新型CH4-CO2重整高抗积碳钴基/炭材料催化剂的可控制备及其催化机理研究

CO2 recycling and emission reduction have become a global problem of chemistry and catalysis disciplines in the 21st century. Catalytic CO2 reforming is one of the effective ways to solve the energy and environmental issues. The key issue was how to improve the activity and anti- coking property of the reforming catalyst. Novel cobalt-base/carbonaceous catalysts for CH4-CO2 reforming were not only has high catalytic activity, but also have a good stability. This has important scientific significance and research value to the development and practical application of carbon dioxide reforming technology in the field of energy and the environment. This project will investigate structure-activity relationship of surfactants structure, interfacial microstructure and size effect of reforming catalyst with CO2 reforming conversion by preparing a kind of novel cobalt-based/carbonaceous catalysts. The affection of reaction conditions on the conversion of CO2 and CH4 and kinetics were investigated. Cobalt-base/carbonaceous catalytic CO2 reforming reaction pathways and reaction and anti- coking mechanism were discussed. The controlled preparation and reaction mechanism of novel cobalt-base/carbonaceous catalysts for CH4-CO2 reforming will be developed in the final. Through the research, the process of CH4/CO2 reforming was deepened the understanding over cobalt-base/carbonaceous catalyst, and greatly enriched the development of the science of carbon. Provide the theoretical basis of design and development to the oriented anti-coke cobalt-base/carbonaceous catalyst.

CO2资源化利用和减排已成为21世纪化学和催化学科的世界性难题，催化CO2重整转化是解决该难题的有效途径之一。而提高催化剂活性和抗积碳性是其中两个关键问题。本申请在前期研究基础上，拟借助炭材料表面性能可控的特点，在对CO2、CH4活化和抗积碳组分筛选基础上，将炭材料与钴及助剂进行融合，筛选出性能优异的钴基-炭材料催化剂。利用炭材料与金属协同性，达到对CH4和CO2活化、转化的目的；考察催化剂表面、界面微观结构和材料的尺寸效应与CO2重整转化之间的构效关系，获得催化剂不同功能单元相互耦合机制及其功能调控规律；利用原位等手段对CH4、CO2在催化剂上活化方式和途径进行清晰表达，探究钴基-炭材料催化重整转化反应途径以及抗积碳机理；优化反应体系，建立反应条件对CO2转化率的影响及动力学规律。本研究不仅可成功引领新一代重整催化剂的研制，而且对重整技术发展及其应用具有重要科学意义和研究价值

中央经济工作会议明确将“做好碳达峰、碳中和工作”确定为我国2021年八大重点任务之一。催化CO2重整转化是实现“碳中和”的有效途径之一。而提高催化剂活性和抗积碳性是重整转化的两个关键问题。针对项目申请书中的研究目标，本项目借助炭材料表面性能可控的特点，对CO2、CH4活化和抗积碳组分进行筛选，将炭材料与钴及助剂进行融合；利用炭材料与金属协同作用，实现了对CH4和CO2的活化和转化，获得了高抗积碳钴基/炭材料催化剂的可控制备方法；并运用多种现代技术对所制备的催化剂进行了结构表征，考察了催化剂表面、界面微观结构和材料的尺寸效应与CO2重整转化之间的构效关系，获得了催化剂不同功能单元相互耦合机制及其功能调控规律；根据催化活性中心的动态变化理论，结合原位等手段对CH4、CO2在催化剂上活化方式和途径进行分析，明晰了钴基/炭材料催化重整转化反应途径以及抗积碳机理；通过对反应系统进行优化，获得了CH4-CO2重整动力学规律。上述关于高效重整催化剂的制备和改性等关键问题的探讨和研究，不仅加深了对炭催化CH4-CO2重整的认识，而且对重整技术发展及其应用具有重要科学意义和研究价值。依托基金及研究结果，发表相关研究成果学术论文30篇，其中SCI/EI期刊27篇、中文核心期刊3篇；申请及授权相关专利17项；培养博士/硕士研究生10名，其中4人次获得国家奖学金，参加国际学术会议8次，在国内外相关会议上做学术报告5次，培养高级人才1名，获得“三晋英才”和“山西省优秀科技工作称号”各1名。同时在项目执行期间，积极开展国际合作与交流，引进山西省百人1名。