Hydrodesulfurization of dibenzothiophene and its hydrogenated intermediates over bulk CoP and Co2P catalysts with stoichiometric P/Co ratios

被引:32
作者
Zhou, Xuerong [1 ]
Li, Xiang [2 ]
Prins, Roel [3 ]
Lv, Jinyin [1 ]
Wang, Anjie [1 ,4 ]
Sheng, Qiang [2 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, 2 Linggong Rd, Dalian 116024, Peoples R China
[2] Tianjin Univ Sci & Technol, Coll Chem Engn & Mat Sci, Tianjin Key Lab Brine Chem Engn & Resource Ecouti, Tianjin 300457, Peoples R China
[3] Swiss Fed Inst Technol, Inst Chem & Bioengn, CH-8093 Zurich, Switzerland
[4] Dalian Univ Technol, Penn State & Dalian Univ Technol Joint Ctr Energ, Dalian 116024, Peoples R China
关键词
Hydrodesulfurization; Dibenzothiophene; Hydrogenated intermediates; CoP; Co2P; Piperidine;
D O I
10.1016/j.jcat.2020.08.030
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
CoP and Co2P were prepared by temperature-programmed reduction of the mixtures of Co(OH)(2) and H3PO3 with stoichiometric P/Co ratios, but their surfaces were still enriched in phosphorus. Based on the product distributions of the hydrodesulfurization (HDS) of dibenzothiophene (DBT), 1,2,3,4-tetrahy dro-dibenzothiophene (TH-DBT), and 1,2,3,4,4a,9b-hexahydro-dibenzothiophene (HH-DBT), a reaction network of DBT HDS was proposed and the mechanisms of the cleavage of different CAS bonds in DBT and its hydrogenated intermediates were discussed. CoP was much more active and more nitrogen tolerant than Co2P, which make it a promising HDS catalyst. The HDS reactions over CoP and Co2P followed a pseudo-first-order kinetics and a pseudo-zero-order kinetics, respectively. Piperidine strongly inhibited the hydrogenation/dehydrogenation reactions and the direct desulfurization of DBT, but its inhibition on the desulfurization of TH-DBT and HH-DBT were less pronounced. The active surfaces of CoP and Co2P in HDS reactions can be cobalt phosphosulfide phases. (c) 2020 Elsevier Inc. All rights reserved.
引用
收藏
页码:167 / 180
页数:14
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