Coordination number engineering of Zn single-atom sites for enhanced transfer hydrogenation performance

被引:23
|
作者
Song, Yaping [1 ]
Guo, Rou [1 ]
Feng, Binbin [1 ]
Fu, Yanghe [1 ,2 ]
Zhang, Fumin [1 ,2 ]
Zhang, Yifei [3 ,4 ]
Chen, De-Li [1 ,2 ]
Zhang, Jiangwei [3 ]
Zhu, Weidong [1 ,2 ]
机构
[1] Zhejiang Normal Univ, Inst Phys Chem, Key Lab, Minist Educ Adv Catalysis Mat, Jinhua 321004, Peoples R China
[2] Zhejiang Normal Univ, Inst Adv Fluorine Containing Mat, Zhejiang Engn Lab Green Synth & Applicat Fluorine, Jinhua 321004, Peoples R China
[3] Inner Mongolia Univ, Coll Chem & Chem Engn, Sci Ctr Energy Mat & Chem, Hohhot 010021, Peoples R China
[4] Shenyang Normal Univ, Coll Chem & Chem Engn, Shenyang 110034, Peoples R China
基金
中国国家自然科学基金;
关键词
Metal-organic framework; Single-atom catalysts; Nitrogen coordination number; Transfer hydrogenation; Electron transfer; N-DOPED CARBON; SELECTIVE HYDROGENATION; CHEMOSELECTIVE CATALYSTS; POROUS CARBON; ACTIVE-SITES; C CATALYSTS; REDUCTION; EFFICIENT; ZIF-8;
D O I
10.1016/j.cej.2023.142920
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
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 py-rolysis 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.
引用
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页数:11
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