催化燃烧甲苯反应中催化剂硫中毒过程及机理研究进展  

Research progress on catalyst sulfur poisoning process and mechanism in catalytic combustion of toluene reaction

作　　者：金泽韬 宁韩棋 蒋百顺 左树锋 JIN Zetao;NING Hanqi;JIANG Baishun;ZUO Shufeng(College of Chemistry&Chemical Engineering,Shaoxing University,Shaoxing 312000,China)

机构地区：[1]绍兴文理学院化学化工学院,浙江绍兴312000

出　　处：《能源环境保护》2024年第4期136-143,共8页Energy Environmental Protection

基　　金：国家自然科学基金资助项目(21577094);浙江省科技厅公益性项目(LGG19B070003)。

摘　　要：挥发性有机物(Volatile Organic Compounds,VOCs)排放量大,来源广泛且种类繁多。催化燃烧法作为最高效的治理技术之一,其技术核心“催化剂”备受关注。然而,当VOCs中含有微量或痕量的硫物种时,会使催化剂硫中毒,导致其活性和寿命大幅度降低。因此,如何提高催化剂的耐硫性,研究催化降解VOCs过程中的硫中毒过程及机理,对于开发性能优异的催化剂至关重要。用于VOCs催化降解的催化剂主要以γ-Al_(2)O_(3)、Beta分子筛和柱撑黏土为载体,以过渡金属氧化物及贵金属为反应活性中心。通过原位硫酸铵热分解法引入定量的硫物种,得到了一系列不同硫中毒程度的催化剂。利用甲苯催化燃烧作为探针反应,研究了硫中毒前后催化剂的孔结构、氧化性、酸性等变化。结合活性组分的永久性硫中毒,明确了催化剂结构与催化燃烧VOCs性能之间的构效关系,深入理解了硫中毒过程及机理。总结近年来本课题组在该领域的研究成果,为构筑高性能催化燃烧含硫VOCs催化剂的研发提供启发,为实现复杂反应体系的工业化应用提供理论和技术基础。Volatile organic compounds(VOCs)are characterized by large emissions,a wide range of sources,and various types.Catalytic combustion,as one of the most efficient treatment technologies,has attracted much attention for its core technology,"the catalyst".However,even a trace amount of sulfur species containing VOCs can poison catalysts,resulting in a significant loss of its catalytic activity and lifetime.Therefore,it is crucial to improve the sulfur tolerance of the catalyst and study the sulfur poisoning process and deactivation mechanism during the catalytic degradation of VOCs.Understanding the sulfur poisoning process is key to develop catalysts with excellent catalytic performance for VOCs degradation.In this paper,the catalysts used for the catalytic degradation of VOCs mainly involveγ-Al_(2)O_(3),Beta zeolite,and pillared clay as carriers,along with transition metal oxides and precious metals as reaction active centers.Quantitative sulfur species are introduced into various fresh catalysts through in-situ(NH_(4))_(2) SO_(4) thermal decomposition,resulting in a series of catalysts with varying degrees of sulfur poisoning.The changes in the structure,redox,acidity,and other properties of the catalyst before and after sulfur poisoning are studied using the catalytic oxidation of toluene as a probe reaction.By combining this with the sulfur poisoning of the active sites,the structure-activity relationship between the catalyst structure and the catalytic performance for VOCs degradation is clarified,providing a deep understanding of the sulfur poisoning mechanism of the catalyst.By summarizing our recent research achievements in this paper,we hope to promote the development of high-performance catalysts for sulfur-containing VOCs catalytic combustion and provide a theoretical and technical basis for achieving the industrial application of catalysts under complex reaction systems.

关 键 词：催化燃烧 甲苯 硫中毒 负载型催化剂 硫中毒机理 

分 类 号：X701[环境科学与工程—环境工程]