Volume 135, Issue 13 e202217473
Forschungsartikel

Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Atomically Dispersed Sn Protuberance

Dr. Lijuan Zhang

Dr. Lijuan Zhang

School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China

SCNU Environmental Research Institute, Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety & MOE Key Laboratory of Theoretical Chemistry of Environment, South China Normal University, Guangzhou, 510006 China

These authors contributed equally to this work.

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Hanfeng Zhou

Hanfeng Zhou

School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China

These authors contributed equally to this work.

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Prof. Xiaoju Yang

Prof. Xiaoju Yang

School of Chemistry and Chemical Engineering, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, Huazhong University of Science and Technology (HUST), 1037 Luoyu Rd, Wuhan, 430074 China

These authors contributed equally to this work.

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Dr. Shengbo Zhang

Dr. Shengbo Zhang

Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences (China)

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Prof. Haimin Zhang

Prof. Haimin Zhang

Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences (China)

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Xuan Yang

Xuan Yang

School of Chemistry and Chemical Engineering, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, Huazhong University of Science and Technology (HUST), 1037 Luoyu Rd, Wuhan, 430074 China

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Prof. Xintai Su

Prof. Xintai Su

School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China

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Prof. Jiangwei Zhang

Corresponding Author

Prof. Jiangwei Zhang

Science Center of Energy Material and Chemistry, College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010021 China

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Prof. Zhang Lin

Corresponding Author

Prof. Zhang Lin

School of Environment and Energy, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, Guangdong, 510006 P. R. China

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First published: 04 February 2023

Abstract

Atomically dispersed metal catalysts show potential advantages in N2 reduction reaction (NRR) due to their excellent activity and efficient metal utilization. Unfortunately, the reported catalysts usually exhibit unsatisfactory NRR activity due to their poor N2 adsorption and activation. Herein, we report a novel Sn atomically dispersed protuberance (ADP) by coordination with substrate C and O to induce positive charge accumulation on Sn site for improving its N2 adsorption, activation and NRR performance. The extended X-ray absorption fine structure (EXAFS) spectra confirmed the local coordination structure of the Sn ADPs. NRR activity was significantly promoted via Sn ADPs, exhibiting a remarkable NH3 yield (RNH3) of 28.3 μg h−1 mgcat−1 (7447 μg h−1 mgSn−1) at −0.3 V. Furthermore, the enhanced N2Hx intermediates was verified by in situ experiments, yielding consistent results with DFT calculation. This work opens a new avenue to regulate the activity and selectivity of N2 fixation.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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