甲醛催化氧化催化剂的研究进展

doi:10.1016/S1872-2067(15)61007-5

催化学报 ›› 2016, Vol. 37 ›› Issue (1): 102-122.DOI: 10.1016/S1872-2067(15)61007-5

甲醛催化氧化催化剂的研究进展

拜冰阳^a,b, 乔琦^a,b, 李俊华^c, 郝吉明^c

a 中国环境科学研究院环境基准与风险评估国家重点实验室, 北京100012;
b 中国环境科学研究院国家环境保护生态工业重点实验室, 北京100012;
c 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:2015-08-27 修回日期:2015-10-20 出版日期:2015-12-26 发布日期:2015-12-26
通讯作者: 李俊华, 拜冰阳
作者简介:李俊华, 拜冰阳
基金资助:
国家自然科学基金(21325731, 51478241, 21221004).

Progress in research on catalysts for catalytic oxidation of formaldehyde

Bingyang Bai^a,b, Qi Qiao^a,b, Junhua Li^c, Jiming Hao^c

a State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing 100012, China;
b Key Laboratory of Eco-Industry of the Ministry of Environmental Protection, Chinese Research Academy of Environmental Sciences, Beijing 100012, China;
c State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

Received:2015-08-27 Revised:2015-10-20 Online:2015-12-26 Published:2015-12-26
Supported by:
This work was supported by the National Natural Science Foundation of China (21325731, 51478241, 21221004).

摘要/Abstract

摘要：

甲醛是致癌致畸物并具有较强的光化学活性.它既来源于纺织、农药、板材或其他精细化学品的生产过程,又来源于机动车尾气和室内各种装潢材料.为了人体健康和大气环境去除甲醛非常必要.用催化氧化法去除甲醛是一种很有前景的技术,但是该技术的关键是研究和发展催化剂.近年来,用于甲醛氧化的催化剂主要分为贵金属催化剂和过渡金属氧化物催化剂.
贵金属催化剂是将Pt,Pd,Au,Ag等贵金属负载在不同类型的载体上而制得.载体可分为常见载体、传统金属氧化物载体和特殊形貌金属氧化物载体.常见载体是具有较大比表面积的SiO₂,Al₂O₃,TiO₂和分子筛等.这类载体有利于活性位的暴露以及反应物和产物的吸附和扩散,而且还能增强载体和活性组分的协同作用.负载在常见载体上的不同贵金属催化剂,其甲醛氧化活性从强到弱排列是: Pt> Pd> Rh> Au> Ag.用这种载体制备的催化剂具有很出色的应用前景.比如Na-Pt/TiO₂是甲醛氧化活性最好的催化剂,目前已被应用在空气净化器中,其次是Pt/TiO₂和Pd/TiO₂.传统金属氧化物载体主要是采用沉淀法、共沉淀法制备的CeO₂,Fe₂O₃,Co₃O₄,MnO₂及其复合氧化物,这类载体负载Pt的催化剂仍然具有出色的室温催化性能,如Pt/MnO_x-CeO₂和Pt/Fe₂O₃等.虽然Pt负载型催化剂应用前景很好,但是其成本较高,工业生产和普及受到限制.用传统金属氧化物载体制备的催化剂如Au/CeO₂,Ag/MnO_x-CeO₂和Ag/CeO₂等同样具有良好的发展前景.对于提高甲醛氧化活性来说,载体的选择至关重要.未来研究趋势可能是甲醛氧化负载型催化剂更多的会选择Ag或Au作为活性组分,而一些有潜力的传统金属氧化物载体将被使用不同的制备方法进一步改良.目前,拥有棒状、球状、孔状等特殊形貌的金属氧化物载体因为它们本身的催化活性要优于用沉淀法制备的传统金属氧化物催化剂,因此,将Ag或Au负载在这类载体上制备的催化剂具有更好的应用前景,如三维(3D)有序大孔Au/CeO₂-Co₃O₄,二维有序介孔Au/Co₃O₄-CeO₂和Au/Co₃O₄以及三维有序介孔K-Ag/Co₃O₄等.
过渡金属氧化物催化剂,因成本低,资源丰富而受到关注.单一过渡金属氧化物催化剂如锰钾矿型的MnO₂纳米棒或纳米球,介孔MnO₂,Co₃O₄和Cr₂O₃等,具有较好的甲醛氧化催化活性(T₅₀和T₁₀₀分别小于等于110和140℃).另外,Ce,Sn,Cu和Zr等元素常常被掺杂到MnO_x和Co₃O₄中,制备成复合金属氧化物催化剂,MnO_x-CeO₂具有较好的甲醛催化活性(T₅₀ < 100℃),因为MnO_x和CeO₂较强的相互作用改变了表面活性氧和活性相的数量.目前,复合金属氧化物催化剂氧化甲醛的报道很少.随着制备方法的改变,单一过渡金属氧化物或他们的复合氧化物催化剂可能会成为贵金属催化剂的替代品.
目前,如何获得高效、低成本、低温甚至常温去除甲醛的催化剂仍然是一项重要的挑战.特殊形貌的金属氧化物催化剂如3D-Cr₂O₃,3D-Co₃O₄,MnO₂纳米球和纳米棒,在常温下完全转化甲醛仍然是个难以越过的鸿沟.
将来,多种形貌的新型纳米金属氧化物及其Au或Ag负载型催化剂的制备和发展会成为一个研究趋势.这种催化剂既能被用于甲醛的催化氧化,也能被用于苯系物或其他VOCs的催化氧化.它能为机动车尾气和工业生产中VOCs产生量的削减提供技术支撑,而VOCs的去除有益于PM2.5浓度的降低和空气质量的恢复.

关键词: 甲醛, 催化氧化, 金属氧化物催化剂, 贵金属催化剂, 低温催化活性

Abstract:

Formaldehyde (HCHO) is carcinogenic and teratogenic, and is therefore a serious danger to human health. It also adversely affects air quality. Catalytic oxidation is an efficient technique for removing HCHO. The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures, even room temperature, is important. Supported Pt and Pd catalysts can completely convert HCHO at room temperature, but their industrial applications are limited because they are expensive. The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO₂, Co₃O₄, or other metal oxides. This is attributed to their specific structures, high specific surface areas, and other factors such as active phase, reducibility, and amount of surface active oxygens. Such catalysts with various morphologies have great potential and can also be used as catalyst supports. The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature. The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal. In this paper, research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties, structure-activity relationships, and factors influencing the catalytic activity and reaction mechanism are discussed. Future prospects and directions for the development of such catalysts are also covered.

Key words: Formaldehyde, Catalytic oxidation, Metal oxide catalyst, Noble metal catalyst, Low-temperature catalytic activity

拜冰阳, 乔琦, 李俊华, 郝吉明. 甲醛催化氧化催化剂的研究进展[J]. 催化学报, 2016, 37(1): 102-122.

Bingyang Bai, Qi Qiao, Junhua Li, Jiming Hao. Progress in research on catalysts for catalytic oxidation of formaldehyde[J]. Chinese Journal of Catalysis, 2016, 37(1): 102-122.

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甲醛催化氧化催化剂的研究进展

Progress in research on catalysts for catalytic oxidation of formaldehyde

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