Citation: WU Meng-de, LI Guang-ci, LI Ming-shi, LI Xue-bing, ZHUANG Qing-fa, CHEN Song. Effect of nickel cobalt co-catalyst on catalytic activity of molybdenum naphthenate for the hydroprocessing of coal tar pitch in suspension bed[J]. Journal of Fuel Chemistry and Technology, ;2021, 49(1): 27-36. doi: 10.1016/S1872-5813(21)60002-6 shu

Effect of nickel cobalt co-catalyst on catalytic activity of molybdenum naphthenate for the hydroprocessing of coal tar pitch in suspension bed

1.
School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China
2.
Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China

Corresponding author: LI Ming-shi, mingshili@cczu.edu.cn
Received Date: 15 September 2020
Revised Date: 17 October 2020

Fund Project: The project was supported by National Natural Science Foundation of China (21761132006), Open Fund of State Key Laboratory of Heavy Oil (2018-02), Scientific Research and Innovation Fund of Qingdao Institute of Energy, and Clean Energy Innovation Institute of Chinese Academy of Sciences (QIBEBT l201933).

Figures(5)

Five dispersed molybdenum, nickel and cobalt oil soluble homogeneous catalysts were synthesized. The hydrogenation of coal tar pitch was under the conditions of 370 °C, 10 MPa hydrogen pressure, and 4 h reaction time in an autoclave reactor. The effects of molybdenum naphthenate addition, molybdenum nickel and molybdenum cobalt bimetallic ratios on hydrogenation were investigated. The catalytic hydrogenation effect was evaluated by the liquid yield. A variety of analytical methods, such as elemental analysis, ICP-MS, TEM, XPS, and four component separation, were used to explore the optimal catalytic system for the slurry bed hydrogenation of coal tar pitch. The results show that the optimal catalytic system is molybdenum naphthenate and nickel naphthenate ratio of 1∶1 at catalyst amount of 2×10³. Under optimal conditions, the liquid yield is 85.3%, the residue yield is 10.6%, and the gas yield is 4.1%.
- coal tar pitch,
- hydro-upgrading,
- homogeneous catalyst,
- slurry bed hydrocracking
1. [1]
  HE D M, GUAN J, WU D, ZHAO S C, ZHANG Q M. Modification of coal tar pitch to reduce the carcinogenic polycyclic aromatic hydrocarbons[J]. Appl Mech and Mater,2013,295−298:3098−3103. doi: 10.4028/www.scientific.net/AMM.295-298.3098
2. [2]
  XIAO Jin, WANG Ying, LIU Yong-dong, LAI Ting-qing, LI Jie. Progress in coal tar pitch modification[J]. Carbon Tech,2010,29(2):31−37. doi: 10.3969/j.issn.1001-3741.2010.02.008
3. [3]
  DANG A-lei, LI Tie-hu, ZHANG Wen-juan, ZHAO Ting-kai, FANG Chang-qing, WANG Zhen. Newest research in progress of coal tar pitch[J]. Carbon Techn,2011,30(6):19−23. doi: 10.3969/j.issn.1001-3741.2011.06.006
4. [4]
  CHANG Hong-hong, WEI Wen-long, WANG Zhi-zhong, YANG Huai-wang, YAO Run-sheng. Properties and application of coal tar pitch[J]. Shanxi Coking Coal Sci & Technol,2007,(2):39−42+46. doi: 10.3969/j.issn.1672-0652.2007.02.014
5. [5]
  WANG L, WANG J, JIA F, WANG C, CHEN M. Nanoporous carbon synthesized with coal tar pitch and its capacitive performance[J]. J Mater Chem A,2013,01(33):9498−9507. doi: 10.1039/c3ta10426e
6. [6]
  DIAZ C, BLANCO C G. NMR: A powerful tool in the characterization of coal tar pitch[J]. Energy Fuels,2003,17(4):907−913.
7. [7]
  SUN Z, LI D, MA H, TIAN P, LI X, LI W, ZHU Y. Characterization of asphaltene isolated from low-temperature coal tar[J]. Fuel Process Technol,2015,138:413−418. doi: 10.1016/j.fuproc.2015.05.008
8. [8]
  LIANG Wen-jie. Heavy Oil Chemistry[M]. Dongying: Petroleum University Press, 2000.
9. [9]
  LIM S H, GO K S, KWON E H, NHO N S, LEE J G. Investigation of asphaltene dispersion stability in slurry-phase hydrocracking reaction[J]. Fuel,2020,271:117509. doi: 10.1016/j.fuel.2020.117509
10. [10]
  ZHAO Lin-yun. Studies on coal/oil Co-Hydroprocessing with mild conditions and preliminary process design[D]. Qingdao: China University of Petroleum (East China), 2016.
11. [11]
  XUE Yong-bing, LIN Kai-cheng, ZOU Gang-ming. Functions and kinds of solvents in coal direct liquefaction[J]. Coal Convers,1999,22(4):1−4. doi: 10.3969/j.issn.1004-4248.1999.04.001
12. [12]
  WANG Xue-yun, ZHAO Yuan, YAN Bing-feng. Study on the slurry ability of different heavy oils using as coal-oil co-processing solvent[J]. Coal Qual Technol,2019,34(3):7−10+14. doi: 10.3969/j.issn.1007-7677.2019.03.002
13. [13]
  PEI Ting, CHEN Gang, LU Yong-bin, LI Bo. Development of Kerosene Co-Refining Technology and Catalyst Research[C]. Proceedings of the 11th Annual National Conference on Industrial Catalytic Technology and Applications, 2014: 30−33.
14. [14]
  HUANG Chuan-feng, LI Da-peng, YANG Tao. Status and research trends of co-processing of coal and oil[J]. Modern Chemical Industry,2016,36(8):8−13.
15. [15]
  GUO Qiang, GAO Xiong-cheng, AI Ke-li. Application of suspended bed hydrocracking technology in kerosene co-refining unit[J]. China Petrochem,2017,(4):45−46.
16. [16]
  SHI Mu-er, ZHONG Chang-wen. Preparation of homogeneous catalyst molybdenum naphthenate[J]. J of Daqing Pet Inst,1998,22(4):40−42+102.
17. [17]
  HU Zhi-meng. Synthesis and antiwear performance of molybdenum naphthenate[J]. China Molybdenum Ind,1999,23(6):33−34.
18. [18]
  GUO Yong-hui, YANG Zhan-kui. Applications and preparation of nickel naphthenate[J]. Value Eng,2010,29(24):247. doi: 10.3969/j.issn.1006-4311.2010.24.228
19. [19]
  HE Xiao-hui. Study on the synthesis of cobalt iso-octoate[J]. Petrochem Technol,1999,28(3):36−38.
20. [20]
  QIN Yi-hong, HE Han-bing, CHEN Yu-xian, HUANG Cao-ming. Study on the synthesis of cobalt iso-octoate[J]. Nonferrous Met (Smelting Part),2005,(6):39−41+45.
21. [21]
  WANG Yu-mei, YAN Ying. Preparation of cobalt naphthenate[J]. Liaoning Chem Ind,2002,31(10):435−436+455. doi: 10.3969/j.issn.1004-0935.2002.10.007
22. [22]
  LI M, LI H, JIANG F, CHU Y, NIE H. The Relation between morphology of (Co)MoS₂ phases and selective hydrodesulfurization for CoMo catalysts[J]. Catal Today,2010,149:35−39. doi: 10.1016/j.cattod.2009.03.017
23. [23]
  DOU Min-na, XIU Yuan, CAO Qing, XU Hua, XIAO Zhan-min. Review of test methods for four components of residue and petroleum bitumen[J]. Petrocheml Technol & Appl,2019, 37(5):356−360. doi: 10.3969/j.issn.1009-0045.2019.05.020
24. [24]
  YAN Fang, XIE Yong-jie. Investigation of separation of four fractions and interfacial properties of Da Qing crucial oil[J]. Chem Anal Meterage,2009,18(4):20−24. doi: 10.3969/j.issn.1008-6145.2009.04.006
25. [25]
  LI Hong-feng, ZHOU Zi-bing. Study on the method of chemical component analysis of asphaltene[J]. Heilongjiang Jiaotong Keji,2004,(8):17−18. doi: 10.3969/j.issn.1008-3383.2004.08.013
26. [26]
  MU Bao-quan, ZHANG Shu-xia. Improvement and optimization teaching of heavy oil four components analysis test[J]. Chem Educ (Chinese and English),2020,41(12):75−78.
27. [27]
  GUO Shu-xiang. Analysis of four component of heavy oil[J]. Spec Petrochem,2013,30(6):75−77. doi: 10.3969/j.issn.1003-9384.2013.06.021
28. [28]
  LI Y, ZHANG T, LIU D, LIU B, LU Y, CHAI Y, LIU C. Study of the promotion effect of citric acid on the active NiMoS phase in NiMo/Al₂O₃ catalysts[J]. Ind Eng Chem Res,2019,58(37):17195−17206.
29. [29]
  CORTÉS-JÁCOME M A, ESCOBAR J, ANGELES C C, LÓPEZ-SALINAS E, ROMERO E, FERRAT G, TOLEDO-ANTONIO J A. Highly dispersed CoMoS phase on titania nanotubes as efficient HDS catalysts[J]. Catal Today,2008,130(01):56−62. doi: 10.1016/j.cattod.2007.07.012
30. [30]
  KIM K D, LEE Y K. Active phase of dispersed mos₂ catalysts for slurry phase hydrocracking of vacuum residue[J]. J Catalysis,2019,369:111−121. doi: 10.1016/j.jcat.2018.10.013
31. [31]
  KRIJN P D J, LEON C A V D O, EELCO T C V, SONJA E, ABRAHAM J, HEINER F, PETRA E, DE J. High-resolution electron tomography study of an industrial Ni-Mo/-Al₂O₃ hydrotreating catalyst[J]. J Phys Chem B,2006,110(21):10209−10212. doi: 10.1021/jp061584f
32. [32]
  DEVERS E, AFANASIEV P, JOUGUET B, VRINAT M. Hydrothermal syntheses and catalytic properties of dispersed molybdenum sulfides[J]. Cata Lett,2002,82:13−17. doi: 10.1023/A:1020512320773
33. [33]
  HUANG Peng, LI Wen-bo, MAO Xue-feng, ZHAO Peng. Study on suspension bed hydrocracking of medium temperature pyrolytic heavy tar fraction[J]. J Fuel Chem Technol,2020,48(2):154−162. doi: 10.3969/j.issn.0253-2409.2020.02.004
34. [34]
  DAI Xin, DENG Wen-an. Application oil-soluble MoS₂ in slurry-bed hydrocraking for heavy oil[J]. Pet Ref Eng,2018,48(4):40−44. doi: 10.3969/j.issn.1002-106X.2018.04.011
35. [35]
  HENRIK T. In situ mössbauer emission spectroscopy studies of unsupported and supported sulfided CoMo hydrodesulfurization catalysts: Evidence for and nature of a CoMoS phase[J]. J Catalysis,1981,68(02):433−452. doi: 10.1016/0021-9517(81)90114-7
36. [36]
  DAAGE M, CHIANELLI R R. Structure-function relations in molybdenum sulfide catalysts: The "Rim-Edge" model[J]. J Catal,1994,149(2):414−427. doi: 10.1006/jcat.1994.1308
37. [37]
  ZHENG P, LI T, CHI K, XIAO C, FAN J, WANG X, DUAN A. DFT Insights into the formation of sulfur vacancies over corner/edge site of Co/Ni-promoted MoS₂ and WS₂ under the hydrodesulfurization conditions[J]. Appl Cata B Environ,2019,257:117937. doi: 10.1016/j.apcatb.2019.117937
38. [38]
  LI C, HAN Y, YANG T, DENG W. Preliminary study on the influence of catalyst dosage on coke formation of heavy oil slurry-bed hydrocracking[J]. Fuel,2020,270:117489. doi: 10.1016/j.fuel.2020.117489
1. [1]
  Wenlong LI , Xinyu JIA , Jie LING , Mengdan MA , Anning ZHOU . Photothermal catalytic CO₂ hydrogenation over a Mg-doped In₂O_3-x catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 919-929. doi: 10.11862/CJIC.20230421
2. [2]
  Hailian Tang , Siyuan Chen , Qiaoyun Liu , Guoyi Bai , Botao Qiao , Fei Liu . Stabilized Rh/hydroxyapatite Catalyst for Furfuryl Alcohol Hydrogenation: Application of Oxidative Strong Metal-Support Interactions in Reducing Conditions. Acta Physico-Chimica Sinica, 2025, 41(4): 100036-. doi: 10.3866/PKU.WHXB202408004
3. [3]
  Liuyun Chen , Wenju Wang , Tairong Lu , Xuan Luo , Xinling Xie , Kelin Huang , Shanli Qin , Tongming Su , Zuzeng Qin , Hongbing Ji . Soft template-induced deep pore structure of Cu/Al₂O₃ for promoting plasma-catalyzed CO₂ hydrogenation to DME. Acta Physico-Chimica Sinica, 2025, 41(6): 100054-. doi: 10.1016/j.actphy.2025.100054
4. [4]
  Fangxuan Liu , Ziyan Liu , Guowei Zhou , Tingting Gao , Wenyu Liu , Bin Sun . Hollow structured photocatalysts. Acta Physico-Chimica Sinica, 2025, 41(7): 100071-. doi: 10.1016/j.actphy.2025.100071
5. [5]
  Weihan Zhang , Menglu Wang , Ankang Jia , Wei Deng , Shuxing Bai . 表面硫物种对钯-硫纳米片加氢性能的影响. Acta Physico-Chimica Sinica, 2024, 40(11): 2309043-. doi: 10.3866/PKU.WHXB202309043
6. [6]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
7. [7]
  Xuejie Wang , Guoqing Cui , Congkai Wang , Yang Yang , Guiyuan Jiang , Chunming Xu . 碳基催化剂催化有机液体氢载体脱氢研究进展. Acta Physico-Chimica Sinica, 2025, 41(5): 100044-. doi: 10.1016/j.actphy.2024.100044
8. [8]
  Juntao Yan , Liang Wei . 2D S-Scheme Heterojunction Photocatalyst. Acta Physico-Chimica Sinica, 2024, 40(10): 2312024-. doi: 10.3866/PKU.WHXB202312024
9. [9]
  Yuanyin Cui , Jinfeng Zhang , Hailiang Chu , Lixian Sun , Kai Dai . Rational Design of Bismuth Based Photocatalysts for Solar Energy Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2405016-. doi: 10.3866/PKU.WHXB202405016
10. [10]
  Dan Li , Hui Xin , Xiaofeng Yi . Comprehensive Experimental Design on Ni-based Catalyst for Biofuel Production. University Chemistry, 2024, 39(8): 204-211. doi: 10.3866/PKU.DXHX202312046
11. [11]
  Haodong JIN , Qingqing LIU , Chaoyang SHI , Danyang WEI , Jie YU , Xuhui XU , Mingli XU . NiCu/ZnO heterostructure photothermal electrocatalyst for efficient hydrogen evolution reaction. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1068-1082. doi: 10.11862/CJIC.20250048
12. [12]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317
13. [13]
  Juan WANG , Zhongqiu WANG , Qin SHANG , Guohong WANG , Jinmao LI . NiS and Pt as dual co-catalysts for the enhanced photocatalytic H₂ production activity of BaTiO₃ nanofibers. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1719-1730. doi: 10.11862/CJIC.20240102
14. [14]
  Yang WANG , Xiaoqin ZHENG , Yang LIU , Kai ZHANG , Jiahui KOU , Linbing SUN . Mn single-atom catalysts based on confined space: Fabrication and the electrocatalytic oxygen evolution reaction performance. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2175-2185. doi: 10.11862/CJIC.20240165
15. [15]
  Wen YANG , Didi WANG , Ziyi HUANG , Yaping ZHOU , Yanyan FENG . La promoted hydrotalcite derived Ni-based catalysts: In situ preparation and CO₂ methanation performance. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 561-570. doi: 10.11862/CJIC.20230276
16. [16]
  Asif Hassan Raza , Shumail Farhan , Zhixian Yu , Yan Wu . 用于高效制氢的双S型ZnS/ZnO/CdS异质结构光催化剂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406020-. doi: 10.3866/PKU.WHXB202406020
17. [17]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
18. [18]
  Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-based Photocatalysts for CO₂ Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2406029-. doi: 10.3866/PKU.WHXB202406029
19. [19]
  Shuang Yang , Qun Wang , Caiqin Miao , Ziqi Geng , Xinran Li , Yang Li , Xiaohong Wu . Ideological and Political Education Design for Research-Oriented Experimental Course of Highly Efficient Hydrogen Production from Water Electrolysis in Aerospace Perspective. University Chemistry, 2024, 39(11): 269-277. doi: 10.12461/PKU.DXHX202403044
20. [20]
  Yulian Hu , Xin Zhou , Xiaojun Han . A Virtual Simulation Experiment on the Design and Property Analysis of CO₂ Reduction Photocatalyst. University Chemistry, 2025, 40(3): 30-35. doi: 10.12461/PKU.DXHX202403088

Get Citation

PDF

XML

Metrics

PDF Downloads(15)
Abstract views(2692)
HTML views(533)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142