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A “competitive occupancy”strategy toward Co-N4 single-atom catalysts embedded in 2D TiN/rGO sheets for high-efficient and stable aromatic nitroreduction

Abstract

The single-atom catalysts (SACs) have been promising in catalytic fields, but the controllable synthesis of SACs with high stability remain challenging. Here, we show a robust strategy toward the highly-efficient and stable SACs based on “competitive occupancy” of two metal (M) species on graphite oxide (GO). The abundant M1 (Ti) species predominantly occupy more groups of GO, thus leaving a tiny of groups at the gaps of M1 species to combine with M2 (Co2+ etc.) species, and consequently, guaranteeing the formation of Co-N4 SACs embedded in 2D TiN/rGO sheets during the nitridation. Also, the TiN can act as a “spacer” to prevent Co-N4 from aggregation, thus improving the stability of the catalyst. The Co-N4/TiN-rGO exhibits outstanding catalytic performance for fast conversion of high-concentrated aromatic nitro compounds (0.3~2 mM) into amino compounds and excellent re-cycled ability, being at the forefront of reported catalysts. In contrast, the TiN/rGO has no obvious activity, and Co4N-rGO prepared without competition of Ti shows poor activity and stability, which indicate vital role of Co-N4 and TiN for remarkable catalytic ability of Co-N4/TiN-rGO. The reaction mechanism is also proposed based on the theoretical calculation. The strategy is indicative to design Ni (Fe, Cr, Cu)-based SACs .

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Supplementary files

Article information


Submitted
12 Dec 2019
Accepted
05 Feb 2020
First published
06 Feb 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

A “competitive occupancy”strategy toward Co-N4 single-atom catalysts embedded in 2D TiN/rGO sheets for high-efficient and stable aromatic nitroreduction

Y. Gu, A. Wu, L. Wang, D. Wang, Y. Xie, H. Yan, P. Yu, C. Tian, F. Sun and H. Fu, J. Mater. Chem. A, 2020, Accepted Manuscript , DOI: 10.1039/C9TA13615K

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