Citation: GUO Shu-jia, WANG Sen, LUO Yao-ya, LUO Li, DONG Mei, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Effect of H-ZSM-5 zeolite morphology on the performance of bifunctional ZnCr₂O₄/H-ZSM-5 catalysts in the direct conversion of syngas into aromatics[J]. Journal of Fuel Chemistry and Technology, ;2020, 48(8): 970-979. shu

Effect of H-ZSM-5 zeolite morphology on the performance of bifunctional ZnCr₂O₄/H-ZSM-5 catalysts in the direct conversion of syngas into aromatics

GUO Shu-jia ^1,2 ,
WANG Sen ^1,, ,
LUO Yao-ya ^1,2 ,
LUO Li ^1,2 ,
DONG Mei ¹ ,
QIN Zhang-feng ^1,, ,
FAN Wei-bin ¹ ,
WANG Jian-guo ²

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: WANG Sen, wangsen@sxicc.ac.cn QIN Zhang-feng, qzhf@sxicc.ac.cn
Received Date: 8 June 2020
Revised Date: 26 July 2020

Fund Project: the National Natural Science Foundation of China U1862101the National Natural Science Foundation of China U1910203the National Natural Science Foundation of China 21773281Natural Science Foundation of Shanxi Province of China 201901D211581the National Natural Science Foundation of China 21802157the National Natural Science Foundation of China 21991092The project was supported by the National Natural Science Foundation of China (21991092, U1910203, U1862101, 21773281, 21802157) and Natural Science Foundation of Shanxi Province of China (201901D211581)

Figures(7)

A series of H-ZSM-5 zeolites with different morphologies including spherical, hollow, sheet and sponge-strip forms were hydrothermally synthesized through elaborately controlling the synthesis conditions and their crystal structural, textural and acidic properties were characterized by XRD, SEM, Py-FTIR, NH₃-TPD, ICP and N₂-sorption. The H-ZSM-5 zeolites of different morphologies and a spinel ZnCr₂O₄ oxide were then used to compose the bifunctional ZnCr₂O₄/H-ZSM-5 catalysts for the direct conversion of syngas into aromatics (STA). The effect of H-ZSM-5 morphology on the catalytic performance of ZnCr₂O₄/H-ZSM-5 in STA was then investigated. The results indicate that the morphology of H-ZSM-5 zeolites has significant influences on the catalytic performance of ZnCr₂O₄/H-ZSM-5 in STA.The selectivity to aromatics over the bifunctional catalysts with different H-ZSM-5 morphologies follows the order of sphere > sponge-strip > hollow > sheet. In particular, the ZnCr₂O₄/H-ZSM-5(sphere) catalyst composed of ZnCr₂O₄ and spherical H-ZSM-5 exhibits excellent performance in STA; under 350℃ and 3.0 MPa, a high selectivity of 68.8% to aromatics is achieved, with a CO conversion of 12.6%, whereas the selectivities to CH₄, C_2-4⁰ alkanes and CO₂ decrease to 1.3%, 14.3% and 41.4%, respectively. The isotropic and moderate particle size (about 350 nm) with appropriate pore length of spherical H-ZSM-5 zeolite are capable of avoiding the formation of lower hydrocarbons from early diffusion out of the acid zeolite channels and meanwhile yet conducive to the diffusion of aromatics, which can promote the aromatization of intermediates in STA and enhance the selectivity to aromatic products.
- syngas to aromatics,
- ZSM-5 zeolite,
- morphology,
- ZnCr₂O₄ spinel,
- bifunctional catalyst
1. [1]
  XU Y, LIU D, LIU X. Conversion of syngas toward aromatics over hybrid Fe-based Fischer-Tropsch catalysts and H-ZSM-5 zeolites[J]. Appl Catal A:Gen, 2018,552:168-183. doi: 10.1016/j.apcata.2018.01.012
2. [2]
  SETTLE A E, BERSTIS L, RORRER N A, ROMAN-LESHKOV Y, BECKHAM G T, RICHARDS R M, VARDON D R. Heterogeneous Diels-Alder catalysis for biomass-derived aromatic compounds[J]. Green Chem, 2017,19(15):3468-3492. doi: 10.1039/C7GC00992E
3. [3]
  DING Ming. Recent progress of aromatics industry and development trend[J]. Guangdong Chem Ind, 2015,42(7):78-80.
4. [4]
  YUNG M M, JABLONSKI W S, MAGRINI-BAIR K A. Review of catalytic conditioning of biomass-derived syngas[J]. Energy Fuels, 2009,23(3/4):1874-1887.
5. [5]
  CHANG C D, LANG W H, SILVESTRI A J. Synthesis gas conversion to aromatic-hydrocarbons[J]. J Catal, 1979,56(2):268-273. doi: 10.1016/0021-9517(79)90113-1
6. [6]
  YANG J H, PAN X L, JIAO F, LI J, BAO X H. Direct conversion of syngas to aromatics[J]. Chem Commun, 2017,53(81):11146-11149. doi: 10.1039/C7CC04768A
7. [7]
  CHENG K, ZHOU W, KANG J C, HE S, SHI S L, ZHANG Q H, PAN Y, WEN W, WANG Y. Bifunctional catalysts for one-step conversion of syngas into aromatics with excellent selectivity and stability[J]. Chem, 2017,3(2):334-347. doi: 10.1016/j.chempr.2017.05.007
8. [8]
  LUO Yao-ya, WANG Sen, GUO Shu-jia, YUAN Kai, WANG Hao, DONG Mei, QIN Zhang-feng, FAN Wei-bin, WANG Jian-guo. Study on different synthesis methods of Zn_xCe_2-yZr_yO₄/SAPO-34 catalyst and its catalytic performance in syngas to low-carbon olefins[J]. J Fuel Chem Technol, 2020,48(05):594-600.
9. [9]
  YANG Cheng, ZHANG Cheng-hua, XU Jian, Wu Bao-shan, YANG Yong, LI Yong-wang. One-step catalytic conversion of syngas to aromatics over ZrO₂ catalyst[J]. J Fuel Chem Technol, 2016,44(7):837-844.
10. [10]
  LIU J G, HE Y R, YAN L L, LI K, ZHANG C H, XIANG H W, WEN X D, LI Y W. Nano-sized ZrO₂ derived from metal-organic frameworks and their catalytic performance for aromatic synthesis from syngas[J]. Catal Sci Technol, 2019,9(11):2982-2992. doi: 10.1039/C9CY00453J
11. [11]
  ZHOU W, SHI S, WANG Y, ZHANG L, WANG Y, ZHANG G, MIN X, CHENG K, ZHANG Q, KANG J, WANG Y. Selective conversion of syngas to aromatics over a Mo-ZrO₂/H-ZSM-5 bifunctional catalyst[J]. ChemCatChem, 2019,11(6):1681-1688. doi: 10.1002/cctc.201801937
12. [12]
  LIU C, LIU S, ZHOU H B, SU J J, JIAO W Q, ZHANG L, WANG Y D, HE H Y, XIE Z K. Selective conversion of syngas to aromatics over metal oxide/HZSM-5 catalyst by matching the activity between CO hydrogenation and aromatization[J]. Appl Catal A:Gen, 2019,585:117206-117215. doi: 10.1016/j.apcata.2019.117206
13. [13]
  YANG X L, SUN T, MA J G, SU X, WANG R F, ZHANG Y R, DUAN H M, HUANG Y Q, ZHANG T. The influence of intimacy on the 'iterative reactions' during OX-ZEO process for aromatic production[J]. J Energy Chem, 2019,35:60-65. doi: 10.1016/j.jechem.2018.11.003
14. [14]
  GILANI S Z A, LU L, ARSLAN M T, ALI B, WANG Q, WEI F. Two-way desorption coupling to enhance the conversion of syngas into aromatics by MnO/H-ZSM-5[J]. Catal Sci Technol, 2020,10(10):3366-3375. doi: 10.1039/D0CY00275E
15. [15]
  ZHOU W, ZHOU C, YIN H R, SHI J Q, ZHANG G Q, ZHENG X L, MIN X J, ZHANG Z Q, CHENG K, KANG J C, ZHANG Q H, WANG Y. Direct conversion of syngas into aromatics over a bifunctional catalyst:Inhibiting net CO₂ release[J]. Chem Commun, 2020,56(39):5239-5242. doi: 10.1039/D0CC00608D
16. [16]
  FIROOZI M, BAGHALHA M, ASADI M. The effect of micro and nano particle sizes of H-ZSM-5 on the selectivity of MTP reaction[J]. Catal Commun, 2009,10(12):1582-1585. doi: 10.1016/j.catcom.2009.04.021
17. [17]
  CHOI M, NA K, KIM J, SAKAMOTO Y, TERASAKI O, RYOO R. Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts[J]. Nature, 2009,461:246-249. doi: 10.1038/nature08288
18. [18]
  WANG K, DONG M, LI J, LIU P, ZHANG K, WANG J, FAN W. Facile fabrication of ZSM-5 zeolite hollow spheres for catalytic conversion of methanol to aromatics[J]. Catal Sci Technol, 2017,7(3):560-564. doi: 10.1039/C6CY02476A
19. [19]
  YANG J H, GONG K, MIAO D Y, JIAO F, PAN X L, MENG X J, XIAO F S, BAO X H. Enhanced aromatic selectivity by the sheet-like ZSM-5 in syngas conversion[J]. J Energy Chem, 2019,35:44-48. doi: 10.1016/j.jechem.2018.10.008
20. [20]
  XU Y, LIU J, WANG J, MA G, LIN J, YANG Y, LI Y, ZHANG C, DING M. Selective conversion of syngas to aromatics over Fe₃O₄@MnO₂ and hollow HZSM-5 bifunctional catalysts[J]. ACS Catal, 2019,9(6):5147-5156. doi: 10.1021/acscatal.9b01045
21. [21]
  LI Q H, HEDLUND J, STERTE J, CREASER D, BONS A J. Synthesis and characterization of zoned MFI films by seeded growth[J]. Microporous Mesoporous Mater, 2002,56(3):291-302. doi: 10.1016/S1387-1811(02)00503-6
22. [22]
  NA J, LIU G, ZHOU T, DING G, HU S, WANG L. Synthesis and catalytic performance of ZSM-5/MCM-41 zeolites with varying mesopore size by surfactant-directed recrystallization[J]. Catal Lett, 2013,143(3):267-275. doi: 10.1007/s10562-013-0963-0
23. [23]
  WEI Z H, XIA T F, LIU M H, CAO Q S, XU Y R, ZHU K, ZHU X D. Alkaline modification of ZSM-5 catalysts for methanol aromatization:The effect of the alkaline concentration[J]. Front Chem Sci Eng, 2015,9(4):450-460. doi: 10.1007/s11705-015-1542-2
24. [24]
  WANG Yu-jie, FU Ting-jun, MA Zhe, SHAO Juan, MA Qian, LI Han, GUO Yu-hang, CUI Li-ping, LI Zhong. Recent progress on the control of microporous channel for ZSM-5 catalyst in methanol to hydrocarbon[J]. Chem Ind Eng Prog, 2019,38(10):4554-4563.
25. [25]
  JANG H G, MIN H K, LEE J K, HONG S B, SEO G. SAPO-34 and ZSM-5 nanocrystals' size effects on their catalysis of methanol-to-olefin reactions[J]. Appl Catal A:Gen, 2012,437:120-130.
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Effect of H-ZSM-5 zeolite morphology on the performance of bifunctional ZnCr2O4/H-ZSM-5 catalysts in the direct conversion of syngas into aromatics

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通讯作者: 陈斌, bchen63@163.com

Effect of H-ZSM-5 zeolite morphology on the performance of bifunctional ZnCr₂O₄/H-ZSM-5 catalysts in the direct conversion of syngas into aromatics