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化学进展 2020, Vol. 32 Issue (8): 1172-1183 DOI: 10.7536/PC200434 前一篇   后一篇

• 综述 •

缺陷与催化

谢超1, 周波1, 周灵1, 吴雨洁1, 王双印1,**()   

  1. 1. 湖南大学化学生物传感与计量学国家重点实验室 湖南省石墨烯材料与器件重点实验室 湖南大学化学化工学院 长沙 410082
  • 收稿日期:2020-03-12 修回日期:2020-04-03 出版日期:2020-08-24 发布日期:2020-04-23
  • 通讯作者: 王双印
  • 基金资助:
    国家自然科学基金项目(51402100); 国家自然科学基金项目(21573066); 国家自然科学基金项目(U19A2017); 国家自然科学基金项目(21825201); 湖南省自然科学基金项目(2016JJ1006); 湖南省自然科学基金项目(2016TP1009)
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Defect with Catalysis

Chao Xie1, Bo Zhou1, Ling Zhou1, Yujie Wu1, Shuangyin Wang1,**()   

  1. 1. State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Hunan Provincial Key Laboratory for Graphene Materials and Devices, School of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
  • Received:2020-03-12 Revised:2020-04-03 Online:2020-08-24 Published:2020-04-23
  • Contact: Shuangyin Wang
  • About author:
    ** e-mail:
  • Supported by:
    the National Natural Science Foundation of China(51402100); the National Natural Science Foundation of China(21573066); the National Natural Science Foundation of China(U19A2017); the National Natural Science Foundation of China(21825201); Provincial Natural Science Foundation of Hunan(2016JJ1006); Provincial Natural Science Foundation of Hunan(2016TP1009)

催化技术在现代工业生产和日常生活中发挥着举足轻重的作用,开发高效的催化剂是催化领域重要的研究方向。近些年来,许多研究发现催化剂的缺陷对其催化活性有着重要的影响,同时各种各样的缺陷催化剂也被开发出来。尽管如此,缺陷与催化活性之间的关系仍有待厘清。本文围绕这一主题,分别介绍了固体缺陷化学的基础、催化剂中缺陷的类型、表征、可控构筑以及在催化中的作用和动态变化,最后进行总结和展望。希望通过本文阐明催化剂缺陷化学研究的起源与发展,强调缺陷对催化的重要性,为今后高效催化剂的进一步开发与机理研究提供指导。

关键词： 缺陷, 催化, 活性位点, 吸附能, 凝聚态化学, 原位表征

Catalysis plays a significant role in modern industrial production and daily life and the exploration of efficient catalysts is an important issue of catalysis research. In recent decades, many researchers found the important effect of catalyst defects for their catalytic activity and various defective catalysts are prepared. Nevertheless, the relationship between defect and catalysis still needs clarification. In this review, we mainly introduce solid defect chemistry fundamental, defect types in catalysts, characterization and controllable construction of defects, the roles and the dynamic evolution of defects in catalysis. Finally, the summary and outlook for “defect with catalysis” are demonstrated. We hope this review can reveal the origin and development of catalyst defect chemistry, emphasize the importance of defect for catalysis and provide some guidance for exploration and mechanism researches of defect catalysts.

Contents

1 Introduction

2 Solid defect chemistry fundamental

2.1 Classification of solid defects

2.2 Symbols and chemical reaction of solid defect

3 Types, characterization and synthesis of defects in catalysts

3.1 Defect types in catalysts

3.2 Characterization of catalyst defects

3.3 Controllable synthesis of catalyst defects

4 Relationship between defects and activity of catalysts

5 Conclusion and outlook

Key words: defect, catalysis, activity sites, adsorption energy, condensed state chemistry, in-situ characterization
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表1 晶体缺陷的Kröger-Vink符号标记法[20]
Table 1 Kröger-Vink symbolic notation of crystal defects[20]
Defect types Symbols Defect types Symbols
Metal ions M vacancy VM Non-metal vacancy on the position of non-metal Y VY
Doped metal A on metal M AM Doped non-metal vacancy Z on the position of non-metal Y ZY
Interstitial metal M Mi Interstitial non-metal Y Yi
Electroneutral metal ions M vacancy Electroneutral non-metal ions Y vacancy
Metal ions M vacancy with effective negative charge V'M Non-metal ions Y vacancy with effective positive charge
Metal ions M vacancy with effective positive charge Non-metal ions X vacancy with effective negative charge X'i
Interstitial metal M with n effective positive charge Interstitial non-metal Y with n effective positive charge
Free electron b e' Free hole b h·
Associated defect(vacancies pair) (VMVY) Associated defect with effective positive charge (VMVY) ·
图1 (a) 不同缺陷程度的TiO2/b-Si的EPR谱图[40];(b) 体相CoSe2 和CoSe2超薄纳米片的正电子寿命谱图[42];(c) Mono-NTi-MMO及对照样品的XANES Ni K-edge 的R空间谱图[30]; (d) CoFe LDHs的XANES Fe K-edge 的R空间谱图[43]
Fig.1 (a) EPR spectra of TiO2/b-Si samples with different defects[40]; (b) Positron lifetime spectrum of the two CoSe2 samples[42]; (c) R space data of the Ni K-edge XANES spectra for the Mono-NTi-MMO and control samples[30]; (d) R space data of the Fe K-edge XANES spectra for CoFe LDHs[43]
图2 (a) 含有缺陷的CeO2的STM图像[46];(b) CO吸附在TiO2(111)上的STM图像[47];(c) 缺陷石墨烯的STEM图[49]; (d) 含有硫空位的WS2的STEM图像[51]
Fig.2 (a) STM image of CeO2 with defects[46]; (b) STM image of TiO2(111) with CO adsorption[47]; (c) STEM image of defective graphene[49]; (d) STEM image of WS2 with sulfur vacancies[51]
图3 (a) O空位在CO氧化过程中的作用的示意图[86];(b) 表面电荷与电催化活性的火山型关系图[96]
Fig.3 (a) Schematic diagram of the role of oxygen vacancy in catalyzing CO oxidation[86]; (b) Volcano relationships of surface charge and catalytic activities[96]
图4 (a) Au-SA/Def-TiO2及对比样的催化CO氧化的性能;(b) Au-SA/Def-TiO2 的活性中心结构示意图及其催化反应的稳定性[107]
Fig.4 (a) Catalytic performance of Au-SA/Def-TiO2 and control for CO oxidation; (b) Schematic diagram of active site structure and the catalytic stability of Au-SA/Def-TiO2[107]
图5 Pd nanoparticles/black TiO2/b-Si水还原光电阴极的示意图,梯度缺陷提升了b-TiO2的电子空穴对分离效率[40]
Fig.5 Schematic of Pd nanoparticles/black TiO2/b-Si photocathode for water reduction, graded oxygen defects of b-TiO2 improve the separation efficiency of electron-hole pair[40]
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摘要

缺陷与催化