燃料化学学报（中英文）2024，Vol.52Issue(9)：1290-1298,9.DOI:10.1016/S1872-5813(24)60457-3
苯和环己烯分步制联环己烷过程催化剂设计及性能提升研究
The study of design and performance improvement of catalysts for the stepwise production of bicyclohexane from benzene and cyclohexene
摘要
Abstract
Bicyclohexane is a hydrogen storage reagent with high hydrogen density and low boiling point.Compared with the hydrogenation of biphenyl,the alkylation of benzene and cyclohexene to cyclohexylbenzene and hydrogenation is a promising way to prepare cyclohexane on a large scale.The research and development of high-efficiency cyclohexyl benzene hydrogenation catalyst should be further developed based on mature alkylation technology.This paper used an acidified USY molecular sieve to catalyze the alkylation of benzene and cyclohexene to cyclohexylbenzene,which achieved 100％conversion and selectivity.Furthermore,Pt/TiO2/γ-Al2O3 catalyst is prepared by pre-deposition TiO2 film of different thicknesses on γ-Al2O3 surface and then supported with platinum particles by Atomic layer deposition(ALD).The role of TiO2 film in improving the cyclohexylbenzene hydrogenation performance of the catalyst is studied.TEM,CO pulse chemisorption,CO-DRIFTs,quasi-in situ XPS,H-D exchange,and H2-TPR characterization show that compared with Pt/γ-Al2O3,TiO2 thin films on Pt/TiO2/γ-Al2O3 do not change the dispersion of Pt particles,but can form new Pt-TiO2 interactions.The hydrogenation performance of cyclohexylbenzene was improved by increasing the electron density and the proportion of planar active sites on the surface of platinum and reducing the energy barrier of hydrogen spillover.The research provides theoretical support for further bicyclohexane organic liquid hydrogen storage reagent development.The relevant metal-support interaction regulation strategy can be applied to the development of efficient catalysts for other aromatic molecules hydrogenation.关键词
有机液态储氢/联环己烷/加氢/金属载体相互作用/原子层沉积Key words
organic liquid hydrogen storage/bicyclohexane/hydrogenation/metal-support interaction/atomic layer deposition分类
化学化工引用本文复制引用
刘瑞林,王森,孟繁春,李卓,杨慧敏,赵世超,覃勇,张斌..苯和环己烯分步制联环己烷过程催化剂设计及性能提升研究[J].燃料化学学报（中英文）,2024,52(9):1290-1298,9.基金项目
The project was supported by National Natural Science Foundation of China(22072172,22202227),National Science Fund for Distinguished Young Scholars(21825204),the Youth Innovation Promotion Association CAS(Y2021056),Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2022007),the Special Fund for Science and Technology Innovation Teams of Shanxi Province(202304051001007).国家自然科学基金(22072172,22202227),国家杰出青年科学基金(21825204),中国科学院青年创新促进会(Y2021056),榆林学院与大连清洁能源国家实验室合作基金(YLU-DNL Fund 2022007)和山西省科技创新团队专项资金(202304051001007)资助 （22072172,22202227）
