Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia

Author:

Wang Yunhao1,Xiong Yuecheng12,Sun Mingzi3,Zhou Jingwen12,Hao Fengkun1,Zhang Qinghua4,Ye Chenliang5,Wang Xixi1,Xu Zhihang6,Wa Qingbo1,Liu Fu1,Meng Xiang1,Wang Juan1,Lu Pengyi12,Ma Yangbo1,Yin Jinwen1,Zhu Ye6,Chu Shengqi7,Huang Bolong3,Gu Lin8,Fan Zhanxi129ORCID

Affiliation:

1. Department of Chemistry City University of Hong Kong Kowloon Hong Kong 999077 China

2. Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM) City University of Hong Kong Kowloon Hong Kong 999077 China

3. Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University Kowloon Hong Kong 999077 China

4. Institute of Physics Beijing National Laboratory for Condensed Matter Physics Chinese Academy of Sciences Beijing 100190 China

5. Department of Power Engineering North China Electric Power University Baoding 071003 China

6. Department of Applied Physics Research Institute for Smart Energy The Hong Kong Polytechnic University Kowloon Hong Kong 999077 China

7. Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China

8. Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials Department of Materials Science and Engineering Tsinghua University Beijing 100084 China

9. City University of Hong Kong Shenzhen Research Institute Shenzhen 518057 China

Abstract

AbstractThe controlled synthesis of metal nanomaterials with unconventional phases is of significant importance to develop high‐performance catalysts for various applications. However, it remains challenging to modulate the atomic arrangements of metal nanomaterials, especially the alloy nanostructures that involve different metals with distinct redox potentials. Here we report the general one‐pot synthesis of IrNi, IrRhNi and IrFeNi alloy nanobranches with unconventional hexagonal close‐packed (hcp) phase. Notably, the as‐synthesized hcp IrNi nanobranches demonstrate excellent catalytic performance towards electrochemical nitrite reduction reaction (NO2RR), with superior NH3 Faradaic efficiency and yield rate of 98.2 % and 34.6 mg h−1 mgcat−1 (75.5 mg h−1 mgIr−1) at 0 and −0.1 V (vs reversible hydrogen electrode), respectively. Ex/in situ characterizations and theoretical calculations reveal that the Ir−Ni interactions within hcp IrNi alloy improve electron transfer to benefit both nitrite activation and active hydrogen generation, leading to a stronger reaction trend of NO2RR by greatly reducing energy barriers of rate‐determining step.

Funder

National Natural Science Foundation of China

City University of Hong Kong

Publisher

Wiley

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