Role of “post-coordination interaction” boosted performance of rare-earth based MOFs derived catalyst for hydrogenation-alkylation cascade reaction

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL
Danfeng Deng , Wenjing Song , Qiang Li , Weizuo Li , Xin Wang
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引用次数: 0

Abstract

Post-coordination interactions (abbreviated as PCI) play an essential role in the synthesis and optimization of catalysts by influencing their coordination environment, stabilizing reaction intermediates, tuning activity, and allowing for dynamic behavior. In this work, a LaOCl incorporated into carbon-nitrogen supported metallic Co and CoFe alloy catalyst (termed as CF/L-CN-PCI) via PCI strategy has been synthesized. This catalyst was then utilized in a cascade reaction involving nitroarenes and benzyl alcohol. The developed CF/L-CN-PCI catalyst exhibits higher catalytic selectivity compared to CF/L-CN-IWI catalyst prepared by IWI method in cascade reactions. Additionally, this catalyst offers ease of separation and demonstrates good catalytic cycle stability. Various characterization techniques and control experiments were employed to validate the reasons for the enhanced catalytic performance and to investigate the key issues such as the rate-determining step during the reaction process. We hope that this catalyst preparation method can serve as a reference for the development of other superior catalysts and their application in different reactions.

Abstract Image

稀土基mof衍生催化剂的“后配位相互作用”提高了加氢-烷基化级联反应的性能
后配位相互作用(简称PCI)通过影响催化剂的配位环境、稳定反应中间体、调节活性和允许动态行为,在催化剂的合成和优化中起着至关重要的作用。本研究合成了一种通过PCI策略将LaOCl掺入碳氮负载的金属Co和CoFe合金催化剂(CF/L-CN-PCI)中。然后将该催化剂用于涉及硝基芳烃和苯甲醇的级联反应。与IWI法制备的CF/L-CN-IWI催化剂相比,所制备的CF/L-CN-PCI催化剂在级联反应中具有更高的催化选择性。此外,该催化剂易于分离,并表现出良好的催化循环稳定性。采用各种表征技术和控制实验来验证催化性能增强的原因,并研究反应过程中的速率决定步骤等关键问题。我们希望这种催化剂的制备方法可以为其他优良催化剂的开发及其在不同反应中的应用提供参考。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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