异核氧化物团簇与小分子的反应研究

赵艳霞; 何圣贵

doi:10.7536/PC151024

化学进展 ›› 2016, Vol. 28 ›› Issue (4) :401-414 DOI: 10.7536/PC151024

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异核氧化物团簇与小分子的反应研究

赵艳霞, 何圣贵*

作者信息 +

Reactivity of Heteronuclear Oxide Clusters with Small Molecules

Zhao Yanxia, He Shenggui*

Author information +

文章历史 +

摘要

研究气态条件下异核氧化物团簇与小分子的反应,可从分子水平揭示多组分氧化物催化剂中的各组分在化学转化中的作用,为理性设计和氧化物催化剂改进提供理论基础.本文综述了异核氧化物团簇活化和转化小分子的研究新进展,讨论了异核掺杂引起的氧化物团簇局部电荷环境、局部自旋环境以及成键结构的变化对一些重要活性氧物种的反应性的调控,展示了氧化物团簇掺杂贵金属原子所带来的奇特化学反应以及新的反应机理.

Abstract

Gas phase study of the chemical reactions between heteronuclear oxide clusters and small molecules permits to address the behavior of oxides composed of multiple components in catalytic reactions at a strictly molecular level. In this review, we summarize the recent progress in activation and transformation of small molecules by heteronuclear oxide clusters. The local charge, local spin, and structural effects on the reactivity of important reactive oxygen species are discussed. The novel reaction pathways and reaction mechanisms appearing after doping with noble metals are also presented.

Contents
1 Introduction
2 Reactivity of heteronuclear oxide clusters doping with non-noble metals
2.1 Tune the local charge on atomic oxygen radicals
2.2 Tune the local spin on atomic oxygen radicals
2.3 Tune the reactivity of peroxide ions
3 Reactivity of heteronuclear oxide clusters doping with noble metals
3.1 The promotion role of noble metal atoms
3.2 The dominant role of noble metal atoms
3.3 The single atom catalysis
4 Conclusion and outlook

Graphical abstract

关键词

原子团簇 / 异核氧化物 / 活性氧物种 / 贵金属 / 反应机理

Key words

atomic clusters / heteronuclear oxides / reactive oxygen species / noble metals / reaction mechanisms

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赵艳霞, 何圣贵. 异核氧化物团簇与小分子的反应研究[J]. 化学进展, 2016, 28(4): 401-414 DOI:10.7536/PC151024

Zhao Yanxia, He Shenggui. Reactivity of Heteronuclear Oxide Clusters with Small Molecules[J]. Progress in Chemistry, 2016, 28(4): 401-414 DOI:10.7536/PC151024

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