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Title: Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction

Abstract

Artificial nitrogen fixation through the nitrogen reduction reaction (NRR) under ambient conditions is a potentially promising alternative to the traditional energy-intensive Haber–Bosch process. For this purpose, efficient catalysts are urgently required to activate and reduce nitrogen into ammonia. Herein, by the combination of experiments and first-principles calculations, we demonstrate that copper single atoms, attached in a porous nitrogen-doped carbon network, provide highly efficient NRR electrocatalysis, which compares favorably with those previously reported. Benefiting from the high density of exposed active sites and the high level of porosity, the Cu SAC exhibits high NH 3 yield rate and Faradaic efficiency (FE), specifically ~53.3 μg$$_{NH_3}$$ h –1 mg cat –1 and 13.8% under 0.1 M KOH, ~49.3 μg$$_{NH_3}$$ h –1 mg cat –1 and 11.7% under 0.1 M HCl, making them truly pH-universal. They also show good stability with little current attenuation over 12 h of continuous operation. Cu–N 2 coordination is identified as the efficient active sites for the NRR catalysis.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [1]; ORCiD logo [1]; ORCiD logo [1];  [5]; ORCiD logo [2]; ORCiD logo [6]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [1]
  1. National Univ. of Singapore, Singapore (Singapore). Dept. of Materials Science and Engineering
  2. National Univ. of Singapore, Singapore (Singapore). Dept. of Physics
  3. Southern Univ. of Science and Technology (SUSTech), Shenzhen (China)
  4. Inst. of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR), Jurong Island (Singapore)
  5. Inst. of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR), Jurong Island (Singapore)
  6. National Univ. of Singapore, Singapore (Singapore). Dept. of Mechanical Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1570669
Report Number(s):
BNL-212188-2019-JAAM
Journal ID: ISSN 2155-5435
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Name: ACS Catalysis; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Cu single atom catalysts; nitrogen-doped porous carbon; nitrogen

Citation Formats

Zang, Wenjie, Yang, Tong, Zou, Haiyuan, Xi, Shibo, Zhang, Hong, Liu, Ximeng, Kou, Zongkui, Du, Yonghua, Feng, Yuan Ping, Shen, Lei, Duan, Lele, Wang, John, and Pennycook, Stephen J. Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction. United States: N. p., 2019. Web. doi:10.1021/acscatal.9b02944.
Zang, Wenjie, Yang, Tong, Zou, Haiyuan, Xi, Shibo, Zhang, Hong, Liu, Ximeng, Kou, Zongkui, Du, Yonghua, Feng, Yuan Ping, Shen, Lei, Duan, Lele, Wang, John, & Pennycook, Stephen J. Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction. United States. doi:10.1021/acscatal.9b02944.
Zang, Wenjie, Yang, Tong, Zou, Haiyuan, Xi, Shibo, Zhang, Hong, Liu, Ximeng, Kou, Zongkui, Du, Yonghua, Feng, Yuan Ping, Shen, Lei, Duan, Lele, Wang, John, and Pennycook, Stephen J. Mon . "Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction". United States. doi:10.1021/acscatal.9b02944.
@article{osti_1570669,
title = {Copper Single Atoms Anchored in Porous Nitrogen-Doped Carbon as Efficient pH-Universal Catalysts for the Nitrogen Reduction Reaction},
author = {Zang, Wenjie and Yang, Tong and Zou, Haiyuan and Xi, Shibo and Zhang, Hong and Liu, Ximeng and Kou, Zongkui and Du, Yonghua and Feng, Yuan Ping and Shen, Lei and Duan, Lele and Wang, John and Pennycook, Stephen J.},
abstractNote = {Artificial nitrogen fixation through the nitrogen reduction reaction (NRR) under ambient conditions is a potentially promising alternative to the traditional energy-intensive Haber–Bosch process. For this purpose, efficient catalysts are urgently required to activate and reduce nitrogen into ammonia. Herein, by the combination of experiments and first-principles calculations, we demonstrate that copper single atoms, attached in a porous nitrogen-doped carbon network, provide highly efficient NRR electrocatalysis, which compares favorably with those previously reported. Benefiting from the high density of exposed active sites and the high level of porosity, the Cu SAC exhibits high NH3 yield rate and Faradaic efficiency (FE), specifically ~53.3 μg$_{NH_3}$ h–1 mgcat–1 and 13.8% under 0.1 M KOH, ~49.3 μg$_{NH_3}$ h–1 mgcat–1 and 11.7% under 0.1 M HCl, making them truly pH-universal. They also show good stability with little current attenuation over 12 h of continuous operation. Cu–N2 coordination is identified as the efficient active sites for the NRR catalysis.},
doi = {10.1021/acscatal.9b02944},
journal = {ACS Catalysis},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {10}
}

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This content will become publicly available on October 14, 2020
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