低耗可控微波诱导复合吸波材料催化氧化甲苯废气的协同作用机制研究

As one of the main air pollutants causing haze, the treatment method of VOCs with high efficiency and low consumption is urgently needed, because of characteristics of VOCs, such as extensive emission and wide varieties. Though the availability of the technology involving purification using catalysts induced by microwave radiation has been confirmed by domestic and overseas related researchers, the basic theory of reaction is not clear yet, which leads to the fact that the catalytic reaction induced by microwave radiation is difficult to achieve with features of low consumption, controllability and high efficiency. The applicant has found in preliminary studies that the effect of "Hot Spots" presented by catalysts with absorbing property plays an important role for significant improvement of purification efficiency. And the study involving physicochemical and catalytic characteristics of typical catalytic materials with absorbing property under microwave radiation and the analysis involving essential laws of the synergic relationship between the induction under microwave radiation and catalytic reaction are the key basis for building the catalysis technology induced by microwave radiation with low consumption and controllability. .Therefore, toluene as the typical representative of VOCs was chosen to be the research object in this study. On the one hand, effects of characteristics of microwave radiation on the catalytic activity and laws of interrelation involving factors, such as temperature, space velocity, and so on，will be investigated systematically. Moreover, effects of differences of absorbing properties of materials on catalytic reaction under microwave radiation will also be explored and relations of interaction between properties of absorbing materials and catalytic activities will also be analyzed systematically. The essential law of microwave-induced synergistic catalysis reaction will be explored by studying the above two aspects, which provides a theoretical basis for building the catalysis technique induced by microwave radiation with low consumption and controllability and provides a new feasible way for purification of VOCs with low consumption and high efficiency in the future.

VOCs为主要致霾大气污染物之一，因排放面广、种类多等特点，寻求高效低耗的处理方法日益迫切。尽管国内外研究已表明微波诱导催化净化效果良好，但反应基础理论尚不明确，难以实现低耗可控高效微波诱导催化反应。申请人前期研究发现具有吸波性能的催化材料表现出的“Hot Spots”效应对显著提升净化效率有重要作用，研究典型吸波材料在特定微波场中的理化和催化特性，分析微波诱导协同催化反应的本质规律，是构建低耗可控微波诱导催化技术的关键。.为此，本研究拟以甲苯为研究对象，筛选复合吸波材料，一方面系统考察微波特性对催化活性的影响，以及二者与温度、空速等影响因素的关联规律；另一方面，探索材料吸波性能差异对微波场中催化反应的影响，系统分析不同复合吸波材料性能与催化活性的作用关系。由以上两方面，探究微波诱导协同催化反应的本质机制，为构建低耗可控微波诱导催化技术提供理论基础，为VOCs低耗高效净化提供一条新的思路。

作为PM2.5和近地面臭氧的主要前驱体之一，挥发性有机物排放面广且种类繁多，对其高效净化任重而道远。本项目以开发高效低耗的微波诱导处理VOCs技术为主旨，研究典型吸波材料在特定微波场中的理化和催化特性，分析微波诱导协同催化反应的本质规律，在此基础上设计开发了多种性能优异的吸波复合材料。具体的，研制了Nano-Co3O4、双元Ce-Co材料、锰基复合材料（MnO2(Ac)、MnO2/RGO）、镍钴复合材料、ZIF-67衍生钴基催化剂等多种材料，用于微波场下诱导甲苯高效净化，并对各材料的制备条件以及相关参数展开了细致研究，确定了最佳制备条件。结合各种表征手段分析明确了材料的理化性质与吸波性能对材料净化甲苯活性的影响，获取了各材料在微波场中不同条件下催化活性的变化规律。对比分析了微波场与传统热场中，材料性能的不同之处，研究了不同反应条件（系统温度﹑初始浓度﹑吸附剂填充量以及气体流量，等）不同场下材料对甲苯去除的影响，并进行了相关的动力学和热力学研究，揭示了微波诱导协同催化反应的本质机制。相关研究成果发表文章22篇，其中SCI收录17篇，EI收录3篇，核心2篇。授权发明专利2项。通过本项目的研究，不仅开发出了具有优异吸波性能和VOCs净化功能的高效材料，同时分析明确了微波场中材料净化VOCs（甲苯）的相关机理以及材料的构效关系，为实现低耗高效微波诱导催化的相关研究提供了重要的理论基础。