Graphitic phosphorus coordinated single Fe atoms for hydrogenative transformations

Xiangdong Long, Zelong Li, Guang Gao, Peng Sun, Jia Wang, Bingsen Zhang, Jun Zhong, Zheng Jiang and Fuwei Li ()
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Xiangdong Long: Chinese Academy of Sciences
Zelong Li: Lanzhou University
Guang Gao: Chinese Academy of Sciences
Peng Sun: Chinese Academy of Sciences
Jia Wang: Chinese Academy of Sciences
Bingsen Zhang: Chinese Academy of Sciences
Jun Zhong: Soochow University
Zheng Jiang: Chinese Academy of Science
Fuwei Li: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-12

Abstract: Abstract Single-atom metal-nitrogen-carbon (M-N-C) catalysts have sparked intensive interests, however, the development of an atomically dispersed metal-phosphorus-carbon (M-P-C) catalyst has not been achieved, although molecular metal-phosphine complexes have found tremendous applications in homogeneous catalysis. Herein, we successfully construct graphitic phosphorus species coordinated single-atom Fe on P-doped carbon, which display outstanding catalytic performance and reaction generality in the heterogeneous hydrogenation of N-heterocycles, functionalized nitroarenes, and reductive amination reactions, while the corresponding atomically dispersed Fe atoms embedded on N-doped carbon are almost inactive under the same reaction conditions. Furthermore, we find that the catalytic activity of graphitic phosphorus coordinated single-atom Fe sharply decreased when Fe atoms were transformed to Fe clusters/nanoparticles by post-impregnation Fe species. This work can be of fundamental interest for the design of single-atom catalysts by utilizing P atoms as coordination sites as well as of practical use for the application of M-P-C catalysts in heterogeneous catalysis.

Date: 2020
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DOI: 10.1038/s41467-020-17903-0

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