journal article·2024-05-15

Synthesis of Rhenium-Doped Copper Twin Boundary for High-Turnover-Frequency Electrochemical Nitrogen Reduction

Tong Ye, Yajie Wang, Xiang Yao, Hongbin Li, Taishi Xiao, Kun Ba, Yi Tang, Changlin Zheng, Xiaoyong Yang, Zhengzong Sun

ACS Applied Materials & Interfaces· Volume 16· Issue 19
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Abstract

The precise design and synthesis of active sites to improve catalyst’s performance has emerged as a promising tactic for electrochemistry. However, it is challenging to combine different types of active sites and manipulate them simultaneously at atomic resolution. Here, we present a strategy to synthesize Re atom-doped Cu twin boundaries (TBs), through pulsed electrodeposition and boundary segregation. The Re-doped Cu TBs demonstrate a highly efficient nitrogen reduction reaction (NRR) performance. Re-doped Cu TBs showed a turnover frequency of ∼5889 s –1, ∼800 times higher than the pure Cu TB active centers (∼7 s –1 ). In addition to the “acceptance–donation” activation of N 2 molecules, theoretical calculations also reveal that the Re–Re dimer on TB can boost the NRR and impede the hydrogen evolution reaction synchronously, rendering Re-doped Cu TB catalysts with high NRR activity and selectivity.
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Research context

OpenAlex topics: Ammonia Synthesis and Nitrogen Reduction · Electrocatalysts for Energy Conversion · Advanced Photocatalysis Techniques

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

Affiliations

Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, P. R. China

School of Microelectronics and State Key Laboratory of ASIC and System, Fudan University, Shanghai 200433, P. R. China

State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200438, P. R. China

School of National Defense Science and Technology, State Key Laboratory for Environment Friendly Energy Materials, Southwest University of Science and Technology, Mianyang 621010, China

Condensed Matter Theory Group, Materials Theory Division, Department of Physics and Astronomy, Uppsala University, Box 516, Uppsala 75120, Sweden

Yiwu Research Institute of Fudan University, Yiwu, Zhejiang 322000, P. R. China

Funding

Fudan University · National Key Research and Development Program of China · China Scholarship Council · National Natural Science Foundation of China · the Longxing Chemical Program of Fudan University

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