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单原子(铁基)催化剂:合成与应用

Single-Atom (Iron-Based) Catalysts: Synthesis and Applications.

作者信息

Singh Baljeet, Gawande Manoj B, Kute Arun D, Varma Rajender S, Fornasiero Paolo, McNeice Peter, Jagadeesh Rajenahally V, Beller Matthias, Zbořil Radek

机构信息

CICECO-Aveiro Institute of Materials, University of Aveiro, Aveiro, 3810-193 Portugal.

Department of Industrial and Engineering Chemistry, Institute of Chemical Technology Mumbai-Marathwada Campus, Jalna 431213, Maharashtra, India.

出版信息

Chem Rev. 2021 Nov 10;121(21):13620-13697. doi: 10.1021/acs.chemrev.1c00158. Epub 2021 Oct 13.

DOI:10.1021/acs.chemrev.1c00158
PMID:34644065
Abstract

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which are heterogenized on inert supports such as graphene, porous carbon, and metal oxides. Their thermal stability, electronic properties, and catalytic activities can be controlled via interactions between the single-metal atom center and neighboring heteroatoms such as nitrogen, oxygen, and sulfur. Due to the atomic dispersion of the active catalytic centers, the amount of metal required for catalysis can be decreased, thus offering new possibilities to control the selectivity of a given transformation as well as to improve catalyst turnover frequencies and turnover numbers. This review aims to comprehensively summarize the synthesis of Fe-SACs with a focus on anchoring single atoms (SA) on carbon/graphene supports. The characterization of these advanced materials using various spectroscopic techniques and their applications in diverse research areas are described. When applicable, mechanistic investigations conducted to understand the specific behavior of Fe-SACs-based catalysts are highlighted, including the use of theoretical models.

摘要

负载型单金属原子催化剂(SACs)由孤立的活性金属中心构成,这些活性金属中心负载于诸如石墨烯、多孔碳和金属氧化物等惰性载体上。它们的热稳定性、电子性质和催化活性可通过单金属原子中心与相邻杂原子(如氮、氧和硫)之间的相互作用来控制。由于活性催化中心的原子分散性,催化所需的金属量可以减少,从而为控制特定转化的选择性以及提高催化剂的周转频率和周转数提供了新的可能性。本综述旨在全面总结铁单原子催化剂的合成,重点是将单原子(SA)锚定在碳/石墨烯载体上。描述了使用各种光谱技术对这些先进材料的表征及其在不同研究领域的应用。在适用的情况下,突出了为理解铁单原子催化剂基催化剂的特定行为而进行的机理研究,包括理论模型的使用。

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