Nano-pyramid-type Co-ZnO/NC for hydrogen transfer cascade reaction between alcohols and nitrobenzene

Wu, Chen ¹Zhu, Changyan ²Liu, Kangkai ¹Yang, Shaowei ¹Sun, Yu ¹Zhu, Kai ¹Cao, Yueling ¹Zhuo, Sifei ¹Zhang, Min ²Zhang, Qiuyu ¹Zhang, Hepeng ¹Zhang, Sai¹

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作者信息

1. Northwestern Polytech Univ, Sch Chem & Chem Engn, Xian Key Lab Funct Organ Porous Mat, Xian 710129, Peoples R China
2. Northeast Normal Univ, Fac Chem, Inst Funct Mat Chem, Natl & Local United Engn Lab Power Batteries, Changchun 130024, Peoples R China
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Abstract

The catalytic hydrogen transfer (CHT) cascade reaction between alcohols and nitro- compounds meets green chemistry yet involves high catalyst requirements. Herein, a hierarchical nano-pyramid structure, in which cobalt single atoms (Co SAs) are deposited on highly dispersed ZnO nanoparticles supported by nitrogen-doped carbon (denoted as Co-ZnO/NC), was designed and obtained through pyrolysis of ZnCo-ZIF. The catalyst exhibited excellent catalytic performance toward the CHT cascade reaction, achieving a high nitrobenzene conversion (94 %), imine selectivity (97 %), and turnover frequency (8.8 h-1). This nano-pyramid is a state-ofthe-art non-noble-metal catalyst and is comparable to noble-metal catalysts. Experimental and DFT results revealed that the Co SAs supported on ZnO reduced the reaction energy barrier of hydroxyl dehydrogenation, the first and rate-determining step in this heterogeneous catalysis. Furthermore, Co-ZnO/NC exhibits good recyclability and universality. Our findings offer a new catalyst for Schiff base synthesis and aid understanding of the roles of Zn in ZIF-derived carbon catalysts.

Key words

Catalytic hydrogen transfer/Cascade reaction/Imine synthesis/MOF-derived carbon material/Single atom catalysis

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出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量22

参考文献量51

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