Fajie Hu, Rushuo Li, Danfeng Zhao, Xiubing Huang, Ge Wang
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引用次数: 0
摘要
双环戊二烯(DCPD)加氢合成四氢双环戊二烯(THDCPD)是制备高能量密度燃料的关键工艺之一,而低温高活性镍催化剂的开发仍具有挑战性。本研究基于软模板法和液相原位还原法制备了分层多孔(HP)Ce-UiO-66负载镍纳米颗粒(NPs)催化剂。在 Ce-UiO-66 中引入介孔可有效增强对基质的转移和吸附,而 Ni NPs 则是主要的活性中心。此外,通过改变原位沉积条件,还有效地实现了对 Ni NPs 电子结构的调控和对 Ce-Ni 相互作用的促进。在 3 wt% Ni NPs 低负载条件下,制备的 3Ni/HP-UiO-66 催化剂可在 1 h 内实现观察到的 DCPD 完全转化和 THDCPD 100 % 的选择性,并保持了良好的循环稳定性。结果表明,3Ni/HP-UiO-66 催化剂优先吸附并氢化降冰片烯环,证实了 3Ni/HP-UiO-66 催化剂氢化 DCPD 的反应途径。本研究为探索和设计用于烯烃和芳烃氢化的非贵金属催化剂提供了指导。
Promoted synergistic interactions between Ce and Ni in hierarchical porous Ce-UiO-66 supported Ni NPs for dicyclopentadiene hydrogenation to tetrahydrodicyclopentadiene
The hydrogenation of dicyclopentadiene (DCPD) to synthesize tetrahydrodicyclopentadiene (THDCPD) is one of the key processes for the preparation of high-energy–density fuels, and the development of low-temperature and high-activity Ni catalysts is still challenging. In this work, hierarchical porous (HP) Ce-UiO-66 loaded Ni nanoparticles (NPs) catalysts were prepared based on the soft template method and liquid-phase in situ reduction method. The introduction of mesopores into Ce-UiO-66 can effectively enhance the transfer and adsorption of the substrate, and Ni NPs act as the main active centers. Furthermore, the modulation of the electronic structure of Ni NPs and the promotion of Ce-Ni interaction were effectively achieved by changing the in-situ deposition conditions. With a low loading of 3 wt% Ni NPs, the prepared 3Ni/HP-UiO-66 catalysts could achieve the observed complete DCPD conversion and 100 % selectivity of THDCPD within 1 h and retained good cycling stability. The results demonstrated preferential adsorption and hydrogenation of the norbornene ring, confirming the reaction pathway of the 3Ni/HP-UiO-66 catalyst for the hydrogenation of DCPD. The present work provides a guidance for exploring and designing non-noble metal catalysts for the hydrogenation of olefins and aromatics.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.