基于氢溢流效应Ni/钼钨复合金属氧化物催化剂的可控构筑及α-蒎烯选择性加氢性能研究

氢溢流是一种能有效提高催化剂加氢性能的效应。然而，催化剂与氢溢流间的构效关系研究甚少。合理设计催化剂各组分协同作用促进氢溢流，对于系统而全面地认识其构效关系，开发高效加氢催化剂尤为重要。本项目针对江西省香精香料产业中关键中间体合成反应α-蒎烯选择性加氢制备顺式蒎烷的催化剂加氢效率低的问题，通过构筑比单一金属氧化物性质优异的钼钨复合金属氧化物载体，增强氢溢流驱动力，延长活性氢传输距离，采用表面修饰手段引入氧化功能基团和缺陷，增加氢溢流载流子和活性位点，利用小分子有机“碳桥”紧密连接载体和表面Ni金属活性组分，降低氢溢流的界面传输能垒，制备出各组分有效协同作用增强氢溢流效应的Ni/钼钨复合金属氧化物催化剂。设计不同组分的参比催化剂，结合氢同位素红外吸附实验和氢气程序升温脱附等表征技术，揭示催化剂各组分协同作用与氢溢流效应和加氢性能间的构-效关系，为开发高效α-蒎烯选择性加氢催化剂提供科学依据。

Hydrogen spillover is a kind of effect that can effectively improve the hydrogenation performance of the catalyst. However, there are few studies on the structure-performance relationship between catalyst and hydrogen spillover. The rational design of the synergism of all catalyst components to promote hydrogen spillover is particularly important for the systematic and comprehensive understanding of the structure-performance relationship and the development of highly efficient hydrogenation catalysts. This project aims at the problem of low hydrogenation efficiency of the catalyst for the selective hydrogenation of α-pinene to cis-pinene that is the synthesis reaction of key intermediates in the flavor and fragrance industry in Jiangxi province. The molybdenum-tungsten composite metal oxide support with superior properties to single metal oxide will be constructed to enhance the driving force of hydrogen spillover and extend the transport distance of active hydrogen. Surface modification methods will be used to introduce oxidation functional groups and defects to increase hydrogen spillover carriers and active sites. The small molecular organic "carbon bridge" will be used to tightly connect the support and the surface Ni metal active components to reduce the interface transport energy barrier of hydrogen spillover. It will synthesize Ni/molybdenum-tungsten composite metal oxide catalysts with effective synergistic effect of each component to enhance hydrogen spillover effect. The structure-performance relationship between the synergism of all components of the catalyst, the hydrogen spillover effect and the hydrogenation performance will be revealed by the design of reference catalysts with different components combined with the hydrogen isotope infrared absorption experiments and the characterization techniques such as temperature-programmed desorption of hydrogen. This project will provide the scientific basis for developing the highly efficient catalysts of the selective hydrogenation of α-pinene.