Citation: ZHANG Jian-li, WANG Xu, MA Li-ping, YU Xu-fei, Ma Qing-xiang, FAN Su-bing, ZHAO Tian-sheng. Preparation of layered K/Mg-Fe-Al catalysts and its catalytic performances in CO hydrogenation[J]. Journal of Fuel Chemistry and Technology, ;2017, 45(12): 1489-1498. shu

Preparation of layered K/Mg-Fe-Al catalysts and its catalytic performances in CO hydrogenation

State Key Laboratory of High-efficiency Coal Utilization and Green Chemical Engineering, Ningxia University, Yinchuan 750021, China

Corresponding author: ZHANG Jian-li, zhangjl@nxu.edu.cn ZHAO Tian-sheng, zhaots@nxu.edu.cn
Received Date: 20 July 2017
Revised Date: 26 September 2017

Fund Project: the National Natural Science Foundation of China 21666030The project was supported by the National Natural Science Foundation of China (21666030, 21366025) and the National First-Rate Discipline onstruction Project of Ningxia (Chemical Engineering and Technology)the National Natural Science Foundation of China 21366025

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A series of K promoted K/MgFeAl-HTLcs catalysts with different Mg/Fe/Al molar ratios were prepared by means of coprecipitation and impregnation method for direct synthesis of light olefins from CO hydrogenation. The samples were characterized by XRD, N₂ adsorption-desorption, SEM, TG, H₂-TPR and XPS measurements. The results show that MgFeAl-HTLcs catalyst precursors has typical layered structure. MgO, Fe₂O₃ and small amount of MgFeAlO₄ are formed after calcination. MgCO₃ and Fe₃O₄ could be observed after reaction, and a little Fe₅C₂ iron carbide with broad and weak peaks appear simultaneously. Thermal stability of K/MgFeAl-HTLcs is improved due to recovery of hydrotalcite-like structure after K promotion. With increase of Al content, specific surface area of the precursors decreases monotonically after structure reconstruction. Reduction of Fe₂O₃ to Fe₃O₄ is inhibited with addition of Al, compared with K/Mg-Fe sample. Fe enrichment before reaction and K enrichment after reaction are observed on secondary calcination samples. During CO hydrogenation, the prepared samples show high activity and C_2-4⁼ selectivity with low C₅₊ weight fraction. C₅₊ hydrocarbons decrease and olefin selectivity increases with increasing Fe/Al molar ratio. The C₅₊ decreases from 22.17% to 10.90%, and C_2-4⁼ weight content increases from 40.98% to 47.28% on K/1.5Mg-0.67Fe-0.33Al sample compared with that of K/1.5Mg-0.67Fe sample.
- Fischer-Tropsch synthesis,
- K/Mg-Fe-Al catalyst,
- CO hydrogenation,
- light olefins
1. [1]
  TORRES GALVIS H M, BITTER J H, KHARE C B, RUITENBEEK M, IULIAN DUGULAN A, DE JONG K P. Supported iron nanoparticles as catalysts for sustainable production of lower olefins[J]. Science, 2012,335(6070):835-838. doi: 10.1126/science.1215614
2. [2]
  JIAO F, LI J J, PAN X L, XIAO J P, LI H B, MA H, WEI M M, PAN Y, ZHOU Z Y, LI M R, MIAO S, LI J, ZHU Y F, XIAO D, HE T, YANG J H, QI F, FU Q, BAO X H. Selective conversion of syngas to light olefins[J]. Science, 2016,351(6277):1065-1068. doi: 10.1126/science.aaf1835
3. [3]
  CHENG K, GU B, LIU X L, KANG J C, ZHANG Q H, WANG Y. Direct and highly selective conversion of synthesis gas into lower olefins:design of a bifunctional catalyst combining methanol synthesis and carbon-carbon coupling[J]. Angew Chem Int Ed, 2016,55(15):4725-4728. doi: 10.1002/anie.201601208
4. [4]
  ZHONG L S, YU F, AN Y L, ZHAO Y H, SUN Y H, LI Z J, LIN T J, LIN Y J, QI X Z, DAI Y Y, GU L, HU J S, JIN S F, SHEN Q, WANG H. Cobalt carbide nanoprisms for direct production of lower olefins from syngas[J]. Nature, 2016,538(7623):84-87. doi: 10.1038/nature19786
5. [5]
  ZHAI P, XU C, GAO R, LIU X, LI M Z, LI W Z, FU X P, JIA C J, XIE J L, ZHAO M, WANG X P, LI Y W, ZHANG Q W, WEN X D, MA D. Highly tunable selectivity for syngas-derived alkenes over zinc and sodium-modulated Fe₅C₂ catalyst[J]. Angew Chem Int Ed, 2016,55(34):9902-9907. doi: 10.1002/anie.201603556
6. [6]
  YU Fei, LI Zheng-jia, AN Yun-lei, ZHONG Liang-shu, SUN Yu-han. Research progress in the direct conversion of syngas to lower olefins. J Fuel Chem Technol, 2016, 44(7):801-814.
7. [7]
  CAVANI F, TRIFIRÒF , VACCARI A. Hydrotalcite-type anionic clays:Preparation, properties and applications[J]. Catal Today, 1991,11(2):173-301. doi: 10.1016/0920-5861(91)80068-K
8. [8]
  GAO Peng, LI Feng, ZHAO Ning, WANG Hui, WEI Wei, SUN Yu-han. Preparation of Cu/Zn/Al/(Zr)/(Y) catalysts from hydrotalcite-like precursors and their catalytic performance for the hydrogenation of CO₂ to methanol[J]. Acta Phys-Chim Sin, 2014,30(6):1155-1162. doi: 10.3866/PKU.WHXB201401252
9. [9]
  FRONZO A D, PIROLA C, COMAZZI A, GALLI F, BIANCHI C L, MICHELE A D, VIVANI R, NOCCHETTI M, BASTIANINI M, BOFFITO D C. Co-based hydrotalcites as new catalysts for the Fischer-Tropsch synthesis process[J]. Fuel, 2014,119(3):62-69.
10. [10]
  XIE Xian-mei. Study on the preparation, performances and application of hydrotalcite-like-compounds[D]. Taiyuan:Taiyuan University of Technology, 2006.
11. [11]
  MA Li-ping, ZHANG Jian-li, MA Qing-xiang, FAN Su-bing, ZHAO Tian-sheng. Direct synthesis of light olefins from CO hydrogenation over K/MgFeZn-HTLcs catalysts[J]. J Fuel Chem Technol, 2016,44(4):449-456.
12. [12]
  VISCONTI C G, LIETTI L, TRONCONI E, FORZATTI P, ZENNARO R, FINOCCHIO E. Fischer-Tropsch synthesis on a Co/Al₂O₃ catalyst with CO₂ containing syngas[J]. Appl Catal A:Gen, 2009,355(1/2):61-68.
13. [13]
  PARK S J, BAE J W, OH J H, CHARY K V R, SAI PRASAD P S, JUN K W, RHEE Y W. Influence of bimodal pore size distribution of Ru/Co/ZrO₂-Al₂O₃ during Fischer-Tropsch synthesis in fixed-bed and slurry reactor[J]. J Mol Catal A:Chem, 2009,298(1):81-87.
14. [14]
  TOSHIYUKI HIBINO, YASUMASA Y, KATSUNORI K, ATSUMU T. Decarbonation behavior of Mg-A1-CO₃ hydrotalcite-like compounds during heat treatment[J]. Clay Clay Miner, 1995,43(4):427-432. doi: 10.1346/CCMN
15. [15]
  VALENTE J S, PRINCE J, MAUBERT A M, LARTUNDO-ROJAS L, ANGEL P D, FERRAT G, HERNANDEZ J G, LOPEZ-SALINAS E. Physicochemical study of nanocapsular layered double hydroxides evolution[J]. J Phys Chem C, 2009,113(14):5547-5555. doi: 10.1021/jp810293y
16. [16]
  ZHAO M Q, ZHANG Q, ZHANG W, HUANG J Q, ZHANG Y H, SU D S, WEI F. Embedded high density metal nanoparticles with extraordinary thermal stability derived from guest-host mediated layered double hydroxides[J]. J Am Chem Soc, 2010,132(42):14739-14741. doi: 10.1021/ja106421g
17. [17]
  JOZWIAK W K, KACZMAREK E, MANIECKI T P, IGNACZAK W, MANIUKIEWICZ W. Reduction behavior of iron oxides in hydrogen and carbon monoxide atmospheres[J]. Appl Catal A:Gen, 2007,326(1):17-27. doi: 10.1016/j.apcata.2007.03.021
18. [18]
  LI S, LI A, KRISHNAMOORTHY S, IGLESIA E. Effects of Zn, Cu, and K promoters on the structure and on the reduction, carburization, and catalytic behavior of iron-based Fischer-Tropsch synthesis catalysts[J]. Catal Lett, 2001,77(4):197-205. doi: 10.1023/A:1013284217689
19. [19]
  SUO H, WANG S, ZHANG C, XU J, WU B, YANG Y, XIANG H, LI Y. Chemical and structural effects of silica in iron-based Fischer-Tropsch synthesis catalysts[J]. J Catal, 2012,286(2):111-123.
20. [20]
  GAO X, SHEN J, HSIA Y, CHEN Y. Reduction of supported iron oxide studied by temperature-programmed reduction combined with mössbauer spectroscopy and X-ray diffraction[J]. J Chem Soc Faraday Trans, 1993,89(7):1079-1084. doi: 10.1039/FT9938901079
21. [21]
  CHEN K, FAN Y, HU Z, YAN Q. Carbon monoxide hydrogenation on Fe₂O₃/ZrO₂ catalysts[J]. Catal Lett, 1996,36(3/4):139-144.
22. [22]
  QIN S D, ZHANG C H, XU J, YANG Y, XIANG H W, LI Y W. Fe-Mo interactions and their influence on Fischer-Tropsch synthesis performance[J]. Appl Catal A:Gen, 2011,392(1/2):118-126.
23. [23]
  HUO C F, WU B S, GAO P, YANG Y, LI Y W, JIAO H J. The mechanism of potassium promoter:Enhancing the stability of active surfaces[J]. Angew Chem Int Edit, 2011,50(32):7403-7406. doi: 10.1002/anie.v50.32
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