铈锰基金属有机骨架材料（MOFs）催化氧化乙苯和乙酸乙酯的氧空位演变

Industrial volatile organic compounds(VOCs) are causing more serious complex air pollution in modern China, therefore, taking effective treatment of VOCs is of great ugency as a highly focused issue by our country. At present the most widely used function materials, adsorbents and catalysts are faced with the issue on the enhancement of activities and stabilities. Therefore, the development of adsorbents with high adsorption capacity and catalysts with higher catalytic activity under low temperature and stronger anti-deactivation ability, as well as the comprehensively research of the catalytic reaction mechanism, are of important scientific significance and application value. Herein, this project is proposed on the combination of the tunability of metal organic frameworks(MOFs), and the excellent capacity of oxygen storgae and release of ceria. And assisted with computer stimulation, Mn modified ceria based MOFs are synthesized via a controllable route.The competitive adsorption and catalytic oxidation of ethyl benzene and ethyl acetate on these MOFs are investigated, as well as the carbon deposition is studied. With the techniques of in situ IR, in situ Raman, and GC-MS, the evolution of oxygen vacancies is correlated with the transformation of the related reactants, intermediates in this complex system.The pathways of the competitive reaction of ethyl benzene and ethyl acetate on Mn modified ceria based MOFs will be presented. This work will supply basic data for the research and development of novel catalysts towards mixed VOCs elimination, and provide experience for the promotion of excellent performance and carbon deposition tolerance for catalysts, as it will has reference value for the broadening of the application of the catalysis technology for VOCs abatement.

我国当前工业挥发性有机物（VOCs）引起的大气复合污染日益严重，其治理已刻不容缓，国家高度重视。目前广泛使用的吸附剂和催化剂存在材料活性及其稳定性需要强化的问题。因此研制吸附容量高的吸附剂和低温下活性高、抗失活能力强的催化剂，较为全面地研究催化反应历程具有重要科学意义和应用前景。本项目基于金属有机骨架材料（MOFs）的可调控性与CeO2优异的储氧释氧能力，拟辅以计算机模拟，可控合成锰修饰的CeO2-MOFs；研究乙苯和乙酸乙酯的竞争性吸附和催化氧化，考察催化剂上的积碳行为；利用原位拉曼和原位红外、GC-MS等，关联反应过程中氧空位的演变和相关反应物、中间产物的转化；阐明乙苯和乙酸乙酯在MOFs上的竞争性反应历程。研究成果可为研制多组分VOCs净化的新型催化剂提供基础数据，为提升催化剂的低温催化活性和抗积碳能力等实用性能形成经验借鉴，对研究拓宽净化VOCs废气的催化技术的应用范围具有考价值。

我国当前工业挥发性有机物（VOCs）引起的大气复合污染日益严重，其治理已刻不容缓，国家高度重视。目前广泛使用的吸附剂和催化剂存在材料活性及其稳定性需要强化的问题。因此研制吸附容量高的吸附剂和低温下活性高、抗失活能力强的催化剂，较为全面地研究催化反应历程具有重要科学意义和应用前景。本项目基于金属有机骨架材料（MOFs）的可调控性与CeO2优异的储氧释氧能力，拟辅以计算机模拟，可控合成锰修饰的CeO2-MOFs；研究乙苯和乙酸乙酯的竞争性吸附和催化氧化，考察催化剂上的积碳行为；利用原位拉曼和原位红外、GC-MS等，关联反应过程中氧空位的演变和相关反应物、中间产物的转化；阐明乙苯和乙酸乙酯在MOFs上的竞争性反应历程。研究成果可为研制多组分VOCs净化的新型催化剂提供基础数据，为提升催化剂的低温催化活性和抗积碳能力等实用性能形成经验借鉴，对研究拓宽净化VOCs废气的.催化技术的应用范围具有考价值。