Citation: SHI Lin, HUANG Wei, SONG Shu-Zheng, LI Zhi-Bo, LIU Shuang-Qiang. Effect of the Fluorine Addition Method on the Hydrodesulfurization Performance of NiMo Catalysts over Slurry Bed[J]. Acta Physico-Chimica Sinica, ;2015, 31(8): 1559-1566. doi: 10.3866/PKU.WHXB201506083 shu

Effect of the Fluorine Addition Method on the Hydrodesulfurization Performance of NiMo Catalysts over Slurry Bed

1.
Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, P. R. China

Received Date: 18 March 2015
Available Online: 8 June 2015
Fund Project: 国家自然科学基金重点项目(21336006) (21336006) 国家自然科学基金面上项目(21176176) (21176176)高等学校博士学科点专项(优先发展领域)(20111402130002)资助 (优先发展领域)(20111402130002)

NiMo/TiO₂-Al₂O₃ slurry catalysts with fluorine as an additive were prepared by complete liquidphase technology for hydrodesulfurization. The effect of different fluorine addition methods on the properties of the catalysts for 4,6-dimethyldibenzothiophene (4,6-DMDBT) hydrodesulfurization were investigated. The catalysts were characterized by X-ray diffraction (XRD), temperature-programmed reduction of H₂ (H₂-TPR), N₂ adsorption-desorption isotherms (BET), X-ray photoelectron spectroscopy (XPS), and high-resolution transmission electron microscopy (HRTEM). The results reveal that in the absence of nitric acid, adding fluoride into the catalyst before the introduce of molybdenum and nickel ions can significantly increase the surface area and average pore size, improve the dispersion of metallic nickel on the surface of catalyst, and weaken the interaction between the metal and the support. This effectively increases the sulfidation degree of Mo, MoS₂ slab stacking, and the content of the highly active Ni-Mo-S(II) phase, which can promote the hydrogenation of the aromatic ring and the hydrogenolysis of the C-S bond, and thus increase the hydrodesulfurization activity for 4,6-DMDBT.
- Complete liquid-phase technology,
- Fluoride,
- 4, 6-DMDBT,
- Slurry bed
1. [1]
  
  (1) Stanislaus, A.; Marafi, A.; Rana, M. S. Catal. Today 2010, 153, 1. doi: 10.1016/j.cattod.2010.05.011
2. [2]
  (2) Chen, Y. D.; Wang, L.; Liu, T. F.; Zhang, Y. L.; Liu, X. Y.; Jiang, Z. X.; Li, C. Chem. React. Eng. Technol. 2013, 29, 392. [陈燕蝶, 王璐, 刘铁峰. 张玉良, 刘欣毅, 蒋宗轩, 李灿. 化学反应工程与工艺, 2013, 29, 392.]
3. [3]
  (3) Si, Y. H.; Zhu, Y. Q.; Zou, R. M.; Guo, F.; Wang, J. C. Chem. Eng. Oil Gas. 2014, 43, 82. [司云航, 朱玉琴, 邹蓉梅. 郭凡, 王嘉春. 石油与天然气化工, 2014, 43, 82.]
4. [4]
  (4) Mochida, I.; Choi, K. J. Jpn. Pet. Inst. 2004, 47, 145. doi: 10.1627/jpi.47.145
5. [5]
  (5) Song, C. Catal. Today 2003, 86, 211. doi: 10.1016/S0920-5861(03)00412-7
6. [6]
  (6) Matos, E. M.; Guirardello, R.; Mori, M.; Nunhez, J. R. Comput. Chem. Eng. 2009, 33, 1115. doi: 10.1016/j. compchemeng.2008. 12.011
7. [7]
  (7) Deng, Z. H.; Wang, T. F.; Wang, Z. W. Chem. Eng. Sci. 2009, 65, 480.
8. [8]
  (8) Gao, Z. H.; Hao, L. F.; Huang, W.; Xie, K. C. Catal. Lett. 2005, 102, 139. doi: 10.1007/s10562-005-5845-7
9. [9]
  (9) Gao, Z. H.; Huang, W.; Hao, L. F.; Xie, K. C. Chin. J. Catal. 2006, 27, 86. [高志华, 黄伟, 郝利峰, 谢克昌. 催化学报, 2006, 27, 86.]
10. [10]
  (10) Li, Z. B. Complete Liquid-Phase Technology for Ultra Deep Hydrodesulfurizationin in Simulation Diesel. MS. Dissertation, Taiyuan University of Technology, Taiyuan, 2014. [李志博. 完全液相催化剂制备技术在模拟柴油超精脱硫中的应用研究[D]. 太原: 太原理工大学, 2014.]
11. [11]
  (11) Lü, J.; Zhang, W.; Yang, Z. Q.; Li, J. Y.; Tang, X. B.; Lü, J. Chem. World 2012, 9, 567. [吕婧, 张伟, 杨志强, 李娇毅, 唐晓博, 吕剑. 化学世界, 2012, 9, 567.]
12. [12]
  (12) Kim, H.; Lee, J. J.; Moon, S. H. Appl. Catal. B 2003, 44, 287. doi: 10.1016/S0926-3373(03)00077-8
13. [13]
  (13) Sun, M. Y.; Nicosia, D.; Prins, R. Catal. Today 2003, 86, 173. doi: 10.1016/S0920-5861(03)00410-3
14. [14]
  (14) Matralis, H.; Papadopoulou, C.; Lycourghiotis, A. Appl. Catal. A-Gen. 1994, 116, 221. doi: 10.1016/0926-860X(94)80291-2
15. [15]
  (15) Lewis, J. M.; Kydd, R. A.; Boorman, P. M. J. Catal. 1989, 120, 413. doi: 10.1016/0021-9517(89)90281-9
16. [16]
  (16) Sarbak, Z.; Andersson, S. L. T. Appl. Catal. 1991, 69, 235. doi: 10.1016/S0166-9834(00)83305-9
17. [17]
  (17) Eliche-Quesada, D.; Merida-Robles, J.; Maireles-Torres, P.; Rodriguez-Castellon, E.; Jimenez-Lopez, A. Langmuir 2003, 19, 4985. doi: 10.1021/la020865l
18. [18]
  (18) Lai, W. K.; Pang, L. Q.; Zheng, J. B.; Li, J. J.; Wu, Z. F.; Yi, X. D.; Fang, W. P.; Jia, L. S. Fuel. Process. Technol. 2013, 110, 8. doi: 10.1016/j.fuproc.2013.01.006
19. [19]
  (19) Liu, H.; Yin, C. L.; Li, H.; Liu, B.; Li, X. H.; Chai, Y. M.; Li, Y. P.; Liu, C. G. Fuel 2014, 129, 138. doi: 10.1016/j.fuel. 2014.03.055
20. [20]
  (20) Qu, L. L.; Zhang, W. P.; Prins, R.; Kooyman, P. J. J. Catal. 2003, 215, 7. doi: 10.1016/S0021-9517(02)00181-1
21. [21]
  (21) Cuevas, R.; Ramirez, J.; Busca, G. J. Fluorine Chem. 2003, 122, 151. doi: 10.1016/S0022-1139(03)00054-X
22. [22]
  (22) Al-Dalama, K.; Stanislaus, A. Thermochim. Acta 2011, 520, 67. doi: 10.1016/j.tca.2011.03.017
23. [23]
  (23) Damyanova, S.; Petrov, L.; Grange, P. Appl. Catal. A-Gen. 2003, 239, 241. doi: 10.1016/S0926-860X(02)00385-X
24. [24]
  (24) Rashidi, F.; Sasaki, T.; Rashidi, A. M.; Nemati K. A.; Jozani, K. J. J. Catal. 2013, 299, 321.. doi: 10.1016/j.jcat.2012.11.012
25. [25]
  (25) Li, H. F.; Li, M. F.; Chu, Y.; Liu, F.; Nie, H. Appl. Catal. A-Gen. 2011, 403, 75. doi: 10.1016/j.apcata.2011.06.015
26. [26]
  (26) Yao, S. D.; Zheng, Y.; Ng, S.; Ding, L. H.; Yang, H. Appl. Catal. A-Gen. 2012, 435-436, 61.
27. [27]
  (27) Shimada, H. Catal. Today 2003, 86, 17. doi: 10.1016/S0920-5861(03)00401-2
28. [28]
  (28) Guo, R.; Shen, B. X.; Fang, X. C.; Sun, J.; Peng, C.; Cui, X. L. China Pet. Process. Pe. 2014, 16, 12.
29. [29]
  (29) Sanchez-Minero F.; Ramirez, J.; Gutierrez-Alejandre, A.; Fernandez-Vargasa, C.; Torres-Manceraa, P.; Cuevas-Garciaa, R. Catal. Today 2008, 133-135, 267.
30. [30]
  (30) Manoli, J. M.; Costa, P. D.; Brun, M.; Vrinat, M.; Mauge, F.; Potvin, C. J. Catal. 2004, 221, 365. doi: 10.1016/j.jcat. 2003.08.011
31. [31]
  (31) Zhang, Z. C.; Huang, X. L.; Wei, H. J.; Liu, J. J.; Liu, Z. Petrochem. Technol. 2009, 38, 1353. [张志成, 黄星亮, 魏焕景, 刘建军, 刘志. 石油化工, 2009, 38, 1353.]
32. [32]
  (32) Vradman, L.; Landau, M. V.; Herskowitz, M. Fuel 2003, 82, 633. doi: 10.1016/S0016-2361(02)00354-X
33. [33]
  (33) Qihe, R. M.; Yuan, H.; Li, H. F.; Zhang, W. H.; Xu, G. T. Acta Petrolei. Sin.(Pet. Process. Sect.) 2011, 27, 429. [齐和日玛, 袁蕙, 李会峰, 张韫宏, 徐广通. 石油学报(石油加工), 2011, 27, 429.]
1. [1]
  Yanglin Jiang , Mingqing Chen , Min Liang , Yige Yao , Yan Zhang , Peng Wang , Jianping Zhang . Experimental and Theoretical Investigations of Solvent Polarity Effect on ESIPT Mechanism in 4′-N,N-diethylamino-3-hydroxybenzoflavone. Acta Physico-Chimica Sinica, 2025, 41(2): 100012-. doi: 10.3866/PKU.WHXB202309027
2. [2]
  Xiaoning TANG , Shu XIA , Jie LEI , Xingfu YANG , Qiuyang LUO , Junnan LIU , An XUE . Fluorine-doped MnO₂ with oxygen vacancy for stabilizing Zn-ion batteries. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1671-1678. doi: 10.11862/CJIC.20240149
3. [3]
  Tingting Yu , Si Chen , Lianglong Sun , Tongtong Shi , Kai Sun , Xin Wang . Comprehensive Experimental Design for the Photochemical Synthesis, Analysis, and Characterization of Difluoropyrroles. University Chemistry, 2024, 39(11): 196-203. doi: 10.3866/PKU.DXHX202401022
4. [4]
  Xiaofeng Xia , Jielian Zhu . Innovative Comprehensive Experimental Design: Synthesis of 6-Fluoro-N-benzoyl Tetrahydroquinoline. University Chemistry, 2024, 39(10): 344-352. doi: 10.12461/PKU.DXHX202405063
5. [5]
  Shahua Huang , Xiaoming Guo , Lin Lin , Guangping Chang , Sheng Han , Zuxin Zhou . Application of “Integration of Industry and Education” in Engineering Chemistry: Improvement of the Pesticide Fipronil Production. University Chemistry, 2024, 39(3): 199-204. doi: 10.3866/PKU.DXHX202309064
6. [6]
  Runhua Chen , Qiong Wu , Jingchen Luo , Xiaolong Zu , Shan Zhu , Yongfu Sun . 缺陷态二维超薄材料用于光/电催化CO₂还原的基础与展望. Acta Physico-Chimica Sinica, 2025, 41(3): 2308052-. doi: 10.3866/PKU.WHXB202308052
7. [7]
  Yanhui Zhong , Ran Wang , Zian Lin . Analysis of Halogenated Quinone Compounds in Environmental Water by Dispersive Solid-Phase Extraction with Liquid Chromatography-Triple Quadrupole Mass Spectrometry. University Chemistry, 2024, 39(11): 296-303. doi: 10.12461/PKU.DXHX202402017
8. [8]
  Caixia Lin , Zhaojiang Shi , Yi Yu , Jianfeng Yan , Keyin Ye , Yaofeng Yuan . Ideological and Political Design for the Electrochemical Synthesis of Benzoxathiazine Dioxide Experiment. University Chemistry, 2024, 39(2): 61-66. doi: 10.3866/PKU.DXHX202309005
9. [9]
  Yang Chen , Peng Chen , Yuyang Song , Yuxue Jin , Song Wu . Application of Chemical Transformation Driven Impurity Separation in Experiments Teaching: A Novel Method for Purification of α-Fluorinated Mandelic Acid. University Chemistry, 2024, 39(6): 253-263. doi: 10.3866/PKU.DXHX202310077
10. [10]
  Mingyang Men , Jinghua Wu , Gaozhan Liu , Jing Zhang , Nini Zhang , Xiayin Yao . 液相法制备硫化物固体电解质及其在全固态锂电池中的应用. Acta Physico-Chimica Sinica, 2025, 41(1): 2309019-. doi: 10.3866/PKU.WHXB202309019
11. [11]
  Zizheng LU , Wanyi SU , Qin SHI , Honghui PAN , Chuanqi ZHAO , Chengfeng HUANG , Jinguo PENG . Surface state behavior of W doped BiVO₄ photoanode for ciprofloxacin degradation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 591-600. doi: 10.11862/CJIC.20230225
12. [12]
  Liangzhen Hu , Li Ni , Ziyi Liu , Xiaohui Zhang , Bo Qin , Yan Xiong . A Green Chemistry Experiment on Electrochemical Synthesis of Benzophenone. University Chemistry, 2024, 39(6): 350-356. doi: 10.3866/PKU.DXHX202312001
13. [13]
  Xiaoling LUO , Pintian ZOU , Xiaoyan WANG , Zheng LIU , Xiangfei KONG , Qun TANG , Sheng WANG . Synthesis, crystal structures, and properties of lanthanide metal-organic frameworks based on 2, 5-dibromoterephthalic acid ligand. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1143-1150. doi: 10.11862/CJIC.20230271
14. [14]
  Lianghong Ye , Junqing Ni , Zhongyi Yan , Zhanming Zhang , Can Zhu , Mo Sun . Chemical Fuel-Driven Non-Equilibrium Color Change. University Chemistry, 2025, 40(3): 349-354. doi: 10.12461/PKU.DXHX202406109
15. [15]
  Yonghui ZHOU , Rujun HUANG , Dongchao YAO , Aiwei ZHANG , Yuhang SUN , Zhujun CHEN , Baisong ZHU , Youxuan ZHENG . Synthesis and photoelectric properties of fluorescence materials with electron donor-acceptor structures based on quinoxaline and pyridinopyrazine, carbazole, and diphenylamine derivatives. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 701-712. doi: 10.11862/CJIC.20230373
16. [16]
  Yihao Zhao , Jitian Rao , Jie Han . Synthesis and Photochromic Properties of 3,3-Diphenyl-3H-Naphthopyran: Design and Teaching Practice of a Comprehensive Organic Experiment. University Chemistry, 2024, 39(10): 149-155. doi: 10.3866/PKU.DXHX202402050
17. [17]
  Yutong Dong , Huiling Xu , Yucheng Zhao , Zexin Zhang , Ying Wang . The Hidden World of Surface Tension and Droplets. University Chemistry, 2024, 39(6): 357-365. doi: 10.3866/PKU.DXHX202312022
18. [18]
  Gaoyan Chen , Chaoyue Wang , Juanjuan Gao , Junke Wang , Yingxiao Zong , Kin Shing Chan . Heart to Heart: Exploring Cardiac CT. University Chemistry, 2024, 39(9): 146-150. doi: 10.12461/PKU.DXHX202402011
19. [19]
  Qingjun PAN , Zhongliang GONG , Yuwu ZHONG . Advances in modulation of the excited states of photofunctional iron complexes. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 45-58. doi: 10.11862/CJIC.20240365
20. [20]
  Sheng Zhang , Mingyu Wang , Xiaohong Wang , Jiancheng Feng . Multidimensional Teaching Design and Ideological and Political Exploration of Analytical Chemistry Experiment under the Complete Credit System. University Chemistry, 2024, 39(2): 189-195. doi: 10.3866/PKU.DXHX202307071

Get Citation

PDF

XML

Metrics

PDF Downloads(270)
Abstract views(617)
HTML views(45)

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