Sn掺杂量对Pt/Sn-MFI催化剂的丙烷脱氢性能影响
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摘要
随着对丙烯需求的日渐增加,由丙烷催化脱氢制丙烯来实现对丙烯的增产,已成为增产丙烯的重要手段之一。利用水热法制备一系列不同Sn掺杂量的Sn-MFI载体,采用等体积浸渍法制备相同Pt负载量的Pt/Sn-MFI催化剂,通过XRD、N2吸附-脱附、FT-IR和H2-TPR等表征考察不同Sn掺杂量的催化剂对丙烷催化脱氢性能的影响。结果表明,Pt/Sn1. 3%-MFI催化剂具有最高的催化丙烷脱氢活性和稳定性,丙烷初始转化率为43. 3%,丙烯选择性为98. 9%。反应360 min后,丙烷转化率为25. 1%,选择性保持不变。
With the increasing demand for propylene,production of propylene by catalytic dehydrogenation of propane has become one of the important means. In this work,a series of Sn-MFI supports with different Sn-doped amounts were prepared by hydrothermal method. Pt/Sn-MFI catalysts with the same Pt loading were prepared by impregnation. Catalysts were characterized by XRD,N2adsorption-desorption,FT-IR and so on. Influences of Sn-doped contents on propane dehydrogenation were also investigated.Results showed that Pt/Sn1. 3%-MFI catalyst had the highest activity and stability for dehydrogenation of propane among the as-prepared catalysts. Initial conversion of propane was 43. 3% and selectivity of propylene was 98. 9%. After 360 min of reaction,conversion of propane decreased to 25. 1% and selectivity unchanged.
With the increasing demand for propylene,production of propylene by catalytic dehydrogenation of propane has become one of the important means. In this work,a series of Sn-MFI supports with different Sn-doped amounts were prepared by hydrothermal method. Pt/Sn-MFI catalysts with the same Pt loading were prepared by impregnation. Catalysts were characterized by XRD,N2adsorption-desorption,FT-IR and so on. Influences of Sn-doped contents on propane dehydrogenation were also investigated.Results showed that Pt/Sn1. 3%-MFI catalyst had the highest activity and stability for dehydrogenation of propane among the as-prepared catalysts. Initial conversion of propane was 43. 3% and selectivity of propylene was 98. 9%. After 360 min of reaction,conversion of propane decreased to 25. 1% and selectivity unchanged.
引文
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[2]Pakhomov N A,Kashkin V N,Nemykina E I,et al. Dehydrogenation of C3-C4,paraffins on Cr2O3/Al2O3,catalysts in fluidized and fixed bed reactors[J]. Chemical Engineering Journal,2009,154(1/3):185-188.
[3]Fan X Q,Li J C,Zhao Z,et al. Dehydrogenation of propane over Pt Sn/SBA-15 catalysts:effect of the amount of metal loading and state[J]. RSC Advances,2015,5(36):28305-28315.
[4]Nawaz Z,Tang X,Zhang Q,et al. SAPO-34 supported PtSn-based novel catalyst for propane dehydrogenation to propylene[J]. Catalysis Communications,2009,10(14):1925-1930.
[5]Sattler J J,Ruiz-Martinez J,Santillan-Jimenez E,et al.Catalytic dehydrogenation of light alkanes on metals and metal oxides[J]. Chemical Reviews,2014,114(20):10613-10653.
[6]李思漩,张惠民,夏蕾,等.丙烷脱氢制丙烯催化剂研究进展[J].现代化工,2018,38(2):14-21.Li Sixuan,Zhang Huimin,Xia Lei,et al. Research progress on catalysts for the dehydrogenation of propane to propylene[J]. Modern Chemical Industry,2018,38(2):14-21.
[7]Liu G,Zeng L,Zhao Z J,et al. Platinum-modified Zn O/Al2O3for propane dehydrogenation:minimized platinum usage and improved catalytic stability[J]. ACS Catalysis,2016,6(4):2158-2162.
[8]Jiang F,Zeng L,Li S,et al. Propane dehydrogenation over Pt/Ti O2-Al2O3catalysts[J]. ACS Catalysis,2015,5(1):438-447.
[9]Kwak J H,Hu J Z,Mei D H,et al. Coordinatively unsaturated Al3+centers as binding sites for active catalyst phases of platinum onγ-Al2O3[J]. Science,2009,325(5948):1670-1673.
[10]Kim W,So J,Choi S W,et al. Hierarchical Ga-MFI catalysts for propane dehydrogenation[J]. Chemistry of Materials,2017,29(17):7213-7222.
[11]Li J,Li J,Zhao Z,et al. Size effect of TS-1 supports on the catalytic performance of Pt Sn/TS-1 catalysts for propane dehydrogenation[J]. Journal of Catalysis,2017,352:361-370.
[12]Feng B,Song C,LüG,et al. Structural characterization and selective catalytic reduction of nitrogen oxides with ammonia:a comparison between Co/ZSM-5 and Co/SBA-15[J]. Journal of Physical Chemistry C,2012,116(50):26262-26274.
[13]Zhang Y,Zhou Y,Qiu A,et al. Propane dehydrogenation on Pt Sn/ZSM-5 catalyst:effect of tin as a promoter[J].Catalysis Communications,2006,7(11):860-866.
[14]Li B,Xu Z,Chu W,et al. Ordered mesoporous Sn-SBA-15 as support for Pt catalyst with enhanced performance in propane dehydrogenation[J]. Chinese Journal of Catalysis,2017,38(4):726-735.
[15]Zhang Y,Zhou Y,Huang L,et al. Sn-modified ZSM-5 as support for platinum catalyst in propane dehydrogenation[J]. Industrial&Engineering Chemistry Research,2011,50(13):7896-7902.
[16]Luo H Y,Bui L,Gunther W R,et al. Synthesis and catalytic activity of Sn-MFI nanosheets for the baeyer-villiger oxidation of cyclic ketones[J]. Acs Catalysis,2014,2(12):2695-2699.
[17]Ren L,Guo Q,Kumar P,et al. Self-pillared,single-unitcell Sn-MFI zeolite nanosheets and their use for glucose and lactose isomerization[J]. Angewandte Chemie International Edtion,2015,54(37):10848-10851.
[18]Hong J C,Dornath P,Fan W. Synthesis of hierarchical SnMFI as lewis acid catalysts for isomerization of cellulosic sugars[J]. Acs Catalysis,2014,4(6):2029-2037.
[19]Su M,Li W,Zhang T,et al. Production of liquid fuel intermediates from furfural via aldol condensation over Lewis acid zeolite catalysts[J]. Catalysis Science&Technology,2017,7(16):3555-3561.
[20]Sun W,Wang X,Yang J,et al. Pervaporation separation of acetic acid-water mixtures through Sn-substituted ZSM-5zeolite membranes[J]. Journal of Membrane Science,2009,335(1):83-88.
[21]Deng L,Shishido T,Teramura K,et al. Effect of reduction method on the activity of Pt-Sn/Si O2,for dehydrogenation of propane[J]. Catalysis Today,2014,232(1):33-39.
[22]Talapaneni S N,Grand J,Thomas S,et al. Nanosized SnMFI zeolite for selective detection of exhaust gases[J].Materials&Design,2016,99:574-580.
[23]Vargas N G,Stevenson S,Shantz D F. Synthesis and characterization of tin(Ⅳ)MFI:sodium inhibits the synthesis of phase pure materials[J]. Microporous&Mesoporous Materials,2012,152(152):37-49.
[24]On D T,Kaliaguine S,Bonneviot L. Titanium boralites with MFI structure characterized using XRD,XANES,IR,and UV-Visible techniques:effect of hydrogen peroxide on the preparation[J]. Journal of Catalysis,1995,157(1):235-243.
[25]Aboul-Gheit A K,Aboul-Fotouh S M. Insight in cyclohexene hydroconversion process using catalysts containing0. 35%Pt on amorphous and zeolite supports[J]. Journal of the Taiwan Institute of Chemical Engineers,2012,43(5):711-717.
[26]Zhang Y,Zhou Y,Tang M,et al. Effect of La calcination temperature on catalytic performance of Pt Sn Na La/ZSM-5catalyst for propane dehydrogenation[J]. Chemical Engineering Journal,2012,181-182(1):530-537.