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Deep hydroconversion of ethanol-soluble portion from the ethanolysis of Hecaogou subbituminous coal to ultra-clean liquid fuel over hierarchical porous zeolite Y supported Ni–Co nanoparticles
Journal of the Energy Institute ( IF 5.7 ) Pub Date : 2021-08-23 , DOI: 10.1016/j.joei.2021.08.006
Yu-Hong Kang 1, 2, 3 , Xiao-Qi Zhang 1 , Juan Gao 1, 2 , Xian-Yong Wei 1, 2, 3 , Cheng-Hu Xue 1 , Yan-Jun Li 1, 2 , Yong Gao 1, 2 , Guang-Hui Liu 1, 2 , Jin-Jun Bai 1, 2 , Xiang-Rong Ma 1, 2 , Hong-Cun Bai 3 , Zhi-Min Zong 2
Affiliation  

A hierarchical porous zeolite Y (HPZY) supported Ni–Co catalyst was prepared by pyrolyzing nickel tetracarbonyl and using modified deposition-precipitation to highly disperse Ni–Co nanoparticles onto HPZY. Hecaogou subbituminous coal was effectively ethanolyzed to obtain ethanol-soluble portion (ESPE) in a high yield (21.2%). Sequentially, ESPE was subjected to the deep hydroconversion (DHC) over prepared Ni10%-Co3%/HPZY at 150 °C under 4 MPa of initial hydrogen pressure for 24 h in n-heptane to produce deeply hydroconverted ethanol-soluble portion (ESPDHC). All the group components in ESPE, including arenes (53.3%), oxygen-containing organic compounds (24.4%), and nitrogen-containing aromatics (2.3%) were completely converted to chain alkanes (CAs, 36.8%), cyclanes (39.2%), and hydroarenes (24.0%). In addition, the hydroisomerization of CAs and hydroreforming of aromatic rings (ARs) in ESPDHC are predominant over Ni10%-Co3%/HPZY with more accessibility of active sites under mild conditions. Ni10%-Co3%/HPZY with suitable acidity and highly dispersed Ni–Co nanoparticles can effectively activate H2 to H⋯H and further heterogeneously split H⋯H to H+ and H. H⋯H and H+ transfer plays crucial roles in the DHC of ESPE. Correspondingly, the related mechanisms are evidenced by the DHC of 2,2′-oxydinaphthalene (ODN) over Ni–Co/HPZY. Ni10%-Co3%/HPZY maintains high activity for the DHC of ODN under mild conditions after 4 recycles.



中文翻译:

河草沟亚烟煤乙醇分解中乙醇可溶部分在分层多孔沸石 Y 负载的 Ni-Co 纳米颗粒上深度加氢转化为超清洁液体燃料

通过热解四羰基镍并使用改进的沉积-沉淀法将 Ni-Co 纳米颗粒高度分散到 HPZY 上,制备了分级多孔沸石 Y (HPZY) 负载的 Ni-Co 催化剂。对河草沟次烟煤进行有效乙醇化,以高收率(21.2%)获得乙醇可溶部分(ESP E)。随后,ESP E在 150 °C 和 4 MPa 的初始氢气压力下在庚烷中对制备的 Ni 10% -Co 3% /HPZY 进行深度加氢转化 (DHC) 24 小时,以产生深度加氢转化的乙醇可溶部分(ESP DHC )。ESP E 中的所有组组件,包括芳烃(53.3%)、含氧有机化合物(24.4%)和含氮芳烃(2.3%)完全转化为链烷烃(CAs,36.8%)、环烷烃(39.2%)和氢芳烃(24.0%) %)。此外,ESP DHC中CA 的加氢异构化和芳环 (AR) 的加氢重整优于 Ni 10% -Co 3% /HPZY,在温和条件下更容易接近活性位点。Ni 10% -Co 3% /HPZY 具有合适的酸度和高度分散的 Ni-Co 纳米粒子可以有效地将 H 2活化为 H⋯H,并进一步将 H⋯H 异质分裂为 H +和 H -。H⋯H 和 H +转移在 ESP E的 DHC 中起着至关重要的作用。相应地,2,2'-氧化二萘(ODN)在Ni-Co/HPZY上的DHC证明了相关机制。Ni 10% -Co 3% /HPZY 在温和条件下在 4 次循环后保持对 ODN 的 DHC 的高活性。

更新日期:2021-08-30
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