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

doi:10.1016/j.cjche.2021.09.015

中国化学工程学报 ›› 2022, Vol. 41 ›› Issue (1): 392-402.DOI: 10.1016/j.cjche.2021.09.015

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

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

Zhentao Chen, Yaxin Liu, Jian Chen, Yang Zhao, Tao Jiang, Fangyu Zhao, Jiahuan Yu, Haoxuan Yang, Fan Yang, Chunming Xu

State Key Laboratory of Heavy Oil Proceeing, China University of Petroleum, Changping, Beijing 102249, China

收稿日期:2021-06-30 修回日期:2021-08-16 出版日期:2022-01-28 发布日期:2022-02-25
通讯作者: Zhentao Chen,E-mail address:czt@cup.edu.cn;Chunming Xu,E-mail address:xcm@cup.edu.cn
基金资助:
The authors acknowledge the supports by National Natural Science Foundation of China (NSFC) (Nos. 21878329 and 21476257), the National Key Research and Development Program Nanotechnology Specific Project (No. 2020YFA0210900) and Science Foundation of China University of Petroleum, Beijing (No. 2462018QZDX04).

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

Zhentao Chen, Yaxin Liu, Jian Chen, Yang Zhao, Tao Jiang, Fangyu Zhao, Jiahuan Yu, Haoxuan Yang, Fan Yang, Chunming Xu

State Key Laboratory of Heavy Oil Proceeing, China University of Petroleum, Changping, Beijing 102249, China

Received:2021-06-30 Revised:2021-08-16 Online:2022-01-28 Published:2022-02-25
Contact: Zhentao Chen,E-mail address:czt@cup.edu.cn;Chunming Xu,E-mail address:xcm@cup.edu.cn
Supported by:
The authors acknowledge the supports by National Natural Science Foundation of China (NSFC) (Nos. 21878329 and 21476257), the National Key Research and Development Program Nanotechnology Specific Project (No. 2020YFA0210900) and Science Foundation of China University of Petroleum, Beijing (No. 2462018QZDX04).

摘要/Abstract

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)

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)

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]. 中国化学工程学报, 2022, 41(1): 392-402.

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

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

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