Citation: LI Xiu-ping, ZHAO Rong-xiang, XING Peng-fei. Preparation of NiWO₄/g-C₃N₄ and its ultra-deep desulfurization properties in ionic liquid[J]. Journal of Fuel Chemistry and Technology, ;2017, 45(11): 1340-1348. shu

Preparation of NiWO₄/g-C₃N₄ and its ultra-deep desulfurization properties in ionic liquid

1.
School of chemistry and Materials Science, College of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, China
2.
School of Petrochemical Engineering, College of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning University of Petroleum & Chemical Technology, Fushun 113001, China

Corresponding author: ZHAO Rong-xiang, zylhzrx@126.com
Received Date: 12 April 2017
Revised Date: 27 July 2017

Figures(12)

The NiWO₄ nanoparticles were synthesized by hydrothermal method. The supported catalysts NiWO₄/g-C₃N₄ were prepared by a simple mixing-calcination method. XRD, FT-IR, EDS, SEM, BET and XPS were used to characterize the morphology and structure of NiWO₄/g-C₃N₄. The prepared NiWO₄/g-C₃N₄ was used as catalyst, hydrogen peroxide as oxidant, 1-butyl-3-methylimidazolium tetrafluoroborate ionic liquid ([BMIM]BF₄) as extractant for oxidative desulfurization. The effects of catalyst loading, the amount of hydrogen peroxide, ionic liquid and catalyst, reaction temperature, reaction time, and different sulfur compounds on desulfurization efficiency were studied. The desulfurization rate can reach 97.35% at the optimum reaction conditions:5 mL of model oil, 0.2 mL of hydrogen peroxide, 1.0 mL of [BMIM] BF₄, 0.03 g of NiWO₄/g-C₃N₄, 80 ℃ of reaction temperature and 140 min of reaction time. The results showed that NiWO₄/g-C₃N₄ had good catalytic stability, and the catalytic activity was not significantly reduced after 5 repeated reactions.
- NiWO₄/g-C₃N₄,
- oxidative desulfurization,
- dibenzothiophene,
- ionic liquid
1. [1]
  LORENÇON E, ALVES D C B, KRAMBROCK K, ERICK S Á, RESENDE R R, FERLAUTO A S, LAGO R M. Oxidative desulfurization of dibenzothiophene over titanate nanotubes[J]. Fuel, 2014,132:53-61. doi: 10.1016/j.fuel.2014.04.020
2. [2]
  YAN X M, SU G S, XIONG L. Oxidative desulfurization of diesel oil over Ag-modified mesoporous HPW/SiO₂catalyst[J]. J Fuel Chem Technol, 2009,7(3):318-323.
3. [3]
  BAZYARI A, KHODADADI A A, MAMAGHANI A H, BEHESHTIAN J, THOMPSON L T, MORTAZAVI Y. Microporous titania-silica nanocomposite catalyst-adsorbent for ultra-deep oxidative desulfurization[J]. Appl Catal B:Environ, 2016,180:65-77. doi: 10.1016/j.apcatb.2015.06.011
4. [4]
  STANISLAUS A, MARAFI A, RANA M S. Recent advances in the science and technology of ultra low sulfur diesel (ULSD) production[J]. Catal Today, 2010,153(1):1-68.
5. [5]
  JIANG B, YANG H, ZHANG L, ZHANG R Y, SUN Y L, HUANG Y. Efficient oxidative desulfurization of diesel fuel using amide-based ionic liquids[J]. Chem Eng J, 2016,283:89-96. doi: 10.1016/j.cej.2015.07.070
6. [6]
  LI C, LI D, ZOU S, LI Z, YIN J M, WANG A L, CUI Y N, YAO Z L, ZHAO Q. Extraction desulfurization process of fuels with ammonium-based deep eutectic solvents[J]. Green Chem, 2013,15(10):2793-2799. doi: 10.1039/c3gc41067f
7. [7]
  HUANG L, WANG G, QIN Z, DONG M, DU M X, GE H, LI X K, ZHAO Y D, ZHANG J, HU T D, WANG J G. In situ XAS study on the mechanism of reactive adsorption desulfurization of oil product over Ni/ZnO[J]. Appl Catal B:Environ, 2011,106(1):26-38.
8. [8]
  MARGETA D, SERTIĆ-BIONDA K, FOGLAR L. Ultrasound assisted oxidative desulfurization of model diesel fuel[J]. Appl Acoust, 2016,103(2):202-206.
9. [9]
  WU L, SITAMRAJU S, XIAO J, LIU B, LI Z, JANIK M J, SONG C S. Effect of liquid-phase O₃ oxidation of activated carbon on the adsorption of thiophene[J]. Chem Eng J, 2014,242:211-219. doi: 10.1016/j.cej.2013.12.077
10. [10]
  BAKAR W A W A, ALI R, KADIR A A A, MOKHTAR W N A W. Effect of transition metal oxides catalysts on oxidative desulfurization of model diesel[J]. Fuel Process Technol, 2012,101:78-84. doi: 10.1016/j.fuproc.2012.04.004
11. [11]
  GARCÍA-GUTIÉRREZ J L, LAREDO G C, GARCÍA-GUTIÉRREZ P, JIMÉNEZ-CRUZ F. Oxidative desulfurization of diesel using promising heterogeneous tungsten catalysts and hydrogen peroxide[J]. Fuel, 2014,138:118-125. doi: 10.1016/j.fuel.2014.07.049
12. [12]
  SHI X Y, SUN M, FAN J, WANG P M, MA W J, WEI J F. Deep oxidative desulfurization of benzothiophene and dibenzothiophene with a peroxophosphotungstate-ionic liquid brush assembly[J]. Appl Organomet Chem, 2015,29(9):633-637. doi: 10.1002/aoc.v29.9
13. [13]
  ZHU W, WU P, YANG L, CHANG Y H, CHAO Y H, LI H M, JIANG Y Q, JIANG W, XUN S H. Pyridinium-based temperature-responsive magnetic ionic liquid for oxidative desulfurization of fuels[J]. Chem Eng J, 2013,229(4):250-256.
14. [14]
  WAN M W, YEN T F. Enhance efficiency of tetraoctylammonium fluoride applied to ultrasound-assisted oxidative desulfurization (UAOD) process[J]. Appl Catal A:Gen, 2007,319(1):237-245.
15. [15]
  ZHANG M, ZHU W, XUN S, LI H M, GU Q Q, ZHAO Z, WANG Q. Deep oxidative desulfurization of dibenzothiophene with POM-based hybrid materials in ionic liquids[J]. Chem Eng J, 2013,220(6):328-336.
16. [16]
  SHAN J H, CHEN L, SUN L B, LIU X Q. Adsorptive removal of thiophene by Cu-modified mesoporous silica MCM-48 derived from direct synthesis[J]. Energy Fuels, 2011,25(7):3093-3099. doi: 10.1021/ef200472j
17. [17]
  ZHU W, XU Y, LI H, DAI B L, XU H, WANG CHAO, CHAO Y H, LIU H. Photocatalytic oxidative desulfurization of dibenzothiophene catalyzed by amorphous TiO₂, in ionic liquid[J]. Korean J Chem Eng, 2014,31(2):211-217. doi: 10.1007/s11814-013-0224-3
18. [18]
  SUN B, ZHAO W, WEI L, LI H W, CHEN P. Enhanced resistive switching effect upon illumination in self-assembled NiWO₄ nano-nests[J]. Chem Commun, 2014,50(86):13142-5. doi: 10.1039/C4CC05784H
19. [19]
  LIU D, GUI J, PENG X, YANG S, SUN Z L. Deep oxidative desulfurization of real diesel catalyzed by Na₂WO₄, in ionic liquid[J]. Energ Source Part A, 2013,35(1):1-8. doi: 10.1080/15567036.2010.503230
20. [20]
  XING Peng-fei, SHI Wei-wei, LI Xiu-ping, ZHAO Rong-xiang. Preparation of NiWO₄ catalyst and its application in the oxidationde sulfurization of model oil[J]. Acta Pet Sin (Pet Process Sect), 2017,33(2):334-342.
21. [21]
  XING P F, ZHAO R X, LI X P, GAO X H. Preparation of CoWO₄/g-C₃N₄and its ultra-deep desulfurization property[J]. Aust J Chem, 2017,70(3):271-279. doi: 10.1071/CH16320
22. [22]
  WANG X C, MAEDA K, THOMAS A, TAKANABE K, XIN G, CARLSSON J M, DOMEN K, ANTONIETTI M. A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J]. Nat Mater, 2009,8(1):76-80. doi: 10.1038/nmat2317
23. [23]
  JING D, LIU Q, ZHANG Z, LIU X, ZHAO J Q, CHENG S B, ZONG B N, DAI W L. Carbon nitride nanosheets decorated with WO₃, nanorods:Ultrasonic-assisted facile synthesis and catalytic application in the green manufacture of dialdehydes[J]. Appl Catal B:Environ, 2015,165:511-518. doi: 10.1016/j.apcatb.2014.10.037
24. [24]
  YAN H, CHEN Y, XU S. Synthesis of graphitic carbon nitride by directly heating sulfuric acid treated melamine for enhanced photocatalytic H₂ production from water under visible light[J]. Int J Hydrogen Energy, 2012,37(1):125-133. doi: 10.1016/j.ijhydene.2011.09.072
25. [25]
  SONG Ji-mei, LIU Xiao-ling, DONG Na, LI Wen-hui, SI Wei, YANG Jie. Preparation and properties of Mesoporous NiWO₄ nanospheres[J]. J Anhui Univ(Nat Sci), 2016,40(1):73-79.
26. [26]
  GREEN S V, KUZMIN A, PURANS J, GRANQVIST C G, NIKLASSON G A. Structure and composition of sputter-deposited nickel-tungsten oxide films[J]. Thin Solid Films, 2011,519(7):2062-2066. doi: 10.1016/j.tsf.2010.10.033
27. [27]
  GU Y, CHEN L, SHI L, MA J H, YANG Z, QIAN Y T. Synthesis of C₃N₄ and graphite by reacting cyanuric chloride with calcium cyanamide[J]. Carbon, 2003,41(13):2674-2676. doi: 10.1016/S0008-6223(03)00357-9
28. [28]
  TALAPANENI S N, ANANDAN S, MANE G P, ANAND C, DHAWALE D S, VARGHESE S, MANO A, MORI T, VINU A. Facile synthesis and basic catalytic application of 3D mesoporous carbon nitride with a controllable bimodal distribution[J]. J Mater Chem, 2012,22(19):9831-9840. doi: 10.1039/c2jm30229b
29. [29]
  DONG F, WU L, SUN Y, FU M, WU Z B, LEE S C. Efficient synthesis of polymeric g-C₃N₄ layered materials as novel efficient visible light driven photocatalysts[J]. J Mater Chem, 2011,21(39):15171-15174. doi: 10.1039/c1jm12844b
30. [30]
  NG K T, HERCULES D M. Studies of nickel-tungsten-alumina catalysts by X-ray photoelectron spectroscopy[J]. J Phys Chem, 1976,80(19):2094-2102. doi: 10.1021/j100560a009
31. [31]
  MOULDER J F, STICKLE W F, SOBOL P E, BOMBEN K D, CHASTAIN J. Handbook of X-ray photoelectron spectroscop[J]. Chem Phys Lett, 1979,220(1):7-10.
32. [32]
  MANCHEVA M N, IORDANOVA R S, KLISSURSKI DIMITAR G, TYULIEV G T, KUNEV B N. Direct mechanochemical synthesis of nanocrystalline NiWO₄[J]. J Phys Chem C, 2007,111(3):1101-1104. doi: 10.1021/jp065071k
33. [33]
  ZHANG J, ZHU W, LI H, JIANG W, JIANG Y Q, HUANG W L, YAN Y S. Deep oxidative desulfurization of fuels by Fenton-like reagent in ionic liquids[J]. Green Chem, 2009,11(11):1801-1807. doi: 10.1039/b914130h
34. [34]
  LI L, ZHANG J, SHEN C, WANG Y J, LUO G S. Oxidative desulfurization of model fuels with pure nano-TiO₂ as catalyst directly without UV irradiation[J]. Fuel, 2015,167:9-16.
35. [35]
  LÜ H, REN W, WANG H, WANG Y, CHEN W, SUO Z H. Deep desulfurization of diesel by ionic liquid extraction coupled with catalytic oxidation using an Anderson-type catalyst[(C₄H₉)₄ N]₄NiMo₆O₂₄H₆[J]. Appl Catal A:Gen, 2013,453:376-382. doi: 10.1016/j.apcata.2012.12.047
36. [36]
  LÜ H, DENG C, REN W, YANG X. Oxidative desulfurization of model diesel using[(C₄H₉)₄N]₆Mo₇O₂₄, as a catalyst in ionic liquids[J]. Fuel Process Technol, 2014,119(1):87-91.
37. [37]
  LI Yu-hui, FENG Li-juan, WANG Jing-gang, ZHOU Xuan, CHENG Bin-bin, WANG Xiao-yan, LI Chun-hu. Catalytic oxidative desulfurization of model oil by MoO₃/mesoporous Al₂O₃[J]. Chem J Chin Univ, 2011,32(3):778-782.
38. [38]
  SU Jian-xun, AI Dong, ZHAO Rong-xiang, LI Xiu-ping. Study of the preparation of CuWO₄/C composite and it's application in oxidative desulfurization of model oil[J]. J Fuel Chem Technol, 2015,43(12):1476-1481. doi: 10.3969/j.issn.0253-2409.2015.12.011
39. [39]
  YI N, DONG Y, LU B, DONG H F, ZHANG X P. Fast oxidative desulfurization of fuel oil using dialkylpyridinium tetrachloroferrates ionic liquids[J]. Fuel, 2013,103(1):997-1002.
40. [40]
  OTSUKI S, NONAKA T, TAKASHIMA N, QIAN W H, ISHIHARA A, IMAI T, KABE T. Oxidative desulfurization of light gas oil and vacuum gas oil by oxidation and solvent extraction[J]. Energy Fuels, 2000,14(6):1232-1239. doi: 10.1021/ef000096i
41. [41]
  LÜ H Y, GAO J B, JIANG Z X, FEI J, YANG Y X, WANG G, LI C. Ultra-deep desulfurization of diesel by selective oxidation with[C₁₈H₃₇N(CH₃)₃]₄[H₂NaPW₁₀O₃₆] catalyst assembled in emulsion droplets[J]. J Catal, 2006,239:369-375. doi: 10.1016/j.jcat.2006.01.025
42. [42]
  LI Jia-hui, HU Jia, ZHAO Rong-xiang, LI Xiu-ping. Prepartion of amino acid functionalized heteropolyacid salt and its catalytic performance for oxidation desulfurization of model oil[J]. J Fuel Chem Technol, 2014,42(11):1394-1399. doi: 10.3969/j.issn.0253-2409.2014.11.018
43. [43]
  ABDALLA Z E A, LI B, TUFAIL A. Preparation of phosphate promoted Na₂WO₄/Al₂O₃ catalyst and its application for oxidative desulfurization[J]. J Ind Eng Chem, 2009,15(6):780-783. doi: 10.1016/j.jiec.2009.09.026
44. [44]
  USUI Y, SATO K A. Green method of adipic acid synthesis:organic solvent-and halide-free oxidation of cycloalkanones with 30% hydrogen peroxide[J]. Green Chem, 2003,5(4):373-375. doi: 10.1039/b305847f
45. [45]
  EDE S R, KUNDU S. Microwave synthesis of SnWO₄ nanoassemblies on DNA scaffold:A novel material for high performance supercapacitor and as catalyst for butanol oxidation[J]. ACS Sustainable Chem Eng, 2015,3(9):2321-2336. doi: 10.1021/acssuschemeng.5b00627
1. [1]
  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
2. [2]
  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
3. [3]
  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
4. [4]
  Xuejiao Wang , Suiying Dong , Kezhen Qi , Vadim Popkov , Xianglin Xiang . Photocatalytic CO₂ Reduction by Modified g-C₃N₄. Acta Physico-Chimica Sinica, 2024, 40(12): 2408005-. doi: 10.3866/PKU.WHXB202408005
5. [5]
  Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A. C. Carabineiro , Kangle Lv . Effect of precursors on the structure and photocatalytic performance of g-C3N4 for NO oxidation and CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(11): 100416-100416. doi: 10.1016/j.cjsc.2024.100416
6. [6]
  Zhi Zhu , Xiaohan Xing , Qi Qi , Wenjing Shen , Hongyue Wu , Dongyi Li , Binrong Li , Jialin Liang , Xu Tang , Jun Zhao , Hongping Li , Pengwei Huo . Fabrication of graphene modified CeO2/g-C3N4 heterostructures for photocatalytic degradation of organic pollutants. Chinese Journal of Structural Chemistry, 2023, 42(12): 100194-100194. doi: 10.1016/j.cjsc.2023.100194
7. [7]
  Guangming YIN , Huaiyao WANG , Jianhua ZHENG , Xinyue DONG , Jian LI , Yi'nan SUN , Yiming GAO , Bingbing WANG . Preparation and photocatalytic degradation performance of Ag/protonated g-C₃N₄ nanorod materials. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1491-1500. doi: 10.11862/CJIC.20240086
8. [8]
  Qingwang LIU . MoS₂/Ag/g-C₃N₄ Z-scheme heterojunction: Preparation and photocatalytic performance. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 821-832. doi: 10.11862/CJIC.20240148
9. [9]
  Wenjun Zheng . Application in Inorganic Synthesis of Ionic Liquids. University Chemistry, 2024, 39(8): 163-168. doi: 10.3866/PKU.DXHX202401020
10. [10]
  Min WANG , Dehua XIN , Yaning SHI , Wenyao ZHU , Yuanqun ZHANG , Wei ZHANG . Construction and full-spectrum catalytic performance of multilevel Ag/Bi/nitrogen vacancy g-C₃N₄/Ti₃C₂T_x Schottky junction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1123-1134. doi: 10.11862/CJIC.20230477
11. [11]
  Jianyu Qin , Yuejiao An , Yanfeng Zhang . In Situ Assembled ZnWO₄/g-C₃N₄ S-Scheme Heterojunction with Nitrogen Defect for CO₂ Photoreduction. Acta Physico-Chimica Sinica, 2024, 40(12): 2408002-. doi: 10.3866/PKU.WHXB202408002
12. [12]
  Yingqi BAI , Hua ZHAO , Huipeng LI , Xinran REN , Jun LI . Perovskite LaCoO₃/g-C₃N₄ heterojunction: Construction and photocatalytic degradation properties. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 480-490. doi: 10.11862/CJIC.20240259
13. [13]
  Xin Jiang , Han Jiang , Yimin Tang , Huizhu Zhang , Libin Yang , Xiuwen Wang , Bing Zhao . g-C₃N₄/TiO_2-X heterojunction with high-efficiency carrier separation and multiple charge transfer paths for ultrasensitive SERS sensing. Chinese Chemical Letters, 2024, 35(10): 109415-. doi: 10.1016/j.cclet.2023.109415
14. [14]
  Wei Zhong , Dan Zheng , Yuanxin Ou , Aiyun Meng , Yaorong Su . K原子掺杂高度面间结晶的g-C₃N₄光催化剂及其高效H₂O₂光合成. Acta Physico-Chimica Sinica, 2024, 40(11): 2406005-. doi: 10.3866/PKU.WHXB202406005
15. [15]
  Guoqiang Chen , Zixuan Zheng , Wei Zhong , Guohong Wang , Xinhe Wu . 熔融中间体运输导向合成富氨基g-C₃N₄纳米片用于高效光催化产H₂O₂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406021-. doi: 10.3866/PKU.WHXB202406021
16. [16]
  Chunyan Yang , Qiuyu Rong , Fengyin Shi , Menghan Cao , Guie Li , Yanjun Xin , Wen Zhang , Guangshan Zhang . Rationally designed S-scheme heterojunction of BiOCl/g-C₃N₄ for photodegradation of sulfamerazine: Mechanism insights, degradation pathways and DFT calculation. Chinese Chemical Letters, 2024, 35(12): 109767-. doi: 10.1016/j.cclet.2024.109767
17. [17]
  Guixu Pan , Zhiling Xia , Ning Wang , Hejia Sun , Zhaoqi Guo , Yunfeng Li , Xin Li . Preparation of high-efficient donor-π-acceptor system with crystalline g-C3N4 as charge transfer module for enhanced photocatalytic hydrogen evolution. Chinese Journal of Structural Chemistry, 2024, 43(12): 100463-100463. doi: 10.1016/j.cjsc.2024.100463
18. [18]
  Hui Wang , Haodong Ji , Dandan Zhang , Xudong Yang , Hanchun Chen , Chunqian Jiang , Weiliang Sun , Jun Duan , Wen Liu . Solar-light-driven photocatalytic degradation and detoxification of ciprofloxacin using sodium niobate nanocubes decorated g-C₃N₄ with built-in electric field. Chinese Chemical Letters, 2025, 36(5): 110200-. doi: 10.1016/j.cclet.2024.110200
19. [19]
  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
20. [20]
  Kexin Dong , Chuqi Shen , Ruyu Yan , Yanping Liu , Chunqiang Zhuang , Shijie Li . Integration of Plasmonic Effect and S-Scheme Heterojunction into Ag/Ag₃PO₄/C₃N₅ Photocatalyst for Boosted Photocatalytic Levofloxacin Degradation. Acta Physico-Chimica Sinica, 2024, 40(10): 2310013-. doi: 10.3866/PKU.WHXB202310013

Get Citation

PDF

XML

Metrics

PDF Downloads(16)
Abstract views(2924)
HTML views(1218)

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

Preparation of NiWO4/g-C3N4 and its ultra-deep desulfurization properties in ionic liquid

Metrics

通讯作者: 陈斌, bchen63@163.com

Preparation of NiWO₄/g-C₃N₄ and its ultra-deep desulfurization properties in ionic liquid