Boosting Electroreduction Kinetics of Nitrogen to Ammonia via Atomically Dispersed Sn Protuberance-Reference-Cited by-同舟云学术

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

Published:2023-02-20 Issue:13 Volume:135 Page:
ISSN:0044-8249
Container-title:Angewandte Chemie
language:en
Short-container-title:Angewandte Chemie

Author:

Zhang Lijuan¹²,Zhou Hanfeng¹,Yang Xiaoju³,Zhang Shengbo⁴,Zhang Haimin⁴,Yang Xuan³,Su Xintai¹,Zhang Jiangwei⁵,Lin Zhang¹^ORCID

Affiliation:

1. 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

2. 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

3. 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

4. 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)

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

Abstract

AbstractAtomically 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.

Funder

National Natural Science Foundation of China

Dalian High-Level Talent Innovation Program

Shenzhen Key Laboratory of Neuropsychiatric Modulation

Key Technologies Research and Development Program

Guangdong Provincial Applied Science and Technology Research and Development Program

Publisher

Wiley

Subject

General Medicine

Link

https://onlinelibrary.wiley.com/doi/pdf/10.1002/ange.202217473

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