Citation: TIAN Ren, WANG Shi-yao, LIAN Chen-shuai, WU Xu, AN Xia, XIE Xian-mei. Synthesis of the hierarchical Fe-substituted porous HBeta zeolite and the exploration of its catalytic performance[J]. Journal of Fuel Chemistry and Technology, ;2019, 47(12): 1476-1485. shu

Synthesis of the hierarchical Fe-substituted porous HBeta zeolite and the exploration of its catalytic performance

  • Corresponding author: XIE Xian-mei, xxmtougao@sina.com
  • Received Date: 9 September 2019
    Revised Date: 25 October 2019

    Fund Project: the National Natural Science Foundation of China 51541210The project was supported by the National Natural Science Foundation of China (51541210), Natural Science Foundation of Shanxi Province(201701D121042)Natural Science Foundation of Shanxi Province 201701D121042

Figures(14)

  • A series of hierarchical isomorphically Fe-substituted porous beta zeolites (BEAs) was synthesised in a one-step process via soft-template approach (nFe-HBeta, n=Fe/Al) and a series of Ni-based catalysts (10Ni/nFe-HBeta) was prepared by equal volume impregnation. The results showed that the nFe-HBeta zeolites possessed a sheet-like structure with a high crystallinity and numerous porous channels. The introduction of the heterogeneous iron atoms could reduce the degree of order of the mesoporous phase and decrease the size of the zeolite particles and the number of moderate and strong acidic sites. For the 10Ni/nFe-HBeta catalyst, a synergistic effect existed between the framework iron and NiO species, which could enhance the interaction between the active Ni and HBeta support, increase the dispersion of the active metal Ni, and reduce the NiO particle size. In the ethanol steam reforming (ESR) reaction, Fe introduction could inhibit the ethanol dehydration reaction through the shielding of acidic sites and could promote the steam reforming reaction of CO and CH4, effectively improving the H2 selectivity. Among the Fe-containing catalysts, 10Ni/0.15Fe-HBeta showed a H2 selectivity of up to 72.15% and an ethanol conversion rate of 99.6% at 500 ℃, while the amount of coke deposition was only 4.3% after a 12 h reaction.
  • 加载中
    1. [1]

      LI D, ZENG L, LI X Y, WANG X, MA H Y, ASSABUMRUNGRAT S, GONG J L. Ceria-promoted Ni/SBA-15 catalysts for ethanol steam reforming with enhanced activity and resistance to deactivation[J]. Appl Catal B:Environ, 2015,176:532-541.  

    2. [2]

      VIZCAÍNO A J, CARRERO A, CALLES J A. Comparison of ethanol steam reforming using Co and Ni catalysts supported on SBA-15 modified by Ca and Mg[J]. Fuel Process Technol, 2016,146:99-109. doi: 10.1016/j.fuproc.2016.02.020

    3. [3]

      LI Bao-ru, YIN Xue-mei, WU Xu, AN Xia, XIE Xian-mei. Study on hydrogen production by steam reforming of ethanol over Ni-Fe/montmorillonite catalyst[J]. J Fuel Chem Technol, 2016,44(8):993-1000. doi: 10.3969/j.issn.0253-2409.2016.08.014 

    4. [4]

      GOICOECHEA S, KRALEVA E, SOKOLOV S, SCHNEIDER M, POHL M, KOCKMANN N, EHRICH H. Support effect on structure and performance of Co and Ni catalysts for steam reforming of acetic acid[J]. Appl Catal A:Gen, 2016,514:182-191. doi: 10.1016/j.apcata.2015.12.025

    5. [5]

      BILAL M, JACKSON S D. Ethanol steam reforming over Pt/Al2O3 and Rh/Al2O3 catalysts:The effect of impurities on selectivity and catalyst deactivation[J]. Appl Catal A:Gen, 2017,529:98-107. doi: 10.1016/j.apcata.2016.10.020

    6. [6]

      WANG Y J, YANG X X, WANG Y H. Catalytic performance of mesoporous MgO supported Ni catalyst in steam reforming of model compounds of biomass fermentation for hydrogen production[J]. In J Hydrogen Energy, 2016,41(40):17846-17857. doi: 10.1016/j.ijhydene.2016.07.258

    7. [7]

      LIU B Y, ZHENG L M, ZHU Z H, LI C, XI H X, QIAN Y. Hierarchically structured Beta zeolites with intercrystal mesopores and the improved catalytic properties[J]. Appl Catal A:Gen, 2014,470:412-419. doi: 10.1016/j.apcata.2013.11.015

    8. [8]

      LIU B Y, DUAN Q Q, LI C, ZHU Z H, XI H X, QIAN Y. Template synthesis of the hierarchically structured MFI zeolite with nanosheet frameworks and tailored structure[J]. New J Chem, 2014,38(9):4380-4387. doi: 10.1039/C4NJ00756E

    9. [9]

      LIU H, ZHANG S, XIE S J, ZHANG W S, XIN W J, LIU S L, XU L Y. Synthesis, characterization, and catalytic performance of hierarchical ZSM-11 zeolite synthesized via dual-template route[J]. Chin J Catal, 2018,39(1):167-180. doi: 10.1016/S1872-2067(17)62984-X

    10. [10]

      ZHANG X F, ZHANG K, ZHANG X G, FENG Y, YAO J F. Controlled synthesis of hierarchical beta zeolite through design template to enhance gas-phase beckmann rearrangement performance[J]. Microporous Mesoporous Mater, 2018,272:202-208. doi: 10.1016/j.micromeso.2018.06.034

    11. [11]

      PARLETT C M A, AYDIN A, DURNDELL L J, FRATTINI L, ISAACS M A, LEE A F, LIU X T, OLIVI L, TROFIMOVAITE R, WILSON K, WU C F. Tailored mesoporous silica supports for Ni catalysed hydrogen production from ethanol steam reforming[J]. Catal Commun, 2017,91:76-79. doi: 10.1016/j.catcom.2016.12.021

    12. [12]

      HOU T F, ZHANG S Y, CHEN Y D, WANG D Z, CAI W J. Hydrogen production from ethanol reforming:Catalysts and reaction mechanism[J]. Renewable Sustainable Energy Rev, 2015,44:132-148. doi: 10.1016/j.rser.2014.12.023

    13. [13]

      WANG S Y, HE B, TIAN R, SUN C, DAI R, LI X, WU X, AN X, XIE X M. Ni-hierarchical beta zeolite catalysts were applied to ethanol steam reforming:Effect of sol gel method on loading Ni and the role of hierarchical structure[J]. Mol Catal, 2018,453:64-73. doi: 10.1016/j.mcat.2018.04.034

    14. [14]

      KUMAR N, LINDFORS L E, BYGGNINGSBACKA R. Synthesis and characterization of H-ZSM-22, Zn-H-ZSM-22 and Ga-H-ZSM-22 zeolite catalysts and their catalytic activity in the aromatization of n-butane[J]. Appl Catal A:Gen, 1996,139(1/2):189-199.  

    15. [15]

      BAECK S H, LEE W Y. Skeletal isomerization of 1-butene to isobutene over Mg-ZSM-22[J]. Appl Catal A:Gen, 1997,164(1/2):291-301.  

    16. [16]

      XIAO Zhi-wen, HE Hong-yun. Synthesis, characterization and catalytic performance of double heteroatom Fe-V-β zeolite[J]. Chin J Catal, 2010,31(6):705-710.  

    17. [17]

      SONG S, WU G J, DAI W L, GUAN N J, LI L D. Al-free Fe-beta as a robust catalyst for selective reduction of nitric oxide by ammonia[J]. Catal Sci Technol, 2016,6(23):8325-8335. doi: 10.1039/C6CY02124G

    18. [18]

      ZHANG Y H, GAO F, WAN H Q, WU C, KONG Y, WU X C, ZHAO B, DONG L, CHEN Y. Synthesis, characterization of bimetallic Ce-Fe-SBA-15 and its catalytic performance in the phenol hydroxylation[J]. Microporous Mesoporous Mater, 2008,113(1/3):393-401.  

    19. [19]

      SIG K Y, AHN W S. Isomorphous substitution of Fe3- in zeolite LTL[J]. Microporous Mater, 1997,9(3/4):131-140.

    20. [20]

      INUI T, MATSUDA H, YAMASE O, NAGATA H, FUKUDA K, UKAWA T, MIYAMOTO A. Highly selective synthesis of light olefins from methanol on a novel Fe-silicate[J]. J Catal, 1986,98(2):491-501.  

    21. [21]

      LIU S Y, REN J, ZHU S J, ZHANG H K, LV E, XU J, LI Y F. Synthesis and characterization of the Fe-substituted ZSM-22 zeolite catalyst with high n-dodecane isomerization performance[J]. J Catal, 2015,330:485-496. doi: 10.1016/j.jcat.2015.07.027

    22. [22]

      JIANG X, SU X F, BAI X F, LI Y Z, YANG L, ZHANG K, ZHANG Y, LIU Y, WU W. Conversion of methanol to light olefins over nanosized[Fe, Al] ZSM-5 zeolites:Influence of Fe incorporated into the framework on the acidity and catalytic performance[J]. Microporous Mesoporous Mater, 2018,263:243-250. doi: 10.1016/j.micromeso.2017.12.029

    23. [23]

      KOEKKOEK A J J, XIN H C, YANG Q H, LI C, HENSEN E J M. Hierarchically structured Fe/ZSM-5 as catalysts for the oxidation of benzene to phenol[J]. Microporous Mesoporous Mater, 2011,145(1/3):172-181.  

    24. [24]

      YUE Y Y, LIU H Y, YUAN P, YU C Z, BAO X J. One-pot synthesis of hierarchical FeZSM-5 zeolites from natural aluminosilicates for selective catalytic reduction of NO by NH3[J]. Sci Rep-UK, 2015,59270. doi: 10.1038/srep09270

    25. [25]

      LI J Q, MIAO P J, LI Z, HE T, HAN D Z, WU J L, WANG Z Q, WU J H. Hydrothermal synthesis of nanocrystalline H[Fe, Al] ZSM-5 zeolites for conversion of methanol to gasoline[J]. Energy Convers Manage, 2015,93:259-266. doi: 10.1016/j.enconman.2015.01.031

    26. [26]

      SUN Hui-yong, WU Dong. Synthesis and characterization of Heteroatom Fe-ZSM-5 molecular sieve[J]. J Fuel Chem Technol, 1999,27(1):7-10.  

    27. [27]

      NICHELE V, SIGNORETTO M, PINNA F, GHEDINI E, COMPAGNONI M, ROSSETTI I, CRUCIANI G, MICHELE A D. Bimetallic Ni-Cu catalysts for the low-temperature ethanol steam reforming:Importance of metal-support interactions[J]. Catal Lett, 2015,145(2):549-558.

  • 加载中
    1. [1]

      Dan Li ,  Hui Xin ,  Xiaofeng Yi . Comprehensive Experimental Design on Ni-based Catalyst for Biofuel Production. University Chemistry, 2024, 39(8): 204-211. doi: 10.3866/PKU.DXHX202312046

    2. [2]

      Xue Liu , Lipeng Wang , Luling Li , Kai Wang , Wenju Liu , Biao Hu , Daofan Cao , Fenghao Jiang , Junguo Li , Ke Liu . Research on Cu-Based and Pt-Based Catalysts for Hydrogen Production through Methanol Steam Reforming. Acta Physico-Chimica Sinica, 2025, 41(5): 100049-0. doi: 10.1016/j.actphy.2025.100049

    3. [3]

      Runran WANG , Qiyue JIAO , Ruifang LI , Hong WANG , Hongwei WANG , Yali BAO , Qi WANG , Xiaoyan WANG . Influence of the loading methods of Ni species in Ni/CeO2 catalysts on the performance of CO methanation. Chinese Journal of Inorganic Chemistry, 2026, 42(5): 1026-1038. doi: 10.11862/CJIC.20250364

    4. [4]

      Yi RU , Tao MENG , Zhaoteng XUE , Dongsen MAO . Synergistic catalysis of Al distribution and pore structure in ZSM-5 zeolite for bioethanol-to-propylene. Chinese Journal of Inorganic Chemistry, 2026, 42(2): 247-262. doi: 10.11862/CJIC.20250255

    5. [5]

      Qinhui Guan , Yuhao Guo , Na Li , Jing Li , Tingjiang Yan . Molecular sieve-mediated indium oxide catalysts for enhancing photocatalytic CO2 hydrogenation. Acta Physico-Chimica Sinica, 2025, 41(11): 100133-0. doi: 10.1016/j.actphy.2025.100133

    6. [6]

      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

    7. [7]

      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

    8. [8]

      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

    9. [9]

      Lele Feng , Xueying Bai , Jifeng Pang , Hongchen Cao , Xiaoyan Liu , Wenhao Luo , Xiaofeng Yang , Pengfei Wu , Mingyuan Zheng . Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(9): 100100-0. doi: 10.1016/j.actphy.2025.100100

    10. [10]

      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

    11. [11]

      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): 100034-0. doi: 10.3866/PKU.WHXB202406012

    12. [12]

      Xichen YAO , Shuxian WANG , Yun WANG , Cheng WANG , Chuang ZHANG . Oxygen reduction performance of self?supported Fe/N/C three-dimensional aerogel catalyst layers. Chinese Journal of Inorganic Chemistry, 2025, 41(7): 1387-1396. doi: 10.11862/CJIC.20240384

    13. [13]

      Xuejie Wang , Guoqing Cui , Congkai Wang , Yang Yang , Guiyuan Jiang , Chunming Xu . Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers. Acta Physico-Chimica Sinica, 2025, 41(5): 100044-0. doi: 10.1016/j.actphy.2024.100044

    14. [14]

      Shanghua Li , Malin Li , Xiwen Chi , Xin Yin , Zhaodi Luo , Jihong Yu . High-Stable Aqueous Zinc Metal Anodes Enabled by an Oriented ZnQ Zeolite Protective Layer with Facile Ion Migration Kinetics. Acta Physico-Chimica Sinica, 2025, 41(1): 100003-0. doi: 10.3866/PKU.WHXB202309003

    15. [15]

      Yunbo ZHU , Linxiang ZHOU , Chaoyang SHI , Jie YU , Danyang WEI , Mingli XU . Stable Fe—P structure catalysts: Enabled by a strong coordination strategy and high-efficiency oxygen electrocatalysis performance. Chinese Journal of Inorganic Chemistry, 2026, 42(9): 2021-2032. doi: 10.11862/CJIC.20260080

    16. [16]

      Meng Li , Haiyan Tan , Wenjun Zhu . Three-motif molecular junction photocatalysts with long-lived charge carriers for H2O2 production. Acta Physico-Chimica Sinica, 2026, 42(6): 100257-0. doi: 10.1016/j.actphy.2026.100257

    17. [17]

      Huiwei Ding , Bo Peng , Zhihao Wang , Qiaofeng Han . Advances in Metal or Nonmetal Modification of Bismuth-Based Photocatalysts. Acta Physico-Chimica Sinica, 2024, 40(4): 2305048-0. doi: 10.3866/PKU.WHXB202305048

    18. [18]

      Yushan Cai , Fang-Xing Xiao . Revisiting MXenes-based Photocatalysis Landscape: Progress, Challenges, and Future Perspectives. Acta Physico-Chimica Sinica, 2024, 40(8): 2306048-0. doi: 10.3866/PKU.WHXB202306048

    19. [19]

      Yuanyin Cui , Jinfeng Zhang , Hailiang Chu , Lixian Sun , Kai Dai . Rational Design of Bismuth Based Photocatalysts for Solar Energy Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2405016-0. doi: 10.3866/PKU.WHXB202405016

    20. [20]

      Enqi CHEN , Xinyi MA , Xiang HAN , Yutong YE , Kexin QIN , Shenghui LI , Changli ZHANG , Min YU , Changyun CHEN . Research progress on MOF-based electrocatalysts for the urea oxidation reaction. Chinese Journal of Inorganic Chemistry, 2026, 42(9): 1871-1892. doi: 10.11862/CJIC.20260168

Metrics
  • PDF Downloads(26)
  • Abstract views(2357)
  • HTML views(398)

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