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多元介孔混合氧化物La-Mn-Ce-O催化剂的制备与表征 被引量:11

Preparation and Characterization of the Multicomponent Mesoporous Mixed Oxide Catalysts La-Mn-Ce-O
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摘要 采用柠檬酸络合-有机模板剂分解法制备出具有不同(n_(La)+n_(Mn))/(n_(La)+n_(Mn)+n_(Ce))比、不同温度焙烧的La-Mn-Ce-O系列多元介孔混合氧化物催化剂,并与传统共沉淀法制备的La-Mn-Ce-O催化剂进行比较.N_2吸附和脱附结果表明,采用模板剂法制得的样品具有较大的比表面积(高达103.5m^2·g^(-1))和较均匀的孔径分布(3.4-4.4nm);500℃焙烧样品的比表面积约为共沉淀法所制样品的三倍.600℃焙烧后,样品的孔径分布范围稍有加宽,但仍保持介孔结构.XRD表征结果表明,Mn物种具有高度的分散性,XRD难以检测,La-Ce和Mn-Ce可能部分形成了固溶体结构.XPS结果揭示,Mn-Ce间存在电子态的强相互作用,出现了Mn2p的震激峰,这种相互作用促进了氧物种在Ce和Mn物种间的传递,增强了样品的氧化还原性能,震激峰最明显的样品具有最佳的氧化性能.H_2-TPR结果表明,采用柠檬酸络合-有机模板剂分解法制备的催化剂中,锰氧化物更容易被还原,Mn—O键的活动度与CO氧化活性密切相关.活性评价结果表明,500℃焙烧的(n_(La)+n_(Mn))/(n_(La)+n_(Mn)+n_(Ce))为0.5的样品,起燃温度比传统共沉淀法制得的样品降低了50℃左右,并表现出较高的热稳定性. A series of mesoporous multicomponent mixed oxide catalysts La-Mn-Ce-O with various (nLa+nMn)/(nLa+ nMn+nCe) ratios were prepared by citric acid complexation-organic template decomposition (CAC-OTD) method. For comparison, the sample with the same composition was also prepared by conventional coprecipitation method. The results of N2 adsorption/desorption showed that the samples prepared by CAC-OTD method possessed relatively large specific surface area and uniform pore diameter distribution (3.4-4.4 nm). The results of X-ray diffraction (XRD) identified the formation of La-Ce and Mn-Ce solid solution. No Mn species were detected by XRD. The results of X-ray photoelectron spectroscopy (XPS) showed that there was a strong electronic state interaction between Mn and Ce species, resulting in the formation of Mn 2p shake-up peak. Such interaction enhanced the transfer of oxygen species from Ce to Mn oxide and therefore increased the redox activity of the samples. The sample with the strongest shake-up peak showed the highest oxidation activity. The results of temperature programmed reduction (TPR) showed that the manganese species in the samples prepared by using CAC-OTD method were easier to be reduced, which was relevant to the oxidation activity of the catalysts. The results of activity evaluation showed that the light-off temperature of the LMC(0.5)-500 sample was about 50 ℃ lower than that of the sample prepared by using coprecipitation method. The samples prepared by using CAC-OTD method showed good thermal stability.
出处 《物理化学学报》 SCIE CAS CSCD 北大核心 2007年第5期641-646,共6页 Acta Physico-Chimica Sinica
基金 国家高技术研究发展计划(863计划)(2006AA06Z348) 国家自然科学基金(20676097)资助项目
关键词 多元介孔催化剂 制备 柠檬酸络合 有机模板剂 结构表征 Multicomponent mesoporous catalyst Preparation Citric acid complexation Organic template Structural characterization
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参考文献20

  • 1Westerholm, R.; Christensen, A.; Rosén, A. Atmospheric Environment, 1996, 30(20): 3529.
  • 2Meng, M.; Zha, Y. Q.; Luo, J. Y.; Hu, T. D.; Xie, Y. N.; Liu, T.; Zhang, J. Appl. Catal. A, 2006, 301(2): 145.
  • 3Hasen, K. K.; Skou, E. M.; Christensen, H.; Turek, T. J. Catal., 2001, 199(1): 132.
  • 4Kaliaguine, S.; van Neste, A.; Szabo, V.; Gallot, J. E.; Bassir, M.; Muzychuk, R. Appl. Catal. A, 2001, 209(1-2): 345.
  • 5陈杨英,韩秀文,包信和.W-SBA-15介孔分子筛的直接合成及其对环己烯环氧化反应的催化性能[J].催化学报,2005,26(5):412-416. 被引量:54
  • 6Kosslick, H.; Lishcke, G.; Landmesser, H.; Parlitz, B.; Storek, W.; Fricke, R. J. Catal., 1998, 176(1): 102.
  • 7Zhang, Z. R.; Suo, J. S.; Zhang, X. M.; Li, S. B. Appl. Catal. A, 1999, 179(1-2): 11.
  • 8翟尚儒,巩雁军,张晔,吴东,孙予罕,蒲敏.用双表面活性剂为共模板合成中孔分子筛MCM-48[J].物理化学学报,2002,18(10):911-915. 被引量:9
  • 9Takahashi, R.; Sato, S.; Sodesawa, T.; Kawakita, M.; Ogura, K. J. Phys. Chem. B, 2000, 104(51): 12184.
  • 10Zou, Z. Q.; Meng, M.; Luo, J. Y.; Zha, Y. Q.; Xie, Y. N.; Hu, T. D.; Liu, T. J. Mol. Catal. A, 2006,249:240.

二级参考文献26

  • 1邹志强,孟明,查宇清,谢亚宁,胡天斗,刘涛.介孔混合氧化物催化剂LA-CO-ZR-O的制备与表征[J].催化学报,2006,27(2):129-134. 被引量:1
  • 2Kresge C T,Leonowicz M E,Roth W J,Vartuli J C,Beck J S. Nature,1992,359(6397):710.
  • 3Tanev P T,Pinnavaia T J. Science,1995,267(5199):865.
  • 4Bagshaw S A,Prouzet E,Pinnavaia T J. Science,1995,269(5228):1242.
  • 5Zhao D,Feng J,Huo Q,Melosh N,Frederickson G H,Chmelka B F,Stucky G D. Science,1998,279(5350):548.
  • 6Weissermal K,Arpe H J. Industrial Organic Chemistry. New York:Verlag Chemie,1978.
  • 7Jin R H,Xia X,Dai W L,Deng J-F,Li H X. Catal Lett,1999,62(2-4):201.
  • 8Zhang Zh R,Suo J Sh,Zhang X M,Li Sh B. Chem Commun,1998,(2):241.
  • 9Chen H,Dai W-L,Deng J-F,Fan K N. Catal Lett,2002,81(1-2):131.
  • 10Dai W-L,Chen H,Cao Y,Li H X,Xia S H,Fan K N. Chem Commun,2003,(7):892.

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