高效消除挥发性有机物的沸石分子筛基材料的设计合成和性能研究

As one kind of the major components in air pollutants, volatile organic compounds (VOCs) are strongly harmful to human health and environmental protection. Moreover, most of VOCs are precursors of ozone and photochemical smog, which are great threats to the environment and human health because of their toxic, carcinogenic, mutagenic, and teratogenetic nature. Thus, elimination of VOCs has become one of hot research topics, due to the safe concerns together with more stringent legislations..Up to now, a series of techniques for removal of VOCs have been well developed, among which catalytic combustion as destructive technology and adsorption as nondestructive technology have been identified as the most effective, economically feasible, and promising routes for VOCs abatement. Catalysts and adsorbents are the key factors in both technologies. Compared with conventional catalysts (transition metal oxides) and adsorbents (activated carbon), zeolites have become one of the most important materials for removal of VOCs due to its unique features and performances such as uniform and controllable micropores as well as designable wettability. .Although the preparation of zeolites have made great progress in recent years, design and synthesis of zeolite-based materials aimed for removal of VOCs are still scarcely. Thus, the target in this project is to design and prepare zeolites involved in the removal VOCs, and we would intensively study the mechanism together with the cooperation between the porous structure and the active sites, and develop sustainable methodology to design and synthesis of zeolites with new structure as well as excellent performance for the removal of VOCs in industrial application.

挥发性有机物 (VOCs)是空气污染物的主要成分，不仅可以直接对人体健康和环境造成伤害，大部分的VOCs还会进一步导致臭氧和光化学烟雾等二次污染的产生，对人体和环境造成更大的威胁和危害。VOCs 废气处理方法可分为以催化氧化为代表的破坏性技术和以吸附法为代表的非破坏性技术两大类。这两类处理方法的核心都是材料：催化材料和吸附材料。相比传统的非贵金属氧化物催化剂和活性炭吸附剂，沸石分子筛由于其独特的结构和性能逐渐成为VOCs处理的研究热点。尽管沸石分子筛近年来在制备方面取得了巨大的突破，但是针对VOCs处理的沸石分子筛的设计合成还有待于进一步发展。本项目将围绕VOCs吸附以及催化氧化反应所涉及的沸石分子筛材料，深入研究其孔道结构与原子水平吸附和催化中心的协同作用，设计新结构和性能优异的沸石分子筛材料，发展绿色高效和低成本的方法实现沸石分子筛材料在VOCs处理工业上大规模应用。

挥发性有机物 (VOCs)是空气污染物的主要成分，不仅可以直接对人体健康和环境造成伤害，大部分的VOCs还会进一步导致臭氧和光化学烟雾等二次污染的产生，对人体和环境造成更大的威胁和危害。VOCs 废气处理方法可分为以催化氧化为代表的破坏性技术和以吸附法为代表的非破坏性技术两大类。这两类处理方法的核心都是材料：催化材料和吸附材料。相比传统的非贵金属氧化物催化剂和活性炭吸附剂，沸石分子筛由于其独特的结构和性能逐渐成为VOCs处理的研究热点。尽管沸石分子筛近年来在制备方面取得了巨大的突破，但是针对VOCs处理的沸石分子筛的设计合成还有待于进一步发展。按照项目计划书的要求，本项目将围绕VOCs吸附以及催化氧化反应所涉及的沸石分子筛材料，深入研究其孔道结构与原子水平吸附和催化中心的协同作用，设计新结构和性能优异的沸石分子筛材料，发展绿色高效和低成本的方法取得了系列突破性进展，主要包括：(1) 研究无有机模板剂合成的Beta分子筛负载Pt在甲醛室温消除反应中活性，揭示了K＋离子对贵金属活性中心的促进作用，并在此基础上深入研究了该分子筛负载MnOx在甲苯催化氧化反应中活性；(2) 使用绿色路线合成的全硅Beta分子筛，并研究其负载Pt后在甲醛催化氧化反应中活性，并通过动力学研究揭示了表明浸润性对反应活性的促进，并在此基础上深入研究了该分子筛负载Ag在甲醛催化氧化反应中活性，并设计了使用MnOx来提高负载Ag的分子筛催化剂活性的路线；(3)系统研究了ZSM-5在一系列VOCs消除反应中的活性，揭示催化剂的构效关系；(4) 设计绿色路线合成全硅Beta沸石并应用在VOCs吸附研究。本项目的实施实现了沸石分子筛材料在VOCs处理工业上大规模应用。