通过[Ru(dcbpy)(bpy)2]2+-加入UiO-67框架的肉桂醛的高效光催化发散脱羰硅化反应

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Huahui Wang, Bingbing Qin, Jiazhuo Cai, Yueshi Wu, Cong Zhao, Xiaoyan Bai, Lu Chen*, Yan-Zhong Fan*, Min Zhang and Jiewei Liu*, 
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引用次数: 0

摘要

我们在此开发了一种创新的方法,用于脱羰硅基化使用分子[Ru(dcbpy)(bpy)2]2+ (dcbpy = 2,2 ' -联吡啶-5,5 ' -二羧酸;bpy = 2,2 ' -联吡啶)将UiO-67金属有机骨架(mof)(表示为UiO-67- ru)作为强效非均相催化剂,应用于光热条件下丰富的肉桂醛与硅烷的反应。机理研究表明,硅烷可以在骨架的空腔内被吸收和激活,导致硅基自由基的产生。硅基自由基在脱羰硅基化过程中起关键作用,并进一步与肉桂醛发生氧化硅基化反应生成相应的烯基硅烷。本研究不仅为从丰富的肉桂醛和硅烷中制备烯基硅烷提供了策略,而且为脱羰硅基化mof材料的合理设计提供了有益的启示。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Highly Efficient Photocatalytic Divergent Decarbonylative Silylation with Cinnamaldehyde via a [Ru(dcbpy)(bpy)2]2+-Incorporated UiO-67 Framework

Highly Efficient Photocatalytic Divergent Decarbonylative Silylation with Cinnamaldehyde via a [Ru(dcbpy)(bpy)2]2+-Incorporated UiO-67 Framework

We herein develop an innovative approach for the decarbonylative silylation using a molecular [Ru(dcbpy)(bpy)2]2+ (dcbpy = 2,2′-bipyridyl-5,5′-dicarboxylic acid; bpy = 2,2′-bipyridine) incorporated UiO-67 metal–organic framework (MOFs) (denoted as UiO-67-Ru) as a powerful heterogeneous catalyst, which is then applied in the reaction of abundantly available cinnamaldehydes with silanes under photothermal condition. Mechanistic studies reveal that the silane can be absorbed and activated within the cavities of the framework, leading to the generation of a silyl radical. The silyl radical plays a key role in the decarbonylative silylation process and further goes through oxidative silylation with cinnamaldehydes to generate the corresponding alkenyl silanes. This work not only develops a strategy for the preparation of alkenyl silane from highly abundant cinnamaldehyde and silanes but also affords useful inspiration on the rational design of MOFs materials for the decarbonylative silylation.

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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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