吸附-催化双功能材料用于低温去除苯系物研究

The combination of adsorption and catalysis is one of the most promising technologies for removal of benzene, toluene, and o-xylene (BTX). Porous materials have excellent adsorption and catalytic activities for removal VOCs, which have the highest potential for application in removal of BTX at low temperature. This project will prepare excellent adsorption and catalysis materials based on metal-organic framework and zeolite with high thermal stability and adsorption ability to improve removal efficiency of BTX at low temperature. The effects of kinds of MOF and zeolite, pore structure, metal and organic species of MOF, ratio of Si/Al, surface area, and preparation method on removal efficiency of BTX will be investigated based on the current achievements made by both domestic and foreign researches and our initial experimental results. Effects of water on the catalytic activities and lifetime will be investigated, followed by hydrophobic modification. Relations between the structure of materials and catalytic activities will be proposed. In addition, formation of intermediates and products and kinetic theory calculation will be studied to investigate the way of BTX purification and mechanism.

吸附-催化协同技术是去除苯系物的主流技术之一。多孔材料具有优异的吸附、催化性能，是低温去除苯系物的首选。本项目拟对筛选出的热稳定性好、吸附性能优异的金属-有机骨架材料（MOF）和分子筛多孔材料进行活性中心结构和酸碱位的构建，制备出高性能的吸附-催化双功能材料，降低催化反应温度，提高BTX的去除效率。获取MOF和分子筛种类、孔结构、MOF材料中金属离子配位构型与配体种类、分子筛中Si/Al 比、活性金属负载方式、酸碱位等对MOF和分子筛在吸附-催化协同技术去除苯系物中的吸附、脱附、活性影响的认知。研究双功能材料的抗水性能，并进行疏水改性。建立双功能材料微观结构与苯系物去除活性的构效关系，结合反应产物以及动力学研究和理论模拟计算，揭示吸附、活化和催化反应去除苯系物的机制，以此指导高性能催化剂的设计。

挥发性有机物（VOCs）广泛来源于工业生产、室内装修装饰材料等，是造成区域性灰霾和臭氧大气复合污染的重要前体物之一，对生态环境和人体健康具有极大危害。目前，吸附浓缩-高温燃烧技术已在全球范围内得到应用，效果理想，但是高温环境的营造提高了成本。本研究以高效吸附、催化去除VOCs材料的研发为研究目标，以实验表征与量化模拟计算相结合的手段，研究了不同拓扑结构和硅铝比分子筛合成方法与吸附去除苯系物性能以及水共存的影响，揭示了不同分子筛的吸附位点以及吸附机理。研究了金属氧化物以及金属有机骨架材料（MOFs）衍生的金属氧化物制备方法与催化氧化苯系物活性，阐明了氧空位、氧缺陷的关键作用和反应机理。实现了分子筛、MOFs、金属氧化物材料筛选与制备参数的优化，为吸附、催化去除VOCs材料的研发鉴定了理论基础。. 基于以上成果，发表SCI论文6篇，申请发明专利1项。