水滑石衍生的复合氧化物催化氧化挥发性有机气体的研究进展

doi:10.1016/S1872-2067(19)63446-7

催化学报 ›› 2020, Vol. 41 ›› Issue (4): 550-560.DOI: 10.1016/S1872-2067(19)63446-7

• 中国科学院青年创新促进会专栏 • 上一篇下一篇

水滑石衍生的复合氧化物催化氧化挥发性有机气体的研究进展

李双德^a, 王东东^a,b, 武晓峰^a, 陈运法^a,c

a 中国科学院过程工程研究所多相复杂系统国家重点实验室, 北京 100190;
b 中国科学院大学, 北京 100049;
c 中国科学院区域大气环境研究卓越创新中心, 福建厦门 361021

收稿日期:2019-09-29 修回日期:2019-11-01 出版日期:2020-04-18 发布日期:2019-12-12
通讯作者: 陈运法
基金资助:
国家重点研发计划（2017YFC0211503，2016YFC0207100）；中国科学院战略性先导科技专项A （XDA23030300）；国家自然科学基金（21401200，51672273）；多相复杂系统国家重点实验室开放课题（MPCS-2017-D-06）；中国科学院区域大气环境研究卓越创新中心青年人才项目（CERAE201805）.

Recent advance on VOCs oxidation over layered double hydroxides derived mixed metal oxides

Shuangde Li^a, Dongdong Wang^a,b, Xiaofeng Wu^a, Yunfa Chen^a,c

a State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
b University of Chinese Academy of Sciences, Beijing 100049, China;
c Center for Excellence in Regional Atmospheric Environment, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, Fujian, China

Received:2019-09-29 Revised:2019-11-01 Online:2020-04-18 Published:2019-12-12
Supported by:
This work was supported by the National Key R&D Program of China (2017YFC0211503, 2016YFC0207100), the Strategic Priority Research Program (A) of the Chinese Academy of Sciences (XDA23030300), the National Natural Science Foundation of China (21401200, 51672273), the Open Research Fund of State Key Laboratory of Multi-phase Complex Systems (MPCS-2017-D-06), and the Young Talent Project of the Center for Excellence in Regional Atmospheric Environment, CAS (CERAE201805).

摘要/Abstract

摘要： 挥发性有机化合物（VOCs）是大气颗粒污染物（PM_2.5）和臭氧污染的主要前体物，来源于工业活动（如溶剂使用过程）、汽车尾气以及植物排放等，具有毒性，对人类和自然生命产生危害.催化氧化技术是在催化剂表面，在较低的操作温度（200-450℃）下，将VOCs非均相催化氧化成CO₂和H₂O，是一种最为有效的分解VOCs的方法，具有副产物少，能耗低的优点.VOCs分解用催化剂主要分为贵金属和金属氧化物两大类.贵金属催化剂活性高，但价格昂贵.因此科研工作者一直在诸多方面调控过渡金属氧化物，例如制备方法、组分协同、结构缺陷等，期望获得高活性、低成本的催化剂.
水滑石（LDHs）是一种层状双金属氢氧化物，由带正电荷的金属氢氧化物层板和层间阴离子组成，可以表示为[M_1-x²⁺M_x³⁺（OH）₂]（A^n-）_x/n·mH₂O.鉴于LDHs特有的结构特点，层板元素可调、比例可调等，其在一定温度下煅烧可以得到过渡金属复合氧化物（MMO）材料.由于LDHs的拓扑焙烧转变得到的MMO材料显示出许多利于多相催化反应的优点，如大表面积和多孔性、高热稳定性、良好的金属氧化物分散性等.水滑石基催化材料用于VOCs催化分解也引起了科研工作者的持续关注和研究，文献大多选择苯、甲苯、乙酸乙酯等工业活动中常用的挥发性有机溶剂作为探针分子来评估催化剂的活性、稳定性等参数.本综述将LDHs衍生的VOCs降解催化剂分为4类，整理了其近10年的研究进展：（1）含过渡金属的LDHs焙烧转变成MMO催化剂：系统论述了层板元素组成、层板元素比例、焙烧温度、制备方法等条件对催化活性的影响规律，阐明了不同处理条件下催化剂的物理化学特性（比表面积、孔结构、表面元素价态、氧缺陷、还原性）与催化活性的关联；（2）贵金属/MMO催化剂：比较了贵金属种类、LDHs载体种类、负载方式等因素对催化活性的影响规律，总结了贵金属负载在LDHs载体的优势；（3）核壳型MMO催化剂：分析了在氧化铝球、MOF等载体上原位负载LDHs的方法构筑多级结构的MMO催化剂，利于促进VOCs分解活性；（4）整体型MMO催化剂：满足VOCs分解实际应用，提出铝片基底上原位生长-煅烧制备高活性位点暴露的整体式催化剂的优点.在催化活性基础上着重介绍了水蒸气对活性的影响以及VOCs分解催化机理.同时提出了3点仍需努力的方向：LDHs向MMO拓扑转变机制认识不足；LDHs衍生的催化剂的VOCs分解机制研究不深入；催化剂活性降低-再生研究不透彻.

关键词: VOCs氧化, 水滑石, 复合金属氧化物, 水汽, 氧化机理

Abstract: Catalytic oxidation is regarded as one of the most promising strategies for volatile organic compounds (VOCs) purification. Mixed metal oxides (MMOs), after topological transformation using layered double hydroxides (LDHs) as precursors, are extensively used as catalysts for VOCs oxidation due to their uniformity advantage. This review summarizes the developments in the LDH-derived VOCs heterogeneous catalytic oxidation over the last 10 years. Particularly, it addresses the VOCs abatement performance over MMO, noble metal/MMO, core-shell structured MMO, and integral MMO film catalysts originating from LDHs. Moreover, it highlights the water vapor effect and oxidation mechanism. This review indicates that LDH-based catalysts are a category of important VOCs oxidation materials.

Key words: Volatile organic compounds oxidation, Layered double hydroxides, Mixed metal oxides, Water vapor, Oxidation mechanism

中图分类号:

李双德, 王东东, 武晓峰, 陈运法. 水滑石衍生的复合氧化物催化氧化挥发性有机气体的研究进展[J]. 催化学报, 2020, 41(4): 550-560.

Shuangde Li, Dongdong Wang, Xiaofeng Wu, Yunfa Chen. Recent advance on VOCs oxidation over layered double hydroxides derived mixed metal oxides[J]. Chinese Journal of Catalysis, 2020, 41(4): 550-560.

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水滑石衍生的复合氧化物催化氧化挥发性有机气体的研究进展

Recent advance on VOCs oxidation over layered double hydroxides derived mixed metal oxides

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