负载型SBA-15铬基催化剂的制备及其催化CO_2氧化乙烷脱氢性能
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摘要
采用水热法制得具有不同孔径的SBA-15材料;采用浸渍法制备了负载型铬基SBA-15催化剂,其结构和性能经XRD、低温氮气吸附脱附、氢气程序升温还原和X-射线光电子能谱表征。并研究了催化剂的CO_2氧化乙烷催化脱氢性能。结果表明:孔径对活性组分在SBA-15孔道内外的分布有影响,进而影响其催化性能。孔径为8.14 nm时,乙烷转化率25.8%,乙烯选择性81.0%。
A series of SBA-15 with different pore sizes were obtained by hydrothermal method. Several Cr-based SBA-15 catalysts were prepared by conventional impregnation method. The structures and properties were characterized by XRD, N_2 adsorption-desorption, H_2-TPR and XPS. The catalytic performances of Cr-based SBA-15 catalysts for ethane ODH in the presence of CO_(2 )were investigated. The results showed that pore size has an influence on the distribution of active components inside and outside the pores, and then affect the catalytic performances. When the pore size was 8.14 nm, the conversion of C_2H_6 was up to 25.8% and the selectivity of ethylene was 81.0%, respectively.
A series of SBA-15 with different pore sizes were obtained by hydrothermal method. Several Cr-based SBA-15 catalysts were prepared by conventional impregnation method. The structures and properties were characterized by XRD, N_2 adsorption-desorption, H_2-TPR and XPS. The catalytic performances of Cr-based SBA-15 catalysts for ethane ODH in the presence of CO_(2 )were investigated. The results showed that pore size has an influence on the distribution of active components inside and outside the pores, and then affect the catalytic performances. When the pore size was 8.14 nm, the conversion of C_2H_6 was up to 25.8% and the selectivity of ethylene was 81.0%, respectively.
引文
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[3] JI M,HONG D Y,CHANG J S,et al.Oxidative dehydrogenation of ethane with carbon dioxide over supported chromium oxide catalysts[J].Studies in Surface Science & Catalysis,2004,153:339-342.
[4] KRUK M,CAO L.Pore size tailoring in large-pore SBA-15 silica synthesized in the presence of hexane[J].Langmuir,2007,23(13):7247-54.
[5] ZHAO D,FENG J,HUO Q,et al.Triblock copolymer syntheses of mesoporous silica with periodic 50 to 300 angstrom pores[J].Science,1998,279(5350):548-552.
[6] ESPARA J M,OJEDA M L,CAMPERO A,et al.N2 adsorption scanning behavior of SBA-15 porous substrates[J].Colloids & Surfaces A Physicochemical & Engineering Aspects,2004,241(1-3):35-45.
[7] KURK M,CAO L.Pore size tailoring in large-pore SBA-15 silica synthesized in the presence of hexane[J].Langmuir,2007,23(13):7247-7254.
[8] HE L,FU L,TANG Y.Catalytic performance of a novel Cr/ZnAlLaO catalyst for oxidative dehydrogenation of isobutene[J].Catalysis Science & Technology,2015,5(2):1115-1125.
[9] HAKULI A,HRLIN M E,BACKMAN L B,et al.Dehydrogenation of i-butane on CrOx/SiO2,catalysts[J].Journal of Catalysis,1999,184(2):349-356.
[10] CAVANI F,KOUTYREV M,TRIFIRO F,et al.Chemical and physical characterization of alumina-supported chromia-based catalysts and their activity in dehydrogenation of isobutane[J].Journal of Catalysis,1996,158(1):236-250.
[11] SHI X,JI S,KAI W,et al.Oxidative dehydrogenation of ethane with CO2 over Novel Cr/SBA15/Al2O3/FeCrAl monolithic catalysts[J].Energy Fuels,2008,22(6):3631-3638.
[12] MICHORAZYK P,OGONOWKSI J,ZENCZAK K.Activity of chromium oxide deposited on different silica supports in the dehydrogenation of propane with CO2:A comparative study[J].Journal of Molecular Catalysis A Chemical,2011,349(1):1-12.
[13] SHISHIDO T,SHIMAURA K,TERAMURA K,et al.Role of CO2,in dehydrogenation of propane over Cr-based catalysts[J].Catalysis Today,2012,185(1):151-156.
[14] WANY S,MURATA K,HAYAKAWA T,et al.Oxidative dehydrogenation of ethane by carbon dioxide over sulfate-modified Cr2O3/SiO2,catalysts[J].Catalysis Letters,1999,63(1-2):59-64.
[15] TAKEHIRA K,OHISHI Y,SHISHIDO T,et al.Behavior of active sites on Cr-MCM-41 catalysts during the dehydrogenation of propane with CO2[J].Journal of Catalysis,2004,224(2):404-416.