Citation: SONG Li-juan, HU Yue-ting, QIN Yu-cai, YU Wen-guang, ZHANG Xiao-tong. Mechanism of effects of surface acidity on performance of adsorption desulfurization of NiY zeolites[J]. Journal of Fuel Chemistry and Technology, ;2016, 44(9): 1082-1088. shu

Mechanism of effects of surface acidity on performance of adsorption desulfurization of NiY zeolites

1.
Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Province, Liaoning ShiHua University, Fushun 113001, China
2.
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China

Corresponding author: SONG Li-juan, lsong56@263.net
Received Date: 29 February 2016
Revised Date: 12 May 2016

Fund Project: China National Petroleum Corporation Refinery Catalyst Major Projects 10-01A-01-01-01the National Natural Science Foundation of China 21076100the National Natural Science Foundation of China 21376114

Figures(8)

The adsorption behaviors of thiophene, cyclohexene and benzene, and competitive adsorption of thiophene & cyclohexene, and thiophene & benzene over NiY zeolites were studied by in situ Py-FTIR spectroscopy method. The results of single probe molecular adsorption indicate that the Lewis (L) acid sites according to Ni species are the major active centers for the thiophene adsorption, more over the Brönsted (B) acid sites of the NiY and HY are the catalytic active centers of the protonation and oligomerization of thiophene and cyclohexene, while the reaction intensity on NiY is significantly weaker than that on HY zeolite. The competitive adsorption results show that the strongly adsorbed dimeric cyclohexene on B acidic sites in NiY zeolite plays a significant competitive adsorption to thiophene adsorption behavior. The effective solutions to solve the competitive adsorption from olefins and aromatics to thiophene are to reduce the surface B acid centers of the adsorbent and to increase temperature of adsorption system.
- in situ Py-FTIR,
- NiY zeolite,
- surface acidity,
- adsorption desulfurization,
- competitive adsorption
1. [1]
  BABICH I V, MOULIJN J A. Science and technology of novel processes for deep desulfurization of oil refinery streams: A review[J]. Fuel, 2003,82(6):607-631. doi: 10.1016/S0016-2361(02)00324-1
2. [2]
  SONG C. An overview of new approaches to deep desulfurization for ultra-clean gasoline, diesel fuel and jet fuel[J]. Catal Today, 2003,86(1):211-263.
3. [3]
  HERNANDEZ-MALDONADO A J, YANG R T. Desulfurization of transportation fuels by adsorption[J]. Catal Rev, 2004,46(2):111-150. doi: 10.1081/CR-200032697
4. [4]
  HERNANDEZ-MALDONADO A J, YANG R T. Desulfurization of diesel fuels via π-complexation with Nickel (Ⅱ)-exchanged X-and Y-zeolites[J]. Ind Eng Chem Res, 2004,43:1081-1089. doi: 10.1021/ie034206v
5. [5]
  HERNANDEZ-MALDONADO A J, YANG F H, QI G S, YANG R T. Desulfurization of transportation fuels by π-complexation sorbents: Cu (Ⅰ)-, Ni (Ⅱ)-, and Zn (Ⅱ)-zeolites[J]. Appl Catal B: Environ, 2005,56(1/2):111-126.
6. [6]
  JU Xiu-Fang. Preparation of NiY and mechanisms of its selective adsorptive desulfurization[D]. Fushun: Liaoning Shihua University, 2009.
7. [7]
  SONG Li-juan, PAN Ming-xue, QIN Yu-cai, JU Xiu-fang, DUAN Lin-hai, CHEN Xiao-lu. Selective adsorption desulfurization performance and adsorptive mechanisms of NiY zeolites[J]. Chem J Chin Univ, 2011,32(3):787-792.
8. [8]
  TANG X L, SHI L. Study of the adsorption reactions of thiophene on Cu (Ⅰ)/HY-Al₂O₃ by Fourier transform infrared and temperature-programmed desorption: Adsorption, desorption, and sorbent regeneration mechanisms[J]. Langmuir, 2011,27(19):11999-12007. doi: 10.1021/la2025654
9. [9]
  GAO J J, LI H Q, ZHANG H X, LU Y Z, MENG H, LI C X. Removal mechanism of thiophenic compounds in model oil by inorganic Lewis acids[J]. Ind Eng Chem Res, 2012,51(12):4682-4691. doi: 10.1021/ie202831p
10. [10]
  SHAO X C, ZHANG X T, YU W G, WU Y Y, QIN Y C, SUN Z L, SONG L J. Effects of surface acidities of MCM-41 modified with MoO₃ on adsorptive desulfurization of gasolin[J]. Appl Sur Sci, 2012,263:1-7. doi: 10.1016/j.apsusc.2012.07.142
11. [11]
  WANG Wang-yin, PAN Ming-xue, QIN Yu-cai, WANG Ling-tao, SONG Li-juan. Effects of surface acidity on the adsorption desulfurization of Cu (Ⅰ) Y Zeolites[J]. Acta Phys Chim Sin, 2011,27(5):1176-1180.
12. [12]
  SHAO Xin-chao, DUAN Lin-hai, WU Yu-ye, QIN Yu-cai, YU Wen-guang, WANG Yuan, LI Huai-lei, SUN Zhao-lin, SONG Li-juan. Effect of surface acidity of CuO-SBA-15 on adsorptive desulfurization of fuel oils[J]. Acta Phys Chim Sin, 2012,28(6):1467-1473.
13. [13]
  WANG Hong-guo, JIANG Heng, XU Jing, SUN Zhao-lin, ZHANG Xiao-tong, ZHU He-li, SONG LI-juan. Effects of benzene and 1-octene on desulfurization by selective adsorption with Ce (Ⅳ) Y[J]. Acta Phys Chim Sin, 2008,24(9):1714-1718.
14. [14]
  ZU Yun, QIN Yu-cai, GAO Xiong-hou, MO Zhou-sheng, ZHANG Lei, ZHANG Xiao-tong, SONG Li-juan. Mechanisms of thiophene conversion over the modified Y zeolites under catalytic cracking conditions[J]. J Fuel Chem Technol, 2015,43(7):862-869.
15. [15]
  LAMBERTI C, ZECCHINA A, GROPPO E, BORDIGA S. Probing the surfaces of heterogeneous catalysts by in situ IR spectroscopy[J]. Chem Soc Rev, 2010,39(12):4951-5001. doi: 10.1039/c0cs00117a
16. [16]
  LERCHER J A, GRUNDLING C, EDER-MIRTH G. Infrared studies of the surface acidity of oxides and zeolites using adsorbed probe molecules[J]. Catal Today, 1996,27(3):353-376.
17. [17]
  COUGHLAN B, KEANE M A. A catalytic and characterization study of the surface acidity generated on the reduction of copper exchanged Y zeolites[J]. Catal Lett, 1990,5(2):113-125. doi: 10.1007/BF00763944
18. [18]
  XIN Qin, ZHANG Hui, LI Xin-sheng, LI Can. Investigation of the coadsorption of thiophene with CO or NO on Co-Mo/Al₂O₃ catalysts by infrared spectroscopy[J]. J Fuel Chem Technol, 1991,19(4):333-338.
19. [19]
  GEOBALDO F, PALOMINO G T, BORDIGA S, ZECCHINA A, AREÁN C O. Spectroscopic study in the UV-Vis, near and mid IR of cationic species formed by interaction of thiophene, dithiophene and terthiophene with the zeolite HY[J]. Phys Chem Chem Phys, 1999,1(4):561-569. doi: 10.1039/a807353h
20. [20]
  DE ANGELIS B A, APPLERTO G J. Infrared spectroscopic study of thiophene adsorbed on zeolites[J]. J Colloid Interf Sci, 1975,53(1):14-19. doi: 10.1016/0021-9797(75)90029-6
21. [21]
  YANG S, KONDO J N, DOMEN K. Formation of alkenyl carbenium ions by adsorption of cyclic precursors on zeolites[J]. Catal today, 2002,73(1):113-125.
22. [22]
  KONDO J N, SHAO L, WAKABAYASHI F, DOMEN K. Doublebond migration of an olefin without protonated species on H (D) form zeolites[J]. J Phys Chem B, 1997,101(45):9314-9320. doi: 10.1021/jp971812t
23. [23]
  KONDO J N, WAKABAYASHI F, DOMEN K. IR study of adsorption of olefins on deuterated ZSM-5[J]. J Phys Chem B, 1998,102(12):2259-2262. doi: 10.1021/jp9800416
24. [24]
  ANGELL C L, HOWELL M V. Infrared spectroscopic investigations of zeolites and adsorbed molecules: III Aromatic hydrocarbons[J]. J Colloid Interf Sci, 1968,28(2):279-287. doi: 10.1016/0021-9797(68)90131-8
1. [1]
  Jiali CHEN , Guoxiang ZHAO , Yayu YAN , Wanting XIA , Qiaohong LI , Jian ZHANG . Machine learning exploring the adsorption of electronic gases on zeolite molecular sieves. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 155-164. doi: 10.11862/CJIC.20240408
2. [2]
  Yang Wang , Yunpeng Fu , Xiaoji Liu , Guotao Zhang , Guobin Li , Wanqiang Liu , Jinglun Wang . Structural Analysis of Nitrile Solutions Based on Infrared Spectroscopy Probes. University Chemistry, 2025, 40(4): 367-374. doi: 10.12461/PKU.DXHX202406113
3. [3]
  Yuhao SUN , Qingzhe DONG , Lei ZHAO , Xiaodan JIANG , Hailing GUO , Xianglong MENG , Yongmei GUO . Synthesis and antibacterial properties of silver-loaded sod-based zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 761-770. doi: 10.11862/CJIC.20230169
4. [4]
  Pei Li , Yuenan Zheng , Zhankai Liu , An-Hui Lu . Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(4): 100034-. doi: 10.3866/PKU.WHXB202406012
5. [5]
  Yiping HUANG , Liqin TANG , Yufan JI , Cheng CHEN , Shuangtao LI , Jingjing HUANG , Xuechao GAO , Xuehong GU . Hollow fiber NaA zeolite membrane for deep dehydration of ethanol solvent by vapor permeation. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 225-234. doi: 10.11862/CJIC.20240224
6. [6]
  Xiaosong PU , Hangkai WU , Taohong LI , Huijuan LI , Shouqing LIU , Yuanbo HUANG , Xuemei LI . Adsorption performance and removal mechanism of Cd(Ⅱ) in water by magnesium modified carbon foam. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1537-1548. doi: 10.11862/CJIC.20240030
7. [7]
  Jingke LIU , Jia CHEN , Yingchao HAN . Nano hydroxyapatite stable suspension system: Preparation and cobalt adsorption performance. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1763-1774. doi: 10.11862/CJIC.20240060
8. [8]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
9. [9]
  Fang Niu , Rong Li , Qiaolan Zhang . Analysis of Gas-Solid Adsorption Behavior in Resistive Gas Sensing Process. University Chemistry, 2024, 39(8): 142-148. doi: 10.3866/PKU.DXHX202311102
10. [10]
  Fei Xie , Chengcheng Yuan , Haiyan Tan , Alireza Z. Moshfegh , Bicheng Zhu , Jiaguo Yu . d带中心调控过渡金属单原子负载COF吸附O₂的理论计算研究. Acta Physico-Chimica Sinica, 2024, 40(11): 2407013-. doi: 10.3866/PKU.WHXB202407013
11. [11]
  Xueqi Yang , Juntao Zhao , Jiawei Ye , Desen Zhou , Tingmin Di , Jun Zhang . 调节NNU-55(Fe)的d带中心以增强CO₂吸附和光催化活性. Acta Physico-Chimica Sinica, 2025, 41(7): 100074-. doi: 10.1016/j.actphy.2025.100074
12. [12]
  Yufang GAO , Nan HOU , Yaning LIANG , Ning LI , Yanting ZHANG , Zelong LI , Xiaofeng LI . Nano-thin layer MCM-22 zeolite: Synthesis and catalytic properties of trimethylbenzene isomerization reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1079-1087. doi: 10.11862/CJIC.20240036
13. [13]
  Shanghua Li , Malin Li , Xiwen Chi , Xin Yin , Zhaodi Luo , Jihong Yu . 基于高离子迁移动力学的取向ZnQ分子筛保护层实现高稳定水系锌金属负极的构筑. Acta Physico-Chimica Sinica, 2025, 41(1): 2309003-. doi: 10.3866/PKU.WHXB202309003
14. [14]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
15. [15]
  Youlin SI , Shuquan SUN , Junsong YANG , Zijun BIE , Yan CHEN , Li LUO . Synthesis and adsorption properties of Zn(Ⅱ) metal-organic framework based on 3, 3', 5, 5'-tetraimidazolyl biphenyl ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1755-1762. doi: 10.11862/CJIC.20240061
16. [16]
  Qianqian Zhong , Yucui Hao , Guotao Yu , Lijuan Zhao , Jingfu Wang , Jian Liu , Xiaohua Ren . Comprehensive Experimental Design for the Preparation of the Magnetic Adsorbent Based on Enteromorpha Prolifera and Its Utilization in the Purification of Heavy Metal Ions Wastewater. University Chemistry, 2024, 39(8): 184-190. doi: 10.3866/PKU.DXHX202312013
17. [17]
  Xinyu Yin , Haiyang Shi , Yu Wang , Xuefei Wang , Ping Wang , Huogen Yu . Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production. Acta Physico-Chimica Sinica, 2024, 40(10): 2312007-. doi: 10.3866/PKU.WHXB202312007
18. [18]
  Shasha Ma , Zujin Yang , Jianyong Zhang . Facile Synthesis of FeBTC Metal-Organic Gel and Its Adsorption of Cr₂O₇²⁻: A Physical Chemistry Innovation Experiment. University Chemistry, 2024, 39(8): 314-323. doi: 10.3866/PKU.DXHX202401008
19. [19]
  Hui Wang , Abdelkader Labidi , Menghan Ren , Feroz Shaik , Chuanyi Wang . 微观结构调控的g-C₃N₄在光催化NO转化中的最新进展：吸附/活化位点的关键作用. Acta Physico-Chimica Sinica, 2025, 41(5): 100039-. doi: 10.1016/j.actphy.2024.100039
20. [20]
  Zhuomin Zhang , Hanbing Huang , Liangqiu Lin , Jingsong Liu , Gongke Li . Course Construction of Instrumental Analysis Experiment: Surface-Enhanced Raman Spectroscopy for Rapid Detection of Edible Pigments. University Chemistry, 2024, 39(2): 133-139. doi: 10.3866/PKU.DXHX202308034

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(778)
HTML views(57)

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