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
-
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.
-
Keywords:
-
Complete liquid-phase technology
, - Fluoride,
- 4, 6-DMDBT,
- Slurry bed
-
-
-
-
[1]
(1) Stanislaus, A.; Marafi, A.; Rana, M. S. Catal. Today 2010, 153, 1. doi: 10.1016/j.cattod.2010.05.011
-
[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) 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) Mochida, I.; Choi, K. J. Jpn. Pet. Inst. 2004, 47, 145. doi: 10.1627/jpi.47.145
-
[5]
(5) Song, C. Catal. Today 2003, 86, 211. doi: 10.1016/S0920-5861(03)00412-7
-
[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) Deng, Z. H.; Wang, T. F.; Wang, Z. W. Chem. Eng. Sci. 2009, 65, 480.
-
[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) 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) 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) 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) Kim, H.; Lee, J. J.; Moon, S. H. Appl. Catal. B 2003, 44, 287. doi: 10.1016/S0926-3373(03)00077-8
-
[13]
(13) Sun, M. Y.; Nicosia, D.; Prins, R. Catal. Today 2003, 86, 173. doi: 10.1016/S0920-5861(03)00410-3
-
[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) Lewis, J. M.; Kydd, R. A.; Boorman, P. M. J. Catal. 1989, 120, 413. doi: 10.1016/0021-9517(89)90281-9
-
[16]
(16) Sarbak, Z.; Andersson, S. L. T. Appl. Catal. 1991, 69, 235. doi: 10.1016/S0166-9834(00)83305-9
-
[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) 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) 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) 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) Cuevas, R.; Ramirez, J.; Busca, G. J. Fluorine Chem. 2003, 122, 151. doi: 10.1016/S0022-1139(03)00054-X
-
[22]
(22) Al-Dalama, K.; Stanislaus, A. Thermochim. Acta 2011, 520, 67. doi: 10.1016/j.tca.2011.03.017
-
[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) 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) 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) Yao, S. D.; Zheng, Y.; Ng, S.; Ding, L. H.; Yang, H. Appl. Catal. A-Gen. 2012, 435-436, 61.
-
[27]
(27) Shimada, H. Catal. Today 2003, 86, 17. doi: 10.1016/S0920-5861(03)00401-2
-
[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) 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) 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) 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) Vradman, L.; Landau, M. V.; Herskowitz, M. Fuel 2003, 82, 633. doi: 10.1016/S0016-2361(02)00354-X
-
[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]
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
-
[2]
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
-
[3]
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): 2309027-0. doi: 10.3866/PKU.WHXB202309027
-
[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]
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]
Aiyi Xin , Jiawei Li , Xinyang Ran , Chuanjiang Fu , Zhiguo Wang . Collaborative Science and Education Based Experimental Design in Organic Chemistry: A Case Study of the Nucleophilic Substitution Reaction of 2-Hydroxymethyl-4,6-Di-Tert-Butylphenol. University Chemistry, 2025, 40(5): 366-375. doi: 10.12461/PKU.DXHX202407031
-
[7]
Xiaoyang Li , Xiaowei Huang , Yimeng Zhang , Huan Liu , Shao Jin , Junpeng Zhuang . Comprehensive Chemical Experiments on the Synthesis of 1,3-Dibromo-5,5-Dimethylhydantoin and Its Application as a Brominating Reagent. University Chemistry, 2025, 40(7): 286-293. doi: 10.12461/PKU.DXHX202408035
-
[8]
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): 100054-0. doi: 10.1016/j.actphy.2025.100054
-
[9]
Jichao XU , Ming HU , Xichang CHEN , Chunhui WANG , Leichen WANG , Lingyi ZHOU , Xing HE , Xiamin CHENG , Su JING . Construction and hydrogen peroxide-activated chemodynamic activity of ferrocene?benzoselenadiazole conjugate. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1495-1504. doi: 10.11862/CJIC.20250144
-
[10]
Runhua Chen , Qiong Wu , Jingchen Luo , Xiaolong Zu , Shan Zhu , Yongfu Sun . Defective Ultrathin Two-Dimensional Materials for Photo-/Electrocatalytic CO2 Reduction: Fundamentals and Perspectives. Acta Physico-Chimica Sinica, 2025, 41(3): 2308052-0. doi: 10.3866/PKU.WHXB202308052
-
[11]
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
-
[12]
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
-
[13]
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
-
[14]
Benhua Wang , Chaoyi Yao , Yiming Li , Qing Liu , Minhuan Lan , Guipeng Yu , Yiming Luo , Xiangzhi Song . 一种基于香豆素氟离子荧光探针的合成、表征及性能测试——“科研反哺教学”在有机化学综合实验教学中的探索与实践. University Chemistry, 2025, 40(6): 201-209. doi: 10.12461/PKU.DXHX202408070
-
[15]
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
-
[16]
Mingyang Men , Jinghua Wu , Gaozhan Liu , Jing Zhang , Nini Zhang , Xiayin Yao . Sulfide Solid Electrolyte Synthesized by Liquid Phase Approach and Application in All-Solid-State Lithium Batteries. Acta Physico-Chimica Sinica, 2025, 41(1): 100004-0. doi: 10.3866/PKU.WHXB202309019
-
[17]
Yajie Li , Bin Chen , Yiping Wang , Hui Xing , Wei Zhao , Geng Zhang , Siqi Shi . Inhibiting Dendrite Growth by Customizing Electrolyte or Separator to Achieve Anisotropic Lithium-Ion Transport: A Phase-Field Study. Acta Physico-Chimica Sinica, 2024, 40(3): 2305053-0. doi: 10.3866/PKU.WHXB202305053
-
[18]
Jianding LI , Junyang FENG , Huimin REN , Gang LI . Proton conductive properties of a Hf(Ⅳ)-based metal-organic framework built by 2,5-dibromophenyl-4,6-dicarboxylic acid. Chinese Journal of Inorganic Chemistry, 2025, 41(6): 1094-1100. doi: 10.11862/CJIC.20240464
-
[19]
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
-
[20]
Qi Wu , Changhua Wang , Yingying Li , Xintong Zhang . Enhanced photocatalytic synthesis of H2O2 by triplet electron transfer at g-C3N4@BN van der Waals heterojunction interface. Acta Physico-Chimica Sinica, 2025, 41(9): 100107-0. doi: 10.1016/j.actphy.2025.100107
-
[1]
Metrics
- PDF Downloads(270)
- Abstract views(676)
- HTML views(48)