Citation: GUO Xing-mei, SONG Mao-ning, ZHAO Xu, ZHAO Liang-fu. Effect of fluoride promoter on the catalytic activity of NiWF/γ-Al2O3 for hydrodenitrogenation and hydrodesulfurization of coal tar[J]. Journal of Fuel Chemistry and Technology, ;2016, 44(11): 1326-1333. shu

Effect of fluoride promoter on the catalytic activity of NiWF/γ-Al2O3 for hydrodenitrogenation and hydrodesulfurization of coal tar

  • Corresponding author: GUO Xing-mei, linyrain@163.com ZHAO Liang-fu, lfzhao@sxicc.ac.cn
  • Received Date: 18 August 2016
    Revised Date: 21 September 2016

    Fund Project: The project was supported by the Strategic Science and Technology Project of Chinese Academy of Sciences XDA07020200the Development of Gasification Coal Tar Hydrogenation Furnace of Luqi CFBYKJ-JSFW-01-2014

Figures(8)

  • A series of NiWF (x)/γ-Al2O3 catalysts were prepared by adding different amounts of ammonium fluoride, and the effects of fluoride amount on the structure and physicochemical properties were investigated with X-ray diffraction, X-ray photoelectron spectroscopy, NH3-TPD and high resolution transmission electron mcroscopy (HRTEM) techniques and N2 sorption experiment. Their hydrodenitrogenation (HDN) and hydrodesulfurization (HDS) catalytic performances were evaluated in a fix-bed reactor with low and middle-temperature coal tar obtained from Inner Mongolia as feedstock. Although fluoride amount has little effect on the pore diameter and pore volume of the catalysts, increase of the fluoride amount decreases the specific surface area. In addition, the sulfidation degree of the catalyst decreases with the fluoride amount when it is sulfided at 643 K for 6 h. Also, the numbers of strong acid sites and total amount acid sites change with increasing fluoride amount. They slightly increase at first, but then obviously decrease. HRTEM shows that WS2 slabs have a typical layered structure. The catalytic activity of NiWF (x)/γ-Al2O3 for HDN and HDS of coal tar shows a volcanic trend with the fluoride amount.
  • 加载中
    1. [1]

      HAN C R.Hydrocracking Technology and Engineering[M].Beijing:China Petrochemical Press, 2006:1-27.

    2. [2]

      LEI Z, HU D N, PAN H T, LU J Y. Research progress of coal tar catalytic hydrogenation[J]. Mod Chem Ind, 2014,34(1):30-35.  

    3. [3]

      CHEN T N, GE X J, MA J. Hydrogenation process of medium & low temperature coal tar[J]. Fuel Chem Process, 2013,44(4):52-57.  

    4. [4]

      YU Y C, GAO H Y, ZHANG M N, QIAO S. Research progress of coal tar hydrogenation catalyst[J]. Ind Prod, 2016,42(2):137-143.  

    5. [5]

      ZHANG K Y, LIU A H, YAN J, GUO J X, LIU C G. Characterization of CoMo/Al2O3 hydrodesulfurization catalysts prepared by different methods[J]. Chin J Catal, 2005,26(8):639-644.  

    6. [6]

      ZHENG A G, FANG S L, ZHANG J, CHEN W B, XU G T. The characterization of NiMo/Al2O3 hydrotreating catalyst by TEM and AEM[J]. Acta Petrol Sin, 2008,24(4):433-437.

    7. [7]

      WANG Y G, ZHANG H Y, ZHANG P Z, XU D P, ZHAO K, WANG F J. Hydroprocessing of low temperature coal tar on NiW/γ-Al2O3 catalyst[J]. J Fuel Chem Technol, 2012,40(12):1492-1497.  

    8. [8]

      WANG W Y, YANG Y Q, LUO H, PENG H Z, ZHANG X Z, HU T. Preparation and hydrodeoxygenation properties of Ni-Co-W-B amorphous catalyst[J]. Chin J Catal, 2011,32(10):1645-1650.  

    9. [9]

      WANG H Y, SONG P P, WANG Y J. Influence of hierarchically mesoporous H βzeolite on the performance of NiWP/H β-Al2O3 catalysts in diesel oil hydro-upgrading[J]. J Fuel Chem Technol, 2016,44(4):470-476.  

    10. [10]

      MAITY S K, LEMUS M, ANCHEYTA J. Effect of preparation methods and content of boron on hydrotreating catalytic activity[J]. Energy Fuels, 2011,25:3100-3107. doi: 10.1021/ef2004915

    11. [11]

      QU L L, JIAN M, SHI Y H, LI D D. Effect of Fluorine on sulfide type NiW/γ-Al2O3 catalyst[J]. Chin J Catal, 1998,19(6):608-609.

    12. [12]

      JIRFITOVFI K, KRANS M. Effect of support properties on the catalytic activity of HDS catalysts[J]. Appl Catal, 1986,27(1):21-29. doi: 10.1016/S0166-9834(00)81043-X

    13. [13]

      MATRALIS H K, LYCOURGHIOTIS A, GRANGE P, DELMON B. Fluorinated hydrotreatment catalysts:Characterization and hydrode-sulphurization activity of fluorine-cobalt-molybdenum/γ-alumina catalysts[J]. Appl Catal, 1988,38(2):273-287. doi: 10.1016/S0166-9834(00)82831-6

    14. [14]

      SARBAK Z, ANDERSSON S L T. Effect of metal-organic compounds on thiophene hydrodesulphurization over sulphided forms of fluoride-containing CoMo/Al2O3 catalysts[J]. Appl Catal, 1991,69(1):235-251. doi: 10.1016/S0166-9834(00)83305-9

    15. [15]

      BENITEZ A, RAMIREZ J, FIERRO J L G, AGUDO A. Effect of fluoride on the structure and activity of NiW/Al2O3 catalysts for HDS of thiophene and HDN of pyridine[J]. Appl Catal, 1996,144(1/2):343-364.

    16. [16]

      LI B, SHAO L L. Appraisal of alumina and aluminium hydroxide by XRD[J]. Inorg Chem Ind, 2008,40(2):54-57.  

    17. [17]

      CUI G Q, WANG J F, FAN H F, SUN X Y, JIANG Y, WANG S J, LIU D, GUI J Z. Towards understanding the microstructures and hydrocracking performance of sulfided Ni-W catalysts:Effect of metal loading[J]. Fuel Process Technol, 2011,92(12):2320-2327. doi: 10.1016/j.fuproc.2011.07.020

    18. [18]

      EBRAHIMYNEJAD M, HAGHIGHI M, ASGARI N. Ultrasound assisted synthesis and physicochemical characterizations of fluorine-modified CoMo/Al2O3 nanocatalysts used for hydrodesulfurization of thiophene[J]. J Nanosci Nanotechnol, 2014,14(9):6848-6857. doi: 10.1166/jnn.2014.8966

    19. [19]

      DING L H, ZHENG Y, ZHANG Z S. Hydrotreating of light cycle oil using WNi catalysts containing hydrothermally and chemically treated zeolite Y[J]. Catal Today, 2007,125(3):229-238.  

    20. [20]

      NIU G X, CHEN H Y, LI Q Z. The effect of treatment of ammonium fluosilicate on NiW/γ-Al2O3[J]. Chin J Catal, 1997,18(4):279-283.

    21. [21]

      CORMA A, FORNES V, ORTEGA E. The nature of acid sites on fluorinated γ-Al2O3[J]. Chin J Catal, 1985,92(2):284-290. doi: 10.1016/0021-9517(85)90262-3

    22. [22]

      MICIUKIEWICZ J. Studies of molybdena-alumina catalysts:XV.Effect of fluorine-modified alumina on catalyst properties[J]. Appl Catal, 1989,49(2):247-257. doi: 10.1016/S0166-9834(00)83021-3

    23. [23]

      BENITEZ A, RAMIREZ J, VAZQUEZ A. Influence of alumina fluoridation on the dispersion and hydrotreating activity of W/Al2O3 catalysis[J]. Appl Catal A:Gen, 1995,133(1):103-119. doi: 10.1016/0926-860X(95)00177-8

    24. [24]

      MENG X X, QIU Z G, GUO X M, LI Z R, HU N F, SONG M N, ZHAO L F. Hydrodenitrogenation and hydrodesulfurization of coal tar on Ni-W catalysts with different metal loadings[J]. J Fuel Chem Technol, 2016,44(5):570-578.  

    25. [25]

      EGOROVA M, PRINS R. Competitive hydrodesulfurization of 4, 6-dimethyl dibenzothiophene, hydrodenitrogenation of 2-methylpyridine and hydrogenation of naphthalene over sulfided NiMo/γ-Al2O3[J]. J Catal, 2004,224(2):278-287. doi: 10.1016/j.jcat.2004.03.005

    26. [26]

      JIAN M, PRINS R. Existence of different catalytic sites in HDN catalysts[J]. Catal Today, 1996,30(1/3):127-134.  

  • 加载中
    1. [1]

      Shunping WANG , Chuandong GE , Shuguang QU , Tianduo LI , Shaomin WANG , Qingyuan YANG . Synthesis of a fluorescent probe based on urea-based coordination and Si—O bond cleavage for F- and Cr(Ⅵ) detection. Chinese Journal of Inorganic Chemistry, 2026, 42(2): 297-308. doi: 10.11862/CJIC.20250214

    2. [2]

      Jilei LIANG , Mengmeng WU , Lü QI , Yunqi LIU , Chenguang LIU . In-situ preparation of mesoporous carbon-encapsulated NiMoS hydrodesulfurization catalyst. Chinese Journal of Inorganic Chemistry, 2026, 42(10): 2127-2137. doi: 10.11862/CJIC.20260127

    3. [3]

      Lixing ZHANG , Yaowen WANG , Xu HAN , Junhong ZHOU , Jinghui WANG , Liping LI , Guangshe LI . Research progress in the synthesis of fluorine-containing perovskites and their derivatives. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1689-1701. doi: 10.11862/CJIC.20250007

    4. [4]

      Yang Li , Yanan Dong , Zhihong Wei , Changzeng Yan , Zhen Li , Lin He , Yuehui Li . Fluoride-promoted Ni-catalyzed cyanation of C–O bond using CO2 and NH3. Chinese Chemical Letters, 2025, 36(5): 110206-. doi: 10.1016/j.cclet.2024.110206

    5. [5]

      Ao Sun , Zipeng Li , Shuchun Li , Xiangbao Meng , Zhongtang Li , Zhongjun Li . Stereoselective synthesis of α-3-deoxy-D-manno-oct-2-ulosonic acid (α-Kdo) derivatives using a C3-p-tolylthio-substituted Kdo fluoride donor. Chinese Chemical Letters, 2025, 36(3): 109972-. doi: 10.1016/j.cclet.2024.109972

    6. [6]

      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

    7. [7]

      Xiaorui Chen , Xuan Luo , Tongming Su , Xinling Xie , Liuyun Chen , Yuejing Bin , Zuzeng Qin , Hongbing Ji . Ga-doped Cu/γ-Al2O3 bifunctional interface sites promote the direct hydrogenation of CO2 to DME. Acta Physico-Chimica Sinica, 2025, 41(10): 100126-0. doi: 10.1016/j.actphy.2025.100126

    8. [8]

      Haotian Zhang , Shengfa Feng , Mufan Cao , Xiong Xiong Liu , Pengcheng Yuan , Yaping Wang , Min Gao , Long Pan , Zhengming Sun . Al2O3 coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries. Chinese Chemical Letters, 2025, 36(8): 111096-. doi: 10.1016/j.cclet.2025.111096

    9. [9]

      Zhiquan YIN , Wenlong ZHEN , Xiaofeng NING , Zhengzhi HAN , Gongxuan LÜ . Mechanism of Al2O3 layer in enhancing the stability and activity of GaN for photocatalytic overall water splitting. Chinese Journal of Inorganic Chemistry, 2026, 42(7): 1523-1533. doi: 10.11862/CJIC.20260038

    10. [10]

      Peng-Fei Li , Chun-Li Hu , Bo Zhang , Jiang-Gao Mao , Fang Kong . From HgGa2(SeO3)4 to Hg2Ga(SeO3)2F: The first HgⅠ-based selenite birefringent crystal triggered by linear groups and fluoride ions. Chinese Chemical Letters, 2026, 37(2): 110588-. doi: 10.1016/j.cclet.2024.110588

    11. [11]

      Kai Han ,  Guohui Dong ,  Ishaaq Saeed ,  Tingting Dong ,  Chenyang Xiao . Morphology and photocatalytic tetracycline degradation of g-C3N4 optimized by the coal gangue. Chinese Journal of Structural Chemistry, 2024, 43(2): 100208-100208. doi: 10.1016/j.cjsc.2023.100208

    12. [12]

      Yaping ZHANG , Tongchen WU , Yun ZHENG , Bizhou LIN . Z-scheme heterojunction β-Bi2O3 pillared CoAl layered double hydroxide nanohybrid: Fabrication and photocatalytic degradation property. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 531-539. doi: 10.11862/CJIC.20240256

    13. [13]

      Linke Zhang ,  Tao Pang ,  Lingwei Zeng ,  Feng Huang ,  Daqin Chen . Recent progress of fluoride core-shell nanocrystals: Manipulating the non-steady-state of upconversion luminescence. Chinese Journal of Structural Chemistry, 2025, 44(11): 100713-100713. doi: 10.1016/j.cjsc.2025.100713

    14. [14]

      Shuai Qiu , Jia Tang , Wan Xu , Zhiying Ma , Chao Zhang , Sheng Zhang , Chunli Li , Wei Tian , Hua Wang . Fluoride-induced sign inversion of circularly polarized luminescence of B,N-thia[8]helicene. Chinese Chemical Letters, 2026, 37(6): 111778-. doi: 10.1016/j.cclet.2025.111778

    15. [15]

      Bingyu Huang , Jipeng Fu , Tianyi Sun , Yuqi Li , Jinru Liu , Kaina Wang , Qian Xu , Wengui Yu , Hongqi Chen , Huajie Luo , Mathieu Allix , Mingxue Tang , Shiqing Xu . Nanothermometry and luminescence modulation via separated activators in core-shell-shell fluoride nanoparticles. Chinese Chemical Letters, 2026, 37(7): 111159-. doi: 10.1016/j.cclet.2025.111159

    16. [16]

      Haiyan Zhang ,  Min Yang ,  Senpei Tang ,  Xin Li ,  Youji Li . Synthesis of CoAl-LDH/CdS Material and Experimental Design for Photocatalytic CO2 Reduction. University Chemistry, 2026, 41(3): 381-389. doi: 10.12461/PKU.DXHX202504067

    17. [17]

      Shuhao FENG , Feibing XIONG , Yaqing LIN , Han SU , Xu HAN . Preparation and luminescent properties of alkaline metal doped Cd3Al2Ge3O12: Pr3+ orange phosphors. Chinese Journal of Inorganic Chemistry, 2026, 42(2): 284-296. doi: 10.11862/CJIC.20250171

    18. [18]

      Aoyun Meng ,  Zhenhua Li ,  Guoyuan Xiong ,  Zhen Li ,  Jinfeng Zhang . Rapid and stable degradation of dichlorvos on chili pepper and histamine in sardines using S-scheme Al6Si2O13/g-C3N4 nanocomposites. Chinese Journal of Structural Chemistry, 2026, 45(5): 100867-100867. doi: 10.1016/j.cjsc.2026.100867

    19. [19]

      Hongyi LI , Aimin WU , Liuyang ZHAO , Xinpeng LIU , Fengqin CHEN , Aikui LI , Hao HUANG . Effect of Y(PO3)3 double-coating modification on the electrochemical properties of Li[Ni0.8Co0.15Al0.05]O2. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1320-1328. doi: 10.11862/CJIC.20230480

    20. [20]

      Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . Effect of Interlayer Anions in Layered Double Hydroxides on the Photothermocatalytic CO2 Methanation of Derived Ni-Al2O3 Catalysts. Acta Physico-Chimica Sinica, 2025, 41(1): 100002-0. doi: 10.3866/PKU.WHXB202309002

Metrics
  • PDF Downloads(2)
  • Abstract views(983)
  • HTML views(81)

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

  1. 本站搜索
  2. 百度学术搜索
  3. 万方数据库搜索
  4. CNKI搜索
Address:Zhongguancun North First Street 2,100190 Beijing, PR China Tel: +86-010-82449177-888
Powered By info@rhhz.net

/

DownLoad:  Full-Size Img  PowerPoint
Return