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化学进展 2024, Vol. 36 Issue (1): 27-47 DOI: 10.7536/PC230604 前一篇   后一篇

• 综述 •

VOCs氧化催化剂设计与结构调控

杨雯皓1, 赵东越1, 宋海涛1,*(), 李俊华2,*()   

  1. 1 中石化石油化工科学研究院有限公司 北京100083
    2 清华大学环境学院 环境模拟与污染控制国家重点联合实验室 北京100084
  • 收稿日期:2023-06-08 修回日期:2023-08-30 出版日期:2024-01-24 发布日期:2024-01-05
  • 作者简介:

    宋海涛 中石化石油化工科学研究院研究员，催化裂化催化剂研究室主任。从事石油炼制及工业烟气污染物治理催化剂研发与应用，近5年主持国家重点研发计划课题1项，中国石化科技项目及课题6项，发表论文20余篇，授权中国发明专利30件，国际专利5件。获中央企业熠星创新创意大赛一等奖，中国环境保护产业协会技术进步一等奖等9项成果奖励（5项排名第一）。

    李俊华 清华大学教授，长江学者特聘教授，国家杰出青年基金获得者，大气污染物与温室气体协同控制国家工程研究中心主任。长期从事工业烟气脱硫脱硝、VOCs减排与CO2捕集利用催化剂研发与应用，发表SCI论文246篇，连续入选“全球高被引科学家”，授权国家发明专利36项。成果获国家科技进步一等奖1项和国家技术发明二等奖1项，省部级特/一等奖3项(均为排名第一)。

  • 基金资助:
    国家自然科学基金项目(22306210); 国家重点研发计划(2022YFB3504004); 中石化石油化工科学研究院院控课题(PR20230115)
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Design and Structure Regulation of VOCs Catalytic Oxidation Catalysts

Wenhao Yang1, Dongyue Zhao1, Haitao Song1(), Junhua Li2()   

  1. 1 SINOPEC Research Institute of Petroleum Processing Co., Ltd., Beijing 100083, China
    2 State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
  • Received:2023-06-08 Revised:2023-08-30 Online:2024-01-24 Published:2024-01-05
  • Contact: * e-mail: songht.ripp@sinopec.com (Haitao Song); lijunhua@tsinghua.edu.cn (Junhua Li)
  • Supported by:
    National Natural Science Foundation Program of China(22306210); National Key Research & Development Program of China(2022YFB3504004); SINOPEC RIPP Project(PR20230115)

近年来我国环境空气质量显著改善，NOx与SO2等传统污染物得到有效控制，挥发性有机物（Volatile Organic Compounds, VOCs）排放控制逐渐成为进一步解决区域复合型大气污染问题的关键因素。催化氧化法因其处理效率高、能耗低及适用范围广等优势，已成为最具应用前景的VOCs减排技术之一。高性能催化剂的研发是该技术的核心，结合反应机理进行催化剂设计和结构调控是目前研究的热点和重点。本文首先对VOCs催化氧化机理进行概述；其次从单一过渡金属氧化物、混合金属氧化物、复合金属氧化物以及相界面结构调控角度综述了非贵金属催化剂结构调控的相关研究进展；聚焦贵金属分散状态，总结了贵金属催化剂中贵金属纳米颗粒/团簇催化剂尺寸效应与载体效应相关研究成果，并对目前新兴的单原子催化剂基于金属-载体相互作用的调控手段进行概括；最后对VOCs氧化催化剂的研究现状与趋势进行总结与展望。我们认为深入解析构效关系，研发简约和精细化的催化剂结构调控手段并适配实际工况和工业放大是未来研究的重点发展方向。

关键词： 挥发性有机物, 催化氧化, 结构调控, 贵金属分散状态调控, 反应机理

In recent years, with the improvement of the air quality in China, traditional pollutants such as NOx and SO2 have been effectively controlled. The emission control of volatile organic compounds (VOCs) has gradually become a key to further alleviating the regional composite air pollution so far. Catalytic oxidation is one of the most promising VOCs emission reduction technologies due to its high treatment efficiency, low energy consumption, and wide applicability. The development of high-performance catalysts is crucial for this technology. The design and structural regulation of catalysts associated with mechanism study is currently a research hotspot. This paper first outlines the catalytic oxidation mechanism of VOCs. Secondly, the research progress on the structural regulation of non-noble metal catalysts is reviewed from the perspectives of single transition metal oxides, mixed metal oxides, composite metal oxides, and interface structure regulation. Based on the dispersion state, the size effect and support effect of noble metal nanoparticles/clusters in noble metal catalysts are summarized. The regulation strategies based on the metal-support interaction for the emerging single-atom catalysts are also discussed. Finally, this paper provides a summary and prospects for future research trends. We believe that based on deeply clarifying the structure-activity relationship, developing simple and refined structure regulation methods of catalysts and adapting to actual operating conditions and industrial scale-up is the focus of future research.

Contents

1 Introduction

2 VOCs catalytic oxidation mechanisms

3 Structure regulation of non-noble metal catalysts

3.1 Single transition metal oxides

3.2 Mixed transition metal oxides

3.3 Composite transition metal oxides

3.4 Interface structure regulation

4 Regulation of metal dispersion state in noble metal catalysts

4.1 Noble metal nanoparticle/cluster catalysts

4.2 Noble metal single-atom catalysts

5 Conclusion and outlook

Key words: volatile organic compounds(VOCs), catalytic oxidation, structure regulation, noble metal dispersion state regulation, reaction mechanism
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图1 （a）催化剂降低VOCs氧化反应活化能示意图；（b）VOCs催化氧化机理
Fig. 1 (a) Schematic diagram of catalyst reducing the activation energy of VOCs oxidation reaction; (b) VOCs catalytic oxidation mechanisms
图2 丙烷与丙烯在YMn2O5表面的活化和氧化过程[21]
Fig. 2 Activation and oxidation of propane and propene on YMn2O5[21], Copyright 2020, American Chemical Society
图3 （a）不同晶型MnO2的合成方法与晶体结构[29]；（b）不同形貌Co3O4与其主要暴露晶面的关系
Fig. 3 (a) Synthesis methods and crystal structures of MnO2 with different crystal phases[29], Copyright 2021, John Wiley and Sons; (b) Relationship between Co3O4 with different morphologies and main exposed crystal facets
图4 （a）δ-MnO2不同层间离子掺杂对甲醛及其氧化中间物种吸附能的影响[43]，（b）MOF-71衍生Co-Ce混合氧化物及其丙酮氧化活性[73]
Fig. 4 (a) The effect of different interlayer ions in δ-MnO2 on the adsorption energy of formaldehyde and oxidation intermediate species[43], Copyright 2020, American Chemical Society; (b) MOF-71-derived Co-Ce mixed oxides and their acetone oxidation activity[73], Copyright 2020, American Chemical Society
图5 尖晶石晶体结构示意图
Fig. 5 Schematic diagram of spinel crystal structure
图6 钙钛矿晶体结构示意图
Fig. 6 Schematic diagram of perovskite crystal structure
图7 Mn基莫来石晶体结构示意图
Fig. 7 Schematic diagram of Mn-based mullite crystal structure
图8 Mn2O3@δ-MnO2核壳异质结构催化剂构建应用于甲苯氧化[115]
Fig. 8 Construction of Mn2O3@δ-MnO2 core-shell heterostructure catalysts for toluene oxidation[115], Copyright 2020, Elsevier
图9 Pt NPs粒径与CeO2表面氧空位和活性氧物种含量的关系
Fig. 9 The relationship between the particle size of Pt NPs and the surface oxygen vacancies/active oxygen species content of CeO2
图10 （a）Pd负载于不同形貌CeO2表面时其CO与丙烷氧化反应速率[152]，（b）MOF原位生长诱导Co3O4与Pt NPs间电子转移促进甲苯氧化机理示意图[153]
Fig. 10 (a) The reaction rate of CO and propane oxidation over Pd loaded on CeO2 with different morphologies[152], Copyright 2016, American Chemical Society; (b) Schematic diagram of electron transfer between Co3O4 and Pt NPs induced by MOF in situ growth promoting toluene oxidation[153], Copyright 2022, American Chemical Society
图11 单原子催化剂的制备方法[162]
Fig. 11 Synthesis strategies of single-atom catalysts[162], Copyright 2021, American Chemical Society
图12 （a）H2O2辅助MnO2表面Mn空位捕获Ag单原子促进氧活化[179]；（b）Co3+位点稳定Ag单原子促进苯氧化[180]
Fig. 12 (a) H2O2-assisted Mn vacancy capture of Ag single atom on MnO2 surface promoting oxygen activation[179], Copyright 2022, Royal Society of Chemistry; (b) Co3+-site stabilized Ag single atom promoting benzene oxidation activity[180], Copyright 2022, American Chemical Society
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摘要

VOCs氧化催化剂设计与结构调控