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

GUO Xing-mei ^1,*,, ,
SONG Mao-ning ^1,2 ,
ZHAO Xu ¹ ,
ZHAO Liang-fu ^2,*,,

1.
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, China
2.
Laboratory of Applied Catalysis and Green Chemical Engineering, Institute of Coal Chemistry Chinese Academy of Sciences, Taiyuan 030001, China

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.
- hydrodesulfurization,
- hydrodenitrogenation,
- fluoride,
- NiWF/γ-Al₂O₃,
- coal tar
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.
1. [1]
  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
2. [2]
  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
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]
  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
5. [5]
  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
6. [6]
  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[Ni_0.8Co_0.15Al_0.05]O₂. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1320-1328. doi: 10.11862/CJIC.20230480
7. [7]
  Lina Guo , Ruizhe Li , Chuang Sun , Xiaoli Luo , Yiqiu Shi , Hong Yuan , Shuxin Ouyang , Tierui Zhang . 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响. Acta Physico-Chimica Sinica, 2025, 41(1): 2309002-. doi: 10.3866/PKU.WHXB202309002
8. [8]
  Junhua Wang , Xin Lian , Xichuan Cao , Qiao Zhao , Baiyan Li , Xian-He Bu . Dual polarization strategy to enhance CH₄ uptake in covalent organic frameworks for coal-bed methane purification. Chinese Chemical Letters, 2024, 35(8): 109180-. doi: 10.1016/j.cclet.2023.109180
9. [9]
  Juan Guo , Mingyuan Fang , Qingsong Liu , Xiao Ren , Yongqiang Qiao , Mingju Chao , Erjun Liang , Qilong Gao . Zero thermal expansion in Cs₂W₃O₁₀. Chinese Chemical Letters, 2024, 35(7): 108957-. doi: 10.1016/j.cclet.2023.108957
10. [10]
  Renshu Huang , Jinli Chen , Xingfa Chen , Tianqi Yu , Huyi Yu , Kaien Li , Bin Li , Shibin Yin . Synergized oxygen vacancies with Mn2O3@CeO2 heterojunction as high current density catalysts for Li–O2 batteries. Chinese Journal of Structural Chemistry, 2023, 42(11): 100171-100171. doi: 10.1016/j.cjsc.2023.100171
11. [11]
  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
12. [12]
  Haojie Duan , Hejingying Niu , Lina Gan , Xiaodi Duan , Shuo Shi , Li Li . Reinterpret the heterogeneous reaction of α-Fe₂O₃ and NO₂ with 2D-COS: The role of SDS, UV and SO₂. Chinese Chemical Letters, 2024, 35(6): 109038-. doi: 10.1016/j.cclet.2023.109038
13. [13]
  Cailiang Yue , Nan Sun , Yixing Qiu , Linlin Zhu , Zhiling Du , Fuqiang Liu . A direct Z-scheme 0D α-Fe₂O₃/TiO₂ heterojunction for enhanced photo-Fenton activity with low H₂O₂ consumption. Chinese Chemical Letters, 2024, 35(12): 109698-. doi: 10.1016/j.cclet.2024.109698
14. [14]
  Lina Wang , Hairu Wang , Qian Bu , Qiong Mei , Junbo Zhong , Bo Bai , Qizhao Wang . Al-O bridged NiFeO_x/BiVO₄ photoanode for exceptional photoelectrochemical water splitting. Chinese Chemical Letters, 2025, 36(4): 110139-. doi: 10.1016/j.cclet.2024.110139
15. [15]
  Dong-Xue Jiao , Hui-Li Zhang , Chao He , Si-Yu Chen , Ke Wang , Xiao-Han Zhang , Li Wei , Qi Wei . Layered (C5H6ON)2[Sb2O(C2O4)3] with a large birefringence derived from the uniform arrangement of π-conjugated units. Chinese Journal of Structural Chemistry, 2024, 43(6): 100304-100304. doi: 10.1016/j.cjsc.2024.100304
16. [16]
  Fei ZHOU , Xiaolin JIA . Co₃O₄/TiO₂ composite photocatalyst: Preparation and synergistic degradation performance of toluene. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2232-2240. doi: 10.11862/CJIC.20240236
17. [17]
  Ran Yu , Chen Hu , Ruili Guo , Ruonan Liu , Lixing Xia , Cenyu Yang , Jianglan Shui . 杂多酸H₃PW₁₂O₄₀高效催化MgH₂储氢. Acta Physico-Chimica Sinica, 2025, 41(1): 2308032-. doi: 10.3866/PKU.WHXB202308032
18. [18]
  Honglin Gao , Chunlin Yuan , Hongyu Chen , Aiyi Dong , Pan Gao , Guangjin Hou . Surface gallium hydride on Ga2O3 polymorphs: A comparative solid-state NMR study. Chinese Journal of Structural Chemistry, 2025, 44(4): 100561-100561. doi: 10.1016/j.cjsc.2025.100561
19. [19]
  Shiyi WANG , Chaolong CHEN , Xiangjian KONG , Lansun ZHENG , Lasheng LONG . Polynuclear lanthanide compound [Ce₄^ⅢCe₆^Ⅳ(μ₃-O)₄(μ₄-O)₄(acac)₁₄(CH₃O)₆]·2CH₃OH for the hydroboration of amides to amine. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 88-96. doi: 10.11862/CJIC.20240342
20. [20]
  Xinpeng LIU , Liuyang ZHAO , Hongyi LI , Yatu CHEN , Aimin WU , Aikui LI , Hao HUANG . Ga₂O₃ coated modification and electrochemical performance of Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ cathode material. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1105-1113. doi: 10.11862/CJIC.20230488

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(378)
HTML views(33)

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

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

Metrics

通讯作者: 陈斌, bchen63@163.com

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