Citation: QING Shao-jun, HOU Xiao-ning, LIU Ya-jie, WANG Lei, LI Lin-dong, GAO Zhi-xian. Catalytic performance of Cu-Ni-Al spinel for methanol steam reforming to hydrogen[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(10): 1210-1217. shu

Catalytic performance of Cu-Ni-Al spinel for methanol steam reforming to hydrogen

1.
Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
School of Chemistry and Chemical Engineering, Xinjiang University, Urumqi 830046, China

Corresponding author: GAO Zhi-xian, gaozx@sxicc.ac.cn
Received Date: 18 July 2018
Revised Date: 22 August 2018

Fund Project: the National Nature Science Foundation of China 21763018the National Nature Science Foundation of China 21673270The project was supported by the National Nature Science Foundation of China (21503254, 21673270, 21763018)the National Nature Science Foundation of China 21503254

Figures(9)

Using copper hydroxide, nickel acetate and pseudoboehmite as materials, the Cu-Ni-Al spinel catalysts were synthesized by the solid-phase method. The effects of Cu/Ni/Al molar ratio and calcination temperature on specific surface area, phase composition, reduction performance and surface property of Cu-Ni-Al spinel catalysts were characterized by BET, XRD, H₂-TPR and XPS. Moreover, the sustained release catalytic performances of Cu-Ni-Al spinel samples for methanol steam reforming were tested. The obtained results indicated that with increasing the calcination temperature, the content of Cu-Ni-Al spinel increased, but the size of spinel particles increased and the specific surface area decreased. Change of the calcination temperature and Cu/Ni/Al molar ratio led to different specific surface area, reduction performance and surface property of Cu-Ni-Al spinel catalysts, thus showing different sustained release catalytic performance. Comparing with those of stoichiometric ratio of Cu/Al=1:2, spinel solid solutions with smaller particle size, higher specific surface area and pore volume, more hardly-reducible spinel and better sustained release catalytic performance were obtained with the nonstoichiometric ratio of Cu/Al=1:3. The results of catalyst evaluation indicated that active copper species were released from Cu-Ni-Al spinel lattice and thus took part in the catalytic action. Among the prepared catalysts, CNA3-1000 catalyst showed the highest catalytic activity and stability.
- Cu-Ni-Al spinel,
- solid-phase method,
- methanol steam reforming,
- hydrogen
1. [1]
  WANG M Y, WANG Z, GONG X Z, GUO Z C. The intensification technologies to water electrolysis for hydrogen production-A review[J]. Renewable Sustainable Energy Rev, 2014,29:573-588. doi: 10.1016/j.rser.2013.08.090
2. [2]
  BELL T E, TORRENTE-MURCIANO L. H₂ Production via ammonia decomposition using non-noble metal catalysts:A review[J]. Top Catal, 2016,59(15):1438-1457.
3. [3]
  PAL D B, CHAND R, UPADHYAY S N, MISHRA P K. Performance of water gas shift reaction catalysts:A review[J]. Renewable Sustainable Energy Rev, 2018,93:549-565. doi: 10.1016/j.rser.2018.05.003
4. [4]
  SÁ S, SILVA H, BRANDÃO L, SOUSA J M, MENDES A. Catalysts for methanol steam reforming:A review[J]. Appl Catal B:Environ, 2010,99(1):43-57.
5. [5]
  LIN L L, ZHOU W, GAO R, YAO S Y, ZHANG X, XU W Q, ZHENG S J, JIANG Z, YU Q L, LI Y W, SHI C, WEN X D, MA D. Low-temperature hydrogen production from water and methanol using Pt/α-MoC catalysts[J]. Nature, 2017,544:80-97. doi: 10.1038/nature21672
6. [6]
  BAGHERZADEH S B, HAGHIGHI M. Plasma-enhanced comparative hydrothermal and coprecipitation preparation of CuO/ZnO/Al₂O₃ nanocatalyst used in hydrogen production via methanol steam reforming[J]. Energy Convers Manage, 2017,142:452-465. doi: 10.1016/j.enconman.2017.03.069
7. [7]
  SANCHES S G, HUERTAS FLORES J, PAIS DA SILVA M I. Influence of aging time on the microstructural characteristics of a Cu/ZnO-based catalyst prepared by homogeneous precipitation for use in methanol steam reforming[J]. React Kinet Mech Catal, 2017,121(2):473-485. doi: 10.1007/s11144-017-1161-7
8. [8]
  YANG Shu-qian, ZHANG Na, HE Jian-ping, ZHANG Lei, WANG Hong-hao, BAI Jin, ZHANG Jian, LIU Dao-sheng, YANG Zhan-xu. Effect of impregnation sequence of Ce on the performance of Cu/Zn-Al catalysts derived from hydrotalcite precursor in methanol steam reforming[J]. J Fuel Chem Technol, 2018,46(4):479-488. doi: 10.3969/j.issn.0253-2409.2018.04.014
9. [9]
  YANG Shu-qian, HE Jian-ping, ZHANG Na, SUI Xiao-wei, ZHANG Lei, YANG Zhan-xu. Effect of rare-earth element modification on the performance of Cu/ZnAl catalysts derived from hydrotalcite precursor in methanol steam reforming[J]. J Fuel Chem Technol, 2018,46(2):179-188. doi: 10.3969/j.issn.0253-2409.2018.02.007
10. [10]
  TAHAY P, KHANI Y, JABARI M, BAHADORAN F, SAFARI N. Highly porous monolith/TiO₂ supported Cu, Cu-Ni, Ru, and Pt catalysts in methanol steam reforming process for H₂ generation[J]. Appl Catal A:Gen, 2018,554:44-53. doi: 10.1016/j.apcata.2018.01.022
11. [11]
  XI H J, HOU X N, LIU Y J, QING S J, GAO Z X. Cu-Al spinel oxide as an efficient catalyst for methanol steam reforming[J]. Angew Chem Int Ed, 2014,53(44):11886-11889. doi: 10.1002/anie.201405213
12. [12]
  LIU Y J, QING S J, HOU X N, QIN F J, WANG X, GAO Z X, XIANG H W. Temperature dependence of Cu-Al spinel formation and its catalytic performance in methanol steam reforming[J]. Catal Sci Technol, 2017,7(21):5069-5078. doi: 10.1039/C7CY01236E
13. [13]
  QIN Fa-jie, LIU Ya-jie, QING Shao-jun, HOU Xiao-ning, GAO Zhi-xian. Cu-Al spinel as a sustained release catalyst for H₂ production from methanol steam reforming:Effects of different copper sources[J]. J Fuel Chem Technol, 2017,45(12):1481-1488. doi: 10.3969/j.issn.0253-2409.2017.12.010
14. [14]
  ZHOU R S, SNYDER R L. Structures and transformation mechanisms of theη, γ and θ transition aluminas[J]. Acta Cryst, 1991,47(5):617-630. doi: 10.1107/S0108768191002719
15. [15]
  AREÁN C O, VIÑUELA J S D. Structural study of copper-nickel aluminate (Cu_xNi_1-xAl₂O₄) spinels[J]. J Solid State Chem, 1985,60(1):1-5.
16. [16]
  STROHMEIER B R, LEYDEN D E, FIELD R S, HERCULES D M. Surface spectroscopic characterization of Cu/Al₂O₃ catalysts[J]. J Catal, 1985,94(2):514-530. doi: 10.1016/0021-9517(85)90216-7
17. [17]
  FIGUEIREDO R T, MARTÍNEZ-ARIAS A, GRANADOS M L, FIERRO J L G. Spectroscopic evidence of Cu-Al interactions in Cu-Zn-Al mixed oxide catalysts used in CO hydrogenation[J]. J Catal, 1998,178(1):146-152. doi: 10.1006/jcat.1998.2106
18. [18]
  WAGNER C D, DAVIS L E, ZELLER M V, TAYLOR J A, RAYMOND R H, GALE L H. Empirical atomic sensitivity factors for quantitative analysis by electron spectroscopy for chemical analysis[J]. Surf Interface Anal, 1981,3(5):211-225. doi: 10.1002/(ISSN)1096-9918
19. [19]
  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
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