催化作用
转移加氢
协调数
金属有机骨架
联氨(抗抑郁剂)
化学
接受者
金属
热解
部分
电子转移
氮气
配位复合体
Atom(片上系统)
纳米颗粒
无机化学
材料科学
纳米技术
光化学
物理化学
立体化学
离子
有机化学
钌
计算机科学
嵌入式系统
物理
吸附
色谱法
凝聚态物理
作者
Yaping Song,Rou Guo,Feng Bao,Yanghe Fu,Fumin Zhang,Yifei Zhang,De-Li Chen,Jiangwei Zhang,Weidong Zhu
标识
DOI:10.1016/j.cej.2023.142920
摘要
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 analysis uncover that appropriately lowering the coordination number increases the electron density of Zn single atoms and simultaneously introduces H-acceptor sites, which cooperatively contribute to the enhancement of the performance for transfer hydrogenation.
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