Isomorphous substitution in CaAl-hydrotalcite to construct high density single-atom catalysts for selective N-Heteroarene hydrogenation

IF 15.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis Pub Date : 2025-03-01 DOI:10.1016/S1872-2067(24)60217-2

Jieting He , Yu Liang , Binbin Zhao , Lei Liu , Qian He , Dingsheng Wang , Jinxiang Dong

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Abstract

Metal oxides as support for constructing precious metal single-atom catalysts hold great promise for a wide range of industrial applications, but achieving a high-loading of thermally stable metal single atoms on such supports has been challenging. Herein, we report an innovative strategy for the fabrication of high-density single-atoms (Rh, Ru, Pd) catalysts on CaAl-layered double hydroxides (https://xueshu.baidu.com/usercenter/paper/show?paperid=acded962fe3d910ccbe68cc7a756fa3a&site=xueshu_seCaAl-LDH) via isomorphous substitution. The Rh species have occupied Ca²⁺ vacancies within CaAl-LDH laminate by ion-exchange, facilitating a substantial loading of isolated Rh single-atoms. Such catalysts displayed superior performance in the selective hydrogenation to quinoline, pivotal for liquid organic hydrogen storage, and the universality for the hydrogenation of N-heterocyclic aromatic hydrocarbons was also verified. Combining the experimental results and density functional theory calculations, the pathway of quinoline hydrogenation over Rh₁CaAl-LDH was proposed. This synthetic strategy marks a significant advancement in the field of single-atom catalysts, expanding their horizons in green chemical processes.

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来源期刊

Chinese Journal of Catalysis 工程技术-工程：化工

CiteScore

25.80

自引率

10.30%

发文量

235

审稿时长

1.2 months

期刊介绍： The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.