Zn Single-Atom Catalysts Enable the Catalytic Transfer Hydrogenation of α,β-Unsaturated Aldehydes

Jiawen Chen, Yongming Xia, Yuxuan Ling, Xuehui Liu, Shuyuan Li, Xiong Yin*, Lipeng Zhang, Minghui Liang, Yi Ming Yan, Qiang Zheng, Wenxing Chen, Yan Jun Guo, En Hui Yuan, Gaofei Hu, Xiaole Zhou, Leyu Wang*

*此作品的通讯作者

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摘要

Highly active nonprecious-metal single-atom catalysts (SACs) toward catalytic transfer hydrogenation (CTH) of α,β-unsaturated aldehydes are of great significance but still are deficient. Herein, we report that Zn-N-C SACs containing Zn-N3 moieties can catalyze the conversion of cinnamaldehyde to cinnamyl alcohol with a conversion of 95.5% and selectivity of 95.4% under a mild temperature and atmospheric pressure, which is the first case of Zn-species-based heterogeneous catalysts for the CTH reaction. Isotopic labeling, in situ FT-IR spectroscopy, and DFT calculations indicate that reactants, coabsorbed at the Zn sites, proceed CTH via a “Meerwein-Ponndorf-Verley” mechanism. DFT calculations also reveal that the high activity over Zn-N3 moieties stems from the suitable adsorption energy and favorable reaction energy of the rate-determining step at the Zn active sites. Our findings demonstrate that Zn-N-C SACs hold extraordinary activity toward CTH reactions and thus provide a promising approach to explore the advanced SACs for high-value-added chemicals.

源语言英语
期刊Nano Letters
DOI
出版状态已接受/待刊 - 2024

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Chen, J., Xia, Y., Ling, Y., Liu, X., Li, S., Yin, X., Zhang, L., Liang, M., Yan, Y. M., Zheng, Q., Chen, W., Guo, Y. J., Yuan, E. H., Hu, G., Zhou, X., & Wang, L. (已接受/印刷中). Zn Single-Atom Catalysts Enable the Catalytic Transfer Hydrogenation of α,β-Unsaturated Aldehydes. Nano Letters. https://doi.org/10.1021/acs.nanolett.4c00512