类整体式纳米管阵列催化剂表界面功能层的构筑及其催化净化VOCs性能研究

VOCs are important air pollutants, and catalytic combustion is an efficient route for VOCs removal due to its high removal efficiency and absence of secondary pollution. A comprehensive consideration of macroscopic catalyst bed construction, mesoscopic catalyst pore structure design and microscopic surface and interface structure regulation is a key for the application of catalytic removal of VOCs over a low noble-metal content catalyst under mild conditions. Our previous studies have shown that monolith-like nanotube array (NT) supported catalysts with long range disorder and short range order offered potential applications in VOCs catalytic combustion. The aim of this work is to improve the performance of the monolith-like NT catalyst by design and in situ preparation of a stable functional layer over the NT surface. Special attention is given to the interaction among noble metal/functional inter layer/NT and their synergistic catalytic mechanism, and the regulation of the VOCs combustion process. A breakthrough is expected on the microscopic VOCs oxidation mechanism and the catalyst structure-activity relationship after the multi work on the catalyst design, in situ characterization and the theoretical calculation. Finally, the understanding of the catalyst structure at the molecular level and the reaction mechanism induced catalyst design is expected.

VOCs是一类重要的空气污染物，催化燃烧技术由于其效率高、无二次污染等特点而被广泛应用。通过宏观催化剂床层设计、介观催化剂孔结构的构筑和微观表界面结构的调控等多尺度协同作用调控是实现在低贵金属含量和温和条件下VOCs催化氧化脱除的关键。申请人在前期工作中发现长程无序、短程有序的纳米管阵列负载型类整体式催化剂在VOCs催化燃烧反应中表现出良好的操作性能。本项目拟通过类整体式二氧化钛和氧化铝纳米管阵列催化剂的表界面功能层的可控稳固构筑与结构调控, 发展高效低贵金属含量VOCs催化燃烧类整体式催化剂的设计和制备方法。以贵金属活性组分/非贵金属表界面功能层/纳米管阵列载体之间协同催化机制、VOCs催化氧化反应的微观机制和催化剂构效关系为基础科学问题，将催化剂材料的理性设计、原位表征技术和模拟计算相结合，实现分子水平上的结构认知和机理导向的催化剂设计。

项目以开发高效低贵金属含量VOCs催化燃烧催化剂为研究目标，通过构建Al2O3和TiO2纳米管阵列等载体的表界面功能层，发展高效VOCs催化燃烧催化剂的设计和制备方法，认知贵金属活性组分/表界面功能中间层/Al2O3或者TiO2纳米管阵列等载体之间的相互作用和协同催化机制。项目自立项以来，项目组全体人员按照项目进度表积极认真地开展各项工作，已完成各项预定目标：(1) 通过在Al2O3或TiO2纳米管阵列等载体上构筑具有协同贵金属活性位点催化作用的功能性活性组分与载体或者助剂的界面层，利用与贵金属活性颗粒紧密结合的界面功能层对活性颗粒的限域锚定作用和活性基团（活性氧或羟基）的储存传递作用，显著提升了负载型贵金属催化剂催化净化有机废气的稳定性和活性；(2) 利用原位红外表征、催化反应测试和量子化学理论计算等技术手段，认知了甲醛和甲苯等VOCs分子催化氧化反应机理和催化剂的构效关系；(3) 通过催化剂表界面微观结构的系统表征和理论计算，揭示了贵金属活性组分/非贵金属表界面功能层/Al2O3或TiO2纳米管阵列等载体之间的相互作用和协同催化机制。在本领域重要的学术期刊上发表论文26篇、申请发明专利6件、授权发明专利4件和实用新型专利1件。项目研究结果为今后高效VOCs燃烧催化剂的设计和推广应用提供了基础数据和参考。