基于氧缺陷型非贵金属氧化物的加氢催化剂及其作用机理研究

Heterogeneous hydrogenation is one of the most important reactions in petrochemical industry. The development of highly active and cheap catalyst can greatly reduce the production cost. Inexpensive metal oxides are recently regarded as a new type of hydrogenation catalyst, but the inherent active site and related mechanism are not studied. Previously, the applicant found that oxygen-defected metal oxides are very active in hydrogenation reaction. In this project, using tungsten oxide as the model, a comprehensive study will be conducted to explore oxygen-defected oxides as hydrogenation catalyst, and solve the key scientific problem, i.e., the mechanism of oxygen defect-mediated hydrogen activation and subsequent hydrogenation. First, systematic reaction evaluation will be conducted to demonstrate the potential of oxygen-defected oxide as hydrogenation catalyst. Then the structure-activity relationship between oxygen defect and hydrogenation activity will be established by tuning the type and concentration of defect. Finally, the critical role of oxygen defect in hydrogenation reaction will be illustrated using DFT computation. This project is expected to develop a promising hydrogenation catalyst for industrial application and provide the basis for rational design and fabrication of metal oxide based hydrogenation catalysts.

催化加氢是石油化工等行业的重要单元反应，研究高效低成本的新型加氢催化剂对降低生产成本具有重要意义。非贵金属氧化物代表了一类新的高效加氢催化剂，但其催化活性位本质及机理仍不清楚。申请人近期发现，含有氧缺陷的金属氧化物具有优异的加氢活性。本项目拟系统开展以氧缺陷型金属氧化物作为新型加氢催化剂的实验和计算研究。围绕氧缺陷对氢分子活化及加氢反应的作用机理这一关键科学问题，采用氧化钨为模型催化剂，通过系统的加氢反应评价来展示缺氧型金属氧化物作为加氢催化剂的可行性；通过可控调节氧缺陷位的种类及浓度，建立其与加氢催化活性的定量构效关系；通过量子化学模拟来验证氧缺陷对加氢共性及关键步骤的决定性作用。项目可望从机理层次理解金属氧化物的催化活性位本质，开发一种具有实际应用价值的加氢催化剂，并为其他金属氧化物加氢催化剂的理性设计和可控制备提供思路。

催化加氢是石油化工等行业的重要单元反应，发展高效低成本的新型加氢催化剂对降低生产成本具有重要意义。本项目采用实验和计算方法系统研究了氧缺陷型金属氧化物作为新型加氢催化剂的可行性及其机理：揭示了氧缺陷在氢分子活化及后续加氢反应中的关键性作用，建立了其与加氢催化活性的定量构效关系；发展了钨氧化物、铁氧化物、钴氧化物等氧缺陷型加氢催化剂，获得了低成本高活性的加氢催化剂；阐述了氧缺陷型催化剂表面的乙烯加氢和芳烃加氢等模型反应的过程机理；并将缺陷结构的理念拓展到碳基催化剂方面；上述催化剂应用于生物质转化和高能航天燃料的制备，降低了其工艺成本。项目结果从机理层次阐明了金属氧化物的催化活性位本质，开发了具有实际应用价值的加氢催化剂，并为其他加氢催化剂的理性设计和可控制备提供了新思路。

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