次表层过渡金属的导电催化作用

IF 16.3 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES National Science Review Pub Date : 2024-01-10 DOI:10.1093/nsr/nwae015
Xin Deng, Caiyan Zheng, Yangsheng Li, Zeyu Zhou, Jiamin Wang, Yihua Ran, Zhenpeng Hu, Fan Yang, Landong Li
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引用次数: 0

摘要

一个多世纪以来,催化的本质一直受到人们的热烈追捧,目前的研究重点是了解活性中心及其电子结构。本文提出了导电催化的概念,并通过理论模拟和实验观察进行了验证。构建了含有埋藏的催化活性过渡金属和暴露的催化惰性主族金属的金属体系,并揭示了它们之间通过金属键产生的电子相互作用。通过电子相互作用,地下过渡金属(钯或铑)的催化特性可以转移到最外层的主族金属(铝或镁)上,用于半加氢、铃木偶联和加氢甲酰化等几种重要的转化。催化力与磁力和静电力类似,具有传导性。导电催化的概念对活性中心的传统定义提出了挑战,催化的电子性质也更容易理解。它可能为保护传统活性中心免受毒害或浸蚀提供了新的机会,并允许导电层对其催化特性进行精确调节。
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Conductive catalysis by subsurface transition metals
The nature of catalysis is being hotly pursued for over a century, and current research is focused on understanding active centers and their electronic structures. Herein, the concept of conductive catalysis is proposed and verified by theoretical simulations and experimental observations. Metallic systems containing buried catalytically active transitional metals and exposed catalytically inert main group metals are constructed, and the electronic interaction between them via metallic bonding is disclosed. Through the electronic interaction, the catalytic properties of subsurface transitional metals (Pd or Rh) can be transferred to outermost main group metals (Al or Mg) for several important transformations like semi-hydrogenation, Suzuki-coupling and hydroformylation. The catalytic force is conductive, in analogy with the magnetic force and electrostatic force. The traditional definition of active centers is challenged by the concept of conductive catalysis and the electronic nature of catalysis is more easily understood. It might provide new opportunities for shielding traditional active centers against poisoning or leaching and allow for precise regulation of their catalytic properties by the conductive layer.
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来源期刊
National Science Review
National Science Review MULTIDISCIPLINARY SCIENCES-
CiteScore
24.10
自引率
1.90%
发文量
249
审稿时长
13 weeks
期刊介绍: National Science Review (NSR; ISSN abbreviation: Natl. Sci. Rev.) is an English-language peer-reviewed multidisciplinary open-access scientific journal published by Oxford University Press under the auspices of the Chinese Academy of Sciences.According to Journal Citation Reports, its 2021 impact factor was 23.178. National Science Review publishes both review articles and perspectives as well as original research in the form of brief communications and research articles.
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