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Coordination number engineering of Zn single-atom sites for enhanced transfer hydrogenation performance by Yaping Song; Rou Guo; Binbin Feng; Yanghe Fu; Fumin Zhang; Yifei Zhang; De-Li Chen; Jiangwei Zhang; Weidong Zhu is a Engineering article available to read on EtoBox.

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Metal single-atom catalysts (SACs) have great potential to replace traditional nanoparticle catalysts in practical applications, however, the task-specific construction of SACs containing metal–nitrogen (M−N) moiety with tunable M−N coordination number remains a colossal challenging issue. Herein, we report a facile strategy to modulate the s-band of Zn by constructing N-coordinated Zn SACs (denoted as Zn–N–C–T, T stands for the pyrolysis temperature) with tunable nitrogen coordination number (denoted as Zn–Nx, x = 2, 3, and 4) and Zn loadings (ranging from 0.8 to 6.8% by weight) via a metal–organic framework-mediated pyrolysis method. The catalytic activity of Zn–N–C–T is found to be closely related to the coordination number of Zn single atomic sites for the transfer hydrogenation of nitroarene to arylamine, using hydrazine hydrate as a hydrogen source under environmental benign conditions, among which the under-coordinated Zn–N3 with defect and asymmetric electron distribution in Zn–N–C–1223 exhibits the best catalytic activity, followed by lower-coordinated Zn–N2 with defect in Zn–N–C–1273 and saturated coordination Zn–N4 in Zn–N–C–1123. Experimental results and theoretical an

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Author

Yaping Song; Rou Guo; Binbin Feng; Yanghe Fu; Fumin Zhang; Yifei Zhang; De-Li Chen; Jiangwei Zhang; Weidong Zhu

Publisher

Elsevier BV

Published

2023

Language

EN

Field

Engineering (Physical Sciences)