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孔结构和酸度对负载型NiMo催化剂上二苯并噻吩加氢脱硫反应的影响

The Influence of Pore Structure and Acidity on the Hydrodesulfurization of Dibenzothiophene over NiMo-Supported Catalysts.

作者信息

Shi Yu, Wang Gang, Mei Jinlin, Xiao Chengkun, Hu Di, Wang Aocheng, Song Yidong, Ni Yan, Jiang Guiyuan, Duan Aijun

机构信息

State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing, 18 Fuxue Road, Beijing 102249, P.R. China.

出版信息

ACS Omega. 2020 Jun 17;5(25):15576-15585. doi: 10.1021/acsomega.0c01783. eCollection 2020 Jun 30.

Abstract

A series of mesoporous materials of SBA-16 were in situ incorporated into ZSM-5 crystallites via a two-step self-assemble method, and hydrodesulfurization (HDS) catalysts were prepared on the corresponding ZSM-5/SBA-16 (ZS) composites. The characterization results indicated that ZSM-5 nanoseeds were fabricated into the silica framework of the ZS composites, and the three-dimensional 3 cubic structure of SBA-16 was retained simultaneously. In addition, the ZS series materials possessed open pores and large surfaces, which would facilitate the diffusion of reactants in the mesoporous channels. Moreover, the introduction of ZSM-5 seeds into composites could enhance the acidities of supports. As a result, the NiMo/ZS series catalysts exhibited high activities for DBT HDS processes. The NiMo/ZS-160 catalyst exhibited the highest catalytic efficiency (96.5%), which was apparently attributed to the synergistic contributions of the physicochemical properties of ZS supports and the dispersion states of active metals. Correspondingly, DBT HDS reactions over the NiMo/ZS series catalysts mainly proceeded via a hydrogenation desulfurization route that benefitted from the enhanced acidities especially the total Brønsted acid.

摘要

通过两步自组装法将一系列SBA-16介孔材料原位引入ZSM-5微晶中,并在相应的ZSM-5/SBA-16(ZS)复合材料上制备了加氢脱硫(HDS)催化剂。表征结果表明,ZSM-5纳米晶被制备到ZS复合材料的二氧化硅骨架中,同时SBA-16的三维立方结构得以保留。此外,ZS系列材料具有开放的孔道和较大的比表面积,这将有利于反应物在介孔通道中的扩散。而且,向复合材料中引入ZSM-5晶种可以增强载体的酸度。结果,NiMo/ZS系列催化剂在DBT加氢脱硫过程中表现出高活性。NiMo/ZS-160催化剂表现出最高的催化效率(96.5%),这显然归因于ZS载体的物理化学性质和活性金属的分散状态的协同作用。相应地,NiMo/ZS系列催化剂上的DBT加氢脱硫反应主要通过加氢脱硫途径进行,这得益于酸度的增强,尤其是总布朗斯特酸。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9efb/7331072/1a1daee6c72a/ao0c01783_0001.jpg

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