Synthesis of alumina-nitrogen-doped carbon support for CoMo catalysts in hydrodesulfurization process

doi:10.1016/j.cjche.2021.09.015

Abstract

Abstract: More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts. In this paper, a series of CoMo/NDC@alumina catalysts were synthesized by combination of the chemical vapor deposition of nitrogen-doped carbon (NDC) using 1,10-phenanthroline and co-impregnation of Mo and Co active components. The optimal catalyst with additive of 25% 1,10-phenanthroline was screened by a series of property characterization and the hydrodesulfrization (HDS) active test. The amount of “CoMoS” active phase of the optimal CoMo/C3 catalyst increased 5.3% as compared with the CoMo/γ-Al₂O₃. The introduction of NDC improved the sulfidation degree of Mo by 21.8% as compared to the CoMo/γ-Al₂O₃ catalyst, which was beneficial to form more active sites. The HDS conversion of the NDC supported catalysts are higher than CoMo/γ-Al₂O₃ whether for the dibenzothiophene (DBT) or 4,6-dimethyl dibenzothiophene (4,6-DMDBT). Further hydroprocessing evaluation with Dagang diesel revealed that the CoMo/C3 catalyst possessed higher HDS property and the removal rate of DBTs in the diesel increased by 4%–11% as compared to the CoMo/γ-Al₂O₃ catalyst.

Key words: Nitrogen-doped carbon materials, Catalyst, hydrodesulfurization (HDS), Diesel, Dibenzothiophene (DBT)

摘要： More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts. In this paper, a series of CoMo/NDC@alumina catalysts were synthesized by combination of the chemical vapor deposition of nitrogen-doped carbon (NDC) using 1,10-phenanthroline and co-impregnation of Mo and Co active components. The optimal catalyst with additive of 25% 1,10-phenanthroline was screened by a series of property characterization and the hydrodesulfrization (HDS) active test. The amount of “CoMoS” active phase of the optimal CoMo/C3 catalyst increased 5.3% as compared with the CoMo/γ-Al₂O₃. The introduction of NDC improved the sulfidation degree of Mo by 21.8% as compared to the CoMo/γ-Al₂O₃ catalyst, which was beneficial to form more active sites. The HDS conversion of the NDC supported catalysts are higher than CoMo/γ-Al₂O₃ whether for the dibenzothiophene (DBT) or 4,6-dimethyl dibenzothiophene (4,6-DMDBT). Further hydroprocessing evaluation with Dagang diesel revealed that the CoMo/C3 catalyst possessed higher HDS property and the removal rate of DBTs in the diesel increased by 4%–11% as compared to the CoMo/γ-Al₂O₃ catalyst.

关键词: Nitrogen-doped carbon materials, Catalyst, hydrodesulfurization (HDS), Diesel, Dibenzothiophene (DBT)

Zhentao Chen, Yaxin Liu, Jian Chen, Yang Zhao, Tao Jiang, Fangyu Zhao, Jiahuan Yu, Haoxuan Yang, Fan Yang, Chunming Xu. Synthesis of alumina-nitrogen-doped carbon support for CoMo catalysts in hydrodesulfurization process[J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 392-402.

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