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

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.

doi:10.1021/acscatal.9b02944

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

Journal Article · Mon Oct 14 00:00:00 EDT 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b02944· OSTI ID:1570669

^[1]; Yang, Tong ^[2]; Zou, Haiyuan ^[3]; Xi, Shibo ^[4]; Zhang, Hong ^[1];

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^[1]; Du, Yonghua ^[5];

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National Univ. of Singapore, Singapore (Singapore). Dept. of Materials Science and Engineering
National Univ. of Singapore, Singapore (Singapore). Dept. of Physics
Southern Univ. of Science and Technology (SUSTech), Shenzhen (China)
Inst. of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR), Jurong Island (Singapore)
Inst. of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR), Jurong Island (Singapore)
National Univ. of Singapore, Singapore (Singapore). Dept. of Mechanical Engineering

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 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–N₂ coordination is identified as the efficient active sites for the NRR catalysis.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1570669

Report Number(s):: BNL-212188-2019-JAAM

Journal Information:: ACS Catalysis, Vol. 9, Issue 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 196 works

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