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纳米金刚石及其衍生物上的原子分散金属催化剂:合成与催化应用。

Atomically dispersed metal catalysts on nanodiamond and its derivatives: synthesis and catalytic application.

作者信息

Chen Xiaowen, Jia Zhimin, Huang Fei, Diao Jiangyong, Liu Hongyang

机构信息

School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, P. R. China.

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, P. R. China.

出版信息

Chem Commun (Camb). 2021 Nov 4;57(88):11591-11603. doi: 10.1039/d1cc05202k.

DOI:10.1039/d1cc05202k
PMID:34657938
Abstract

Atomically dispersed metal catalysts (ADMCs) have attracted increasing interest in the field of heterogeneous catalysis. As sub-nanometric catalysts, ADMCs have exhibited remarkable catalytic performance in many reactions. ADMCs are classified into two categories: single atom catalysts (SACs) and atomically dispersed clusters with a few atoms. To stabilize the highly active ADMCs, nanodiamond (ND) and its derivatives (NDDs) are promising supports. In this Feature Article, we have introduced the advantages of NDDs with a highly curved surface and tunable surface properties. The controllable defective sites and oxygen functional groups are known as the anchoring sites for ADMCs. Tunable surface acid-base properties enable ADMCs supported on NDDs to exhibit unique selectivity towards target products and an extended lifetime in many reactions. In addition, we have firstly overviewed the recent advances in the synthesis strategies for effectively fabricating ADMCs on NDDs, and further discussed how to achieve the atomic dispersion of metal precursors and stabilize the as-formed metal atoms against migration and agglomeration based on NDDs. And then, we have also systematically summarized the advantages of ADMCs supported on NDDs in reactions, including hydrogenation, dehydrogenation, aerobic oxidation and electrochemical reaction. These reactions can also effectively guide the design of ADMCs. The recent progress in understanding the effect of structure of active centers and metal-support interactions (MSIs) on the catalytic performance of ADMCs is particularly highlighted. At last, the possible research directions in ADMCs are forecasted.

摘要

原子分散金属催化剂(ADMCs)在多相催化领域引起了越来越多的关注。作为亚纳米级催化剂,ADMCs在许多反应中表现出卓越的催化性能。ADMCs分为两类:单原子催化剂(SACs)和含有少数原子的原子分散簇。为了稳定高活性的ADMCs,纳米金刚石(ND)及其衍生物(NDDs)是很有前景的载体。在这篇专题文章中,我们介绍了具有高度弯曲表面和可调表面性质的NDDs的优势。可控的缺陷位点和氧官能团被认为是ADMCs的锚定位点。可调的表面酸碱性质使负载在NDDs上的ADMCs在许多反应中对目标产物表现出独特的选择性和延长的寿命。此外,我们首先概述了在NDDs上有效制备ADMCs的合成策略的最新进展,并进一步讨论了如何基于NDDs实现金属前驱体的原子分散以及稳定所形成的金属原子以防止迁移和团聚。然后,我们还系统地总结了负载在NDDs上的ADMCs在氢化、脱氢、有氧氧化和电化学反应等反应中的优势。这些反应也可以有效地指导ADMCs的设计。特别强调了在理解活性中心结构和金属-载体相互作用(MSIs)对ADMCs催化性能影响方面的最新进展。最后,预测了ADMCs可能的研究方向。

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