Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N4 sites by carbon-defect engineering

Shengjie Wei, Yibing Sun, Yun-Ze Qiu, Ang Li, Ching-Yu Chiang (), Hai Xiao (), Jieshu Qian () and Yadong Li ()
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Shengjie Wei: Nankai University
Yibing Sun: Nanjing University of Science and Technology
Yun-Ze Qiu: Tsinghua University
Ang Li: Beijing University of Technology
Ching-Yu Chiang: National Synchrotron Radiation Research Center
Hai Xiao: Tsinghua University
Jieshu Qian: Nanjing University of Science and Technology
Yadong Li: Tsinghua University

Nature Communications, 2023, vol. 14, issue 1, 1-15

Abstract: Abstract Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, and revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect engineering of single Fe-N4 sites in ZnO-Carbon nano-reactor, as efficient catalyst in Fenton-like reaction for degradation of phenol. The carbon vacancies are easily constructed adjacent to single Fe-N4 sites during synthesis, facilitating the formation of C-O bonding and lowering the energy barrier of rate-determining-step during degradation of phenol. Consequently, the catalyst Fe-NCv-900 with carbon vacancies exhibits a much improved activity than the Fe-NC-900 without abundant carbon vacancies, with 13.5 times improvement in the first-order rate constant of phenol degradation. The Fe-NCv-900 shows high activity (97% removal ratio of phenol in only 5 min), good recyclability and the wide-ranging pH universality (pH range 3-9). This work not only provides a rational strategy for improving the Fenton-like activity of metal single-atom catalysts, but also deepens the fundamental understanding on how periphery carbon environment affects the property and performance of metal-N4 sites.

Date: 2023
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DOI: 10.1038/s41467-023-43040-5

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