Heteroatom Enhanced Metal‐free Catalytic Performance of Carbocatalysts for Organic Transformation
Heteroatom Enhanced Metal‐free Catalytic Performance of Carbocatalysts for Organic Transformation
复制标题
杂原子增强有机转化碳催化剂的无金属催化性能
DOI：
10.1002/cctc.201900336
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发表时间：
2019
期刊：
影响因子：
4.5
通讯作者：
Shuang Gao
中科院分区：
文献类型：
--
作者：
Sen S.Shang;Shuang Gao
从基础研究和应用研究的角度来看，开发和设计用于化学转化的无金属催化剂一直是一个迷人的主题。除了其独特的优势，如更低的成本，更高的生物相容性和可靠性，从而更高的可持续性，无金属材料往往出乎意料地呈现出与传统金属催化剂不同的反应途径或机制。因此，无金属催化剂彻底改变并扩展了催化平台。其中，碳是一类典型的非金属材料。迄今为止，一系列元素（例如，B、N、P或S）作为杂原子掺杂剂已经使原始碳具有增强的性能和甚至新的化学官能度。它被认为是由于调制的电性能和表面物理化学特征起源于结构扭曲和电荷密度的变化。在这篇小综述中，我们概述了杂原子掺杂的碳催化剂在氧化、氧化偶联、还原和氢化反应中的催化应用，特别强调了杂原子的作用，从而提高了性能。这篇小综述强调了结构与活性的相关性，从而指导了先进的无金属有机合成催化剂的合理设计。讨论了催化剂活性中心的一些争议和催化剂设计中的挑战。
The exploitation and design of metal‐free catalysts for chemical transformation is always a fascinating theme from the prospective of fundamental and applied research. In addition to their distinct advantages such as lower cost, higher biocompatibility and reliability and thus higher sustainability, metal‐free materials often unexpectedly render different reaction pathway or mechanism from conventional metal catalysts. As a consequence, metal‐free catalysts have revolutionized and expanded the platform of catalysis. Among them, carbons are a typical class of nonmetallic materials. To date, a series of elements (e. g., B, N, P or S) as heteroatom dopants have equipped pristine carbons with enhanced performance and even new chemical functionality. It was proposed to attribute to modulated electrical properties and surface physicochemical features originated from structural distortions and changes of charge densities. In this minireview, we overviewed the catalytic application of heteroatom‐doped carbocatalysts in oxidation, oxidative coupling, reduction and hydrogenation reactions with special emphasis on the role of heteroatoms and consequently enhanced performance. This minireview highlights the structure‐activity correlations, thereby directing the rational design of advanced metal‐free catalysts for organic synthesis. Some controversies about active sites and challenges in catalyst design are also discussed here.