Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation

Yuan Pan, Yinjuan Chen, Konglin Wu, Zheng Chen, Shoujie Liu, Xing Cao, Weng-Chon Cheong, Tao Meng, Jun Luo, Lirong Zheng, Chenguang Liu (), Dingsheng Wang, Qing Peng, Jun Li and Chen Chen ()
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Yuan Pan: Tsinghua University
Yinjuan Chen: Tsinghua University
Konglin Wu: Tsinghua University
Zheng Chen: Tsinghua University
Shoujie Liu: Tsinghua University
Xing Cao: Tsinghua University
Weng-Chon Cheong: Tsinghua University
Tao Meng: Beijing Institute of Technology
Jun Luo: Tianjin University of Technology
Lirong Zheng: Chinese Academy of Sciences
Chenguang Liu: China University of Petroleum (East China)
Dingsheng Wang: Tsinghua University
Qing Peng: Tsinghua University
Jun Li: Tsinghua University
Chen Chen: Tsinghua University

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract Atomically dispersed metal-N-C structures are efficient active sites for catalyzing benzene oxidation reaction (BOR). However, the roles of N and C atoms are still unclear. We report a polymerization-regulated pyrolysis strategy for synthesizing single-atom Fe-based catalysts, and present a systematic study on the coordination effect of Fe-NxCy catalytic sites in BOR. The special coordination environment of single-atom Fe sites brings a surprising discovery: Fe atoms anchored by four-coordinating N atoms exhibit the highest BOR performance with benzene conversion of 78.4% and phenol selectivity of 100%. Upon replacing coordinated N atoms by one or two C atoms, the BOR activities decrease gradually. Theoretical calculations demonstrate the coordination pattern influences not only the structure and electronic features, but also the catalytic reaction pathway and the formation of key oxidative species. The increase of Fe-N coordination number facilitates the generation and activation of the crucial intermediate O=Fe=O species, thereby enhancing the BOR activity.

Date: 2019
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DOI: 10.1038/s41467-019-12362-8

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