−1 gcat.−1 across a wide potential range. Further experimental and theoretical results elucidate the unique role of Cu‐MnO2 solid‐solution for stabilizing Cuδ+ sites in Cuδ+‐Ovs‐Mn3+, endowing the catalyst with superior structural and electrochemical stabilities. This thermodynamically promotes urea formation and kinetically lowers the energy barrier of C‐N coupling.
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Research context

NanomaterialsCatalysis & surfaces

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · CO2 Reduction Techniques and Catalysts · Electrocatalysts for Energy Conversion

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

The Key Laboratory of Functional Molecular Solids Ministry of Education The Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education Institutes College of Chemistry and Materials Science Anhui Normal University Wuhu 241002 P. R. China

Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Qianwan Institute of CNITECH Ningbo Institute of Materials Technology and Engineering Chinese Academy of Sciences Ningbo Zhejiang 315201 P. R. China

School of Chemistry and Physics and Centre for Material Science Faculty of Science Queensland University of Technology Gardens Point Campus Brisbane QLD 4001 Australia

Key Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and Engineering Academy for Advanced Interdisciplinary Studies Henan University Kaifeng 475004 P. R. China

Funding

National Natural Science Foundation of China · Natural Science Foundation of Anhui Province

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