气相金属催化反应综述

doi:10.1016/S1872-2067(17)62782-7

催化学报 ›› 2017, Vol. 38 ›› Issue (9): 1515-1527.DOI: 10.1016/S1872-2067(17)62782-7

气相金属催化反应综述

李晓娜^a, 邹秀平^a,b, 何圣贵^a

a 中国科学院化学研究所, 动态与稳态结构实验室, 北京 100190;
b 华南理工大学, 化学与化工学院, 广东广州 510641

收稿日期:2016-11-30 修回日期:2017-01-05 出版日期:2017-09-18 发布日期:2017-09-06
通讯作者: 何圣贵
基金资助:
国家自然科学基金（21303215，21325314，21573246）；重大研究计划（2013CB834603）；中科院青促会基金（2016030）.

Metal-mediated catalysis in the gas phase:A review

Xiao-Na Li^a, Xiu-Ping Zou^a,b, Sheng-Gui He^a

a Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China;
b School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China

Received:2016-11-30 Revised:2017-01-05 Online:2017-09-18 Published:2017-09-06
Contact: 10.1016/S1872-2067(17)62782-7
Supported by:
This work was supported by the National Natural Science Foundation of China (21303215, 21325215, 21573246), the Major Research Plan of China (No. 2013CB834603) and the grant from the Youth Innovation Promotion Association, Chinese Academy of Sciences (2016030).

摘要/Abstract

摘要：

金属催化剂在工业、环境、能源以及生物等过程具有重要的应用.设计具有特定活性、环境友好型以及室温下具有反应活性的催化剂，需要在分子水平对金属催化剂的基元步骤，活性位点的结构以及催化反应微观机理有充分的认识.然而，由于宏观催化剂表面结构异常复杂，催化反应常受到溶剂、压力、金属颗粒团聚、催化剂表面缺陷等因素的干扰，利用现有实验仪器，从微观角度探索金属催化反应机理仍具有较大挑战，因此，对金属催化剂活性位的结构以及反应微观机理的认识还不十分清楚.
质谱方法结合现代量子化学理论计算，提供了在气相条件下实验探索化学反应微观机理的有力工具，团簇反应可在隔离外界条件、可控以及可重复条件下进行，可以排除一些难以控制因素的干扰，可在化学键和分子结构水平认识金属活性位的结构以及催化反应的微观机理.气相金属团簇离子可用多种实验方法制备，与反应物分子反应后可利用多种质谱仪器探测，根据实验上所得的具有反应活性的团簇，结合现代量子化学理论模拟，得到金属催化反应的基元步骤以及微观反应机理信息，所得反应机理信息为宏观催化剂的设计提供重要理论研究基础.
本综述总结了团簇实验上已经探测到的金属单原子离子、金属团簇、金属氧化物团簇和金属化合物催化的气相反应.反应物分子囊括了大量的无机和有机分子，包括CO，H₂，CH₄，C₂H₂，C₂H₄，C₆H₆，CH₃OH，HCOOH，CH₃COOH等.本综述主要介绍了以下三类催化反应：（1） CO催化氧化；（2） CH₄催化转化；（3）催化脱羧反应，并重点关注贵金属单原子掺杂团簇独特的催化反应性.单原子催化剂可最大限度地利用有限的贵金属.在化学反应方面，单原子催化剂具有特异的反应活性，选择性以及稳定性.本综述对气相团簇反应中报道的两个重要的贵金属单原子掺杂团簇的催化反应进行了详细介绍：（1）金原子掺杂的AuAl₃O_3-5⁺团簇为首次报道的可以利用分子氧催化氧化CO的团簇单原子催化剂，我们对Au原子起催化作用的本质原因进行了介绍：（2）铂原子掺杂的PtAl₃O_5-7^-团簇能利用分子氧催化氧化CO，该研究提出了"电负性阶梯"效应来解释Pt原子催化的微观机理，且此效应有望对大部分贵金属适用.此外，本综述对CO催化氧化反应和CH₄催化转化反应的研究现状以及尚未解决的问题进行了剖析.相比CO的催化氧化反应，科学家对CH₄催化转化反应机理的认识还不够深入，还需要进一步实验研究，而团簇单原子催化剂有望在此领域有所突破.

关键词: 金属催化, 团簇, 单原子催化剂, 一氧化碳, 甲烷

Abstract:

This review summarizes a variety of experimentally identified gas-phase catalytic cycles, all of which are mediated by atomic metal ions, bare metal clusters, metal oxide clusters or metal com-plexes. Emphasis is placed on the latest advances in the unique catalytic reactivity of clus-ter-confined single noble metal atoms. The cycles discussed in this paper cover a wide range of inorganic and organic molecules. The use of start-of-the-art mass spectrometric instrumentation in conjunction with quantum chemistry calculations is also reported, as these techniques have deter-mined the mechanistic details of the elementary steps of such catalytic cycles. The important role of gas-phase data in guiding the rational design of better-performing catalysts in related condensed phase reactions is also examined. In particular, this review focuses on the following three topics:(1) the catalytic oxidation of carbon monoxide, (2) the catalytic functionalization of methane, and (3) catalytic decarboxylation.

Key words: Metal catalysis, Clusters, Single atom catalysts, Carbon monoxide, Methane

李晓娜, 邹秀平, 何圣贵. 气相金属催化反应综述[J]. 催化学报, 2017, 38(9): 1515-1527.

Xiao-Na Li, Xiu-Ping Zou, Sheng-Gui He. Metal-mediated catalysis in the gas phase:A review[J]. Chinese Journal of Catalysis, 2017, 38(9): 1515-1527.

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气相金属催化反应综述

Metal-mediated catalysis in the gas phase:A review

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