用于丙烷催化燃烧的Pd_xPt_y-ZSM-5/Cordierite整体式催化剂
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摘要
以ZSM-5分子筛、铝溶胶、硝酸钯、硝酸铂和水为原料制备分子筛浆料,采用真空抽提-一次涂覆法在堇青石蜂窝陶瓷载体表面制备出Pd_xPt_y-ZSM-5/Cordierite整体式催化剂,考察了Pd负载量、ZSM-5分子筛的硅铝比和Pd/Pt质量比对整体式催化剂的丙烷催化燃烧性能的影响,并用超声波振荡、SEM、XRD、H_2-TPR和C_3H_8-TPD等手段对整体式催化剂进行了表征。当球磨时间为60 min,分子筛浆料固含量为38%时,整体式催化剂的涂层上载量可达到178 g·L~(-1),涂层脱落率低于0.5%。Pd_2Pt_3-ZSM-5/Cordierite整体式催化剂(贵金属总负载量为1.2g·L~(-1))对于丙烷的催化燃烧具有较好的催化活性(T_(50)=259℃,T_(90)=323℃)和稳定性,具有良好的工业应用前景,其中较低的ZSM-5分子筛硅铝比以及Pd和Pt之间的相互作用增加了对丙烷的吸附能力和表面活性氧物种的数量,从而提高了整体式催化剂的催化活性。
PdxPty-ZSM-5/Cordierite monolithic catalysts were prepared on the surface of the cordierite honeycomb supports, via vacuum extraction and one coating method, in which ZSM-5 molecular sieve, alumina sol, platinum or palladium nitrates and water were used as raw materials to prepare molecular sieve slurry. Effects of Pd loading, Si/Al ratio of ZSM-5, the mass ratio of Pd/Pt on the catalytic performance of the monolithic catalysts for the catalytic combustion of propane were investigated. The monolithic catalysts were characterized by ultrasonic oscillation,SEM, XRD, H_2-TPR and C_3H_8-TPD. When the ball milling time is 60 min and the molecular sieve slurry solid content is 38%, the coating amount of the monolith catalyst can reach 178 g·L~(-1), and the coating detachment rate is less than 0.5%. Pd_2Pt_3-ZSM-5/Cordierite catalyst(total loading of noble metals of 1.2 g · L~(-1)) exhibits better catalytic activity and stability(T_(50)=259℃, T_(90)=323℃) for the catalytic combustion of propane, which has better industrial application prospect. Lower Si/Al ratio of ZSM-5 and the interaction between Pd and Pt increase the amounts of adsorbed propane and surface active oxygen species, thus increases the catalytic performance of the monolithic catalyst.
PdxPty-ZSM-5/Cordierite monolithic catalysts were prepared on the surface of the cordierite honeycomb supports, via vacuum extraction and one coating method, in which ZSM-5 molecular sieve, alumina sol, platinum or palladium nitrates and water were used as raw materials to prepare molecular sieve slurry. Effects of Pd loading, Si/Al ratio of ZSM-5, the mass ratio of Pd/Pt on the catalytic performance of the monolithic catalysts for the catalytic combustion of propane were investigated. The monolithic catalysts were characterized by ultrasonic oscillation,SEM, XRD, H_2-TPR and C_3H_8-TPD. When the ball milling time is 60 min and the molecular sieve slurry solid content is 38%, the coating amount of the monolith catalyst can reach 178 g·L~(-1), and the coating detachment rate is less than 0.5%. Pd_2Pt_3-ZSM-5/Cordierite catalyst(total loading of noble metals of 1.2 g · L~(-1)) exhibits better catalytic activity and stability(T_(50)=259℃, T_(90)=323℃) for the catalytic combustion of propane, which has better industrial application prospect. Lower Si/Al ratio of ZSM-5 and the interaction between Pd and Pt increase the amounts of adsorbed propane and surface active oxygen species, thus increases the catalytic performance of the monolithic catalyst.
引文
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[2]Huang B B,Lei C,Wei C H,et al.Chlorinated volatile organic compounds(Cl-VOCs)in environment-sources,potential human health impacts,and current remediation technologies[J].Environment International,2014,71(4):118-138.
[3]Liotta L F.Catalytic oxidation of volatile organic compounds on supported noble metals[J].Applied Catalysis B:Environmental,2010,100(3/4):403-412.
[4]Li W B,Wang J X,Gong H.Catalytic combustion of VOCs on non-noble metal catalysts[J].Catalysis Today,2009,148(1/2):81-87.
[5]Zhang Z,Jiang Z,Shangguan W.Low-temperature catalysis for VOCs removal in technology and application:a state-of-the-art review[J].Catalysis Today,2016,264:270-278.
[6]Kamal M S,Razzak S A,Hossain M M.Catalytic oxidation of volatile organic compounds(VOCs)-a review[J].Atmospheric Environment,2016,140:117-134.
[7]Xie Y J,Yu Y Y,Gong X Q,et al.Effect of the crystal plane figure on the catalytic performance of MnO2for the total oxidation of propane[J].CrystEngComm,2015,17(15):3005-3014.
[8]Xie Y J,Guo Y,Guo Y L,et al.A highly effective Ni-modified MnOx catalyst for total oxidation of propane:the promotional role of nickel oxide[J].RSC Advances,2016,6(55):50228-50237.
[9]Xie Y J,Guo Y,Guo Y L,et al.A highly-efficient La-MnOx catalyst for propane combustion:the promotional role of La and the effect of the preparation method[J].Catalysis Science&Technology,2016,6(23):8222-8233.
[10]Hu Z,Qiu S,You Y,et al.Hydrothermal synthesis of NiCeOx nanosheets and its application to the total oxidation of propane[J].Applied Catalysis B:Environmental,2018,225:110-120.
[11]Hu Z,Wang Z,Guo Y,et al.Total oxidation of propane over a Ru/CeO2catalyst at low temperature[J].Environmental Science&Technology,2018,52(16):9531-9541.
[12]Okal J,Zawadzki M,Tylus W.Microstructure characterization and propane oxidation over supported Ru nanoparticles synthesized by the microwave-polyol method[J].Applied Catalysis B:Environmental,2011,101(3/4):548-559.
[13]Okal J,Zawadzki M.Combustion of propane over novel zinc aluminate-supported ruthenium catalysts[J].Applied Catalysis B:Environmental,2011,105(1/2):182-190.
[14]Zhu Z Z,Lu G Z,Zhang Z G,et al.Highly active and stable Co3O4/ZSM-5 catalyst for propane oxidation:effect of the preparation method[J].ACS Catalysis,2013,3(6):1154-1164.
[15]Hu Z,Liu X F,Meng D M,et al.Effect of ceria crystal plane on the physicochemical and catalytic properties of Pd/ceria for COand propane oxidation[J].ACS Catalysis,2016,6(4):2265-2279.
[16]Zhu Z Z,Lu G Z,Guo Y,et al.High performance and stability of the Pt-W/ZSM-5 catalyst for the total oxidation of propane:the role of tungsten[J].Chemcatchem,2013,5(8):2495-2503.
[17]Avila M S,Vignatti C R,Apesteguía C R,et al.Effect of support on the deep oxidation of propane and propylene on Pt-based catalysts[J].Chemical Engineering Journal,2014,241:52-59.
[18]Park J E,Kim K B,Seo K W,et al.Propane combustion over supported Pt catalysts[J].Research on Chemical Intermediates,2011,37(9):1135-1143.
[19]Maillet T,Solleau C,Barbier J Jr,et al.Oxidation of carbon monoxide,propene,propane and methane over a Pd/Al2O3catalyst.Effect of the chemical state of Pd[J].Applied Catalysis BEnvironmental,1997,14(1/2):85-95.
[20]Maillet T,Barbier J Jr,Duprez D.Reactivity of steam in exhaust gas catalysis(Ⅲ):Steam and oxygen/steam conversions of propane on a Pd/Al2O3catalyst[J].Applied Catalysis B Environmental,1996,9(1/2/3/4):251-266.
[21]Yazawa Y,Takagi N,Yoshida H,et al.The support effect on propane combustion over platinum catalyst:control of the oxidation-resistance of platinum by the acid strength of support materials[J].Applied Catalysis A General,2002,233(1/2):103-112.
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[23]单学蕾,关乃佳,曾翔,等.不同硅铝比的Cu-ZSM-5/堇青石整体式催化剂的NO分解反应性能[J].催化学报,2001,22(3):242-244.Shan X L,Guan N J,Zeng X,et al.NO decomposition on CuZSM-5/cordierite monolithic catalyst samples with different Si/Al ratios[J].Chinese Journal of Catalysis,2001,22(3):242-244.
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[25]Deugd R M D,Kapteijn F,Moulijn J A.Using monolithic catalysts for highly selective Fischer-Tropsch synthesis[J].Catalysis Today,2003,79/80(3):495-501.
[26]Schneider R,Kie?ling D,Wendt G.Cordierite monolith supported perovskite-type oxides-catalysts for the total oxidation of chlorinated hydrocarbons[J].Applied Catalysis B:Environmental,2000,28(3/4):187-195.
[27]Colman-Lerner E,Peluso M A,Sambeth J,et al.Cerium,manganese and cerium/manganese ceramic monolithic catalysts.Study of VOCs and PM removal[J].Journal of Rare Earths,2016,34(7):675-682.
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[29]Mitra B,Kunzru D.Washcoating of different zeolites on cordierite monoliths[J].Journal of the American Ceramic Society,2008,91(1):64-70.
[30]Carvalho L S,Pieck C L,Rangel M C,et al.Trimetallic naphtha reforming catalysts(I):Properties of the metal function and influence of the order of addition of the metal precursors on PtRe-Sn/γ-Al2O3-Cl[J].Applied Catalysis A:General,2004,269(1/2):91-103.
[31]Zhu Z Z,Lu G Z,Guo Y,et al.Influences of Pd precursors and preparation method on the catalytic performances of Pd-only close-coupled catalysts[J].Journal of Industrial and Engineering Chemistry,2012,18(6):2135-2140.
[32]Elangovan S P,Ogura M,Ernst S,et al.A comparative study of zeolites SSZ-33 and MCM-68 for hydrocarbon trap applications[J].Microporous&Mesoporous Materials,2006,96(1/2/3):210-215.