OMS-2负载Pt催化剂的制备及其催化氧化性能研究
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摘要
采用前掺杂法、沉积-沉淀法和浸渍法制备了氧化锰八面体分子筛(OMS-2)负载Pt催化剂(Pt/OMS-2),对所制催化剂进行了结构和织构表征。并研究了不同制备方法和沉积-沉淀法中不同制备(Pt负载量和溶液的pH值)对Pt/OMS-2催化氧化CO性能的影响。结果表明,沉积-沉淀法制备的Pt/OMS-2-DP催化剂活性最好(T100=100℃)。这与Pt/OMS-2-DP催化剂中Pt颗粒大小及OMS-2载体与Pt之间存在强相互作用有关。Pt负载量明显影响Pt/OMS-2-DP催化剂的催化活性,3Pt/OMS-2-DP催化剂(Pt=3.0 wt%)催化活性最高,这是由于适当Pt负载量,Pt颗粒较小,并与载体OMS-2的相互作用较强,能较好地活化OMS-2晶格氧。pH值对Pt/OMS-2-DP催化剂催化性能影响较大,这与OMS-2的等电点和Pt在不同溶液中存在不同Pt配位体形式有关。
Pt/OMS-2 catalysts were prepared by pre-incorporation(PI),typical wet impregnation(IM) and depositionprecipitation(DP) methods.Influences of preparation methods,Pt loading and pH values of preparation solution on the catalytic activity of CO oxidation were studied.The samples were characterized by X-ray diffraction(XRD) and N2adsorption/desorption.Results showed that as compared with typical wet impregnation method and pre-incorporation methods,Pt/OMS-2-DP prepared from deposition-precipitation method revealed higher activity,due to the smaller particle size and stronger interaction between Pt and OMS-2.The catalyst activity for catalytic oxidation of CO increased with an increases of Pt loading and passed through a maximum in activity at 3.0wt% Pt.Pt/OMS-2-DP catalyst,prepared at pH 8 solution,showed a significant improvement of catalytic activity,this may be due to interaction between OMS and Pt,which keep smaller particle size over OMS-2 support.
Pt/OMS-2 catalysts were prepared by pre-incorporation(PI),typical wet impregnation(IM) and depositionprecipitation(DP) methods.Influences of preparation methods,Pt loading and pH values of preparation solution on the catalytic activity of CO oxidation were studied.The samples were characterized by X-ray diffraction(XRD) and N2adsorption/desorption.Results showed that as compared with typical wet impregnation method and pre-incorporation methods,Pt/OMS-2-DP prepared from deposition-precipitation method revealed higher activity,due to the smaller particle size and stronger interaction between Pt and OMS-2.The catalyst activity for catalytic oxidation of CO increased with an increases of Pt loading and passed through a maximum in activity at 3.0wt% Pt.Pt/OMS-2-DP catalyst,prepared at pH 8 solution,showed a significant improvement of catalytic activity,this may be due to interaction between OMS and Pt,which keep smaller particle size over OMS-2 support.
引文
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[26]Jothiramalingam R,Wang M K.Synthesis,characterization and photocatalytic activity of porous manganese oxide doped titania for toluene decomposition[J].Journal of Hazardous Materials,2007,147(1-2):562-569.
[2]李巧霞,周小金,李金光,等.Pt-Ru合金薄膜的电沉积制备及其电化学表面增强红外吸收光谱[J].物理化学学报,2010,26(6):1488-1492.
[3]刘英骏,张继军,李能,等.CO 2对Cu-Ce-O催化剂催化氧化CO活性的影响[J].物理化学学报,1999,15(2):97-100.
[4]夏熙.二氧化锰及相关锰氧化物的晶体结构、制备及放电性能(1)[J].电池,2004,34(6):411-414.
[5]Xia G G,Yin Y G,Willis W S,et al.Efficient stable cata-lysts for low temperature carbon monoxide oxidation[J].Journal of Catalysis,1999,185(1):91-105.
[6]Gac W.The influence of silver on the structural,redox and catalytic properties of the cryptomelane-type manganese ox-ides in the low-temperature CO oxidation reaction[J].Ap-plied Catalysis B:Environment,2007,75(1-2):107-117.
[7]Carno J,Ferrandon M,Bjornbom E E,et al.Mixed man-ganese oxide/platinum catalysts for total oxidation of model gas from wood boilers[J].Applied Catalysis A:General,1997,155:265-281.
[8]Ayastuy J L,Gonza M P,Gonza′lez-Velasco J R,et al.MnO x/Pt/Al 2 O 3 catalysts for CO oxidation in H 2-rich streams[J].Applied Catalyssis B:Environment,2007,70:532-541.
[9]赵红晓,王淑敏,张雷勇,等.Pt-MnO 2/C的制备及对乙醇电催化活性的研究[J].电源技术研究与设计,2009,33(2):98-112.
[10]Mergler Y J,Aalst A V,Delft J V,et al.CO oxidation over promoted Pt catalysts[J].Applied Catalysis A:General,1996,10:245-261.
[11]Hu Rong-rong,Cheng Yi,Xie Lan-ying,et al.Effect of doped Ag on performance of manganese oxide octahedral molecular sieve for CO oxidation[J].Chinese Journal of Catalysis,2007,28(5):463-468.
[12]Tang Xing-fu,Li Yong-gang,Chen Jun-li,et al.Synthesis,characterization and catalytic application of titanium-cryp-tomelane nanorods/fibers[J].Microporous and Mesoporous Materails,2007,103(1-3):250-256.
[13]Wang Z M,Tezuka S,Kanoh H.Characterization of the structural and surface properties of a synthesized hydrous hollandite by gaseous molecular adsorption[J].Chemistry of Materails,2001,13(2):530-537.
[14]Burcu S C,Soykal I I,Aksoylu A.Preferential oxidation of CO over Pt-Sn/AC catalyst:adsorption,performance and drifts studies[J].Applied Catalysis B:Environmental,2011,106(7):540-549.
[15]Trimm D L,Onsan Z I.Onboard fuel convision for hydro-gen-fuel-cell-driven vehicles[J].Catalysis Review:Science and Engineering,2001,43(1-2):31-84.
[16]Garrido G I,Patcas F C,Upper G,et al.Supercritical depo-sition of Pt on SnO 2-coated Al 2 O 3 foams:phase behaviour and catalytic performance[J].Applied Catalysis,A:Gener-al,2008,338(1-2):58-65.
[17]Grass K,Lintz H G.The Kinetics of carbon monoxide oxi-dation on Tin(Ⅳ)oxide supported platinum catalysts[J].Journal of Catalysis,1997,172(2):446-452.
[18]Haruta M,Dat′e M.Advances in the catalysis of Au nanoparticles[J].Applied Catalysis A:General,2001,222(1-2):427-437.
[19]Haruta M,Tsubota S,Kobayashi T,et al.Low-temperture oxidation of CO over gold supported on TiO 2,α-Fe 2 O 3 and CO 3 O 4[J].Journal of Catalysis,1993,144:175-192.
[20]Chen Xiao,Shen Yan-fei,Suib S L,et al.Characterization of manganese oxide octahedral molecular sieve(M-OMS-2)materials with different metal cation dopants[J].Chem-istry of Materials,2002,14(2):940-948.
[21]王东辉,程代云,郝郑平,等.纳米金催化剂及其应用[M].北京:国防工业出版社,2006.
[22]Sillen L G,Martell A E.The stability constants of metal ion complexes[J].The Chemical Society,1971,25(S1).
[23]Kosmulski M.pH-dependent surface charging and points of zero charge II.Update[J].J Colloid Interface Science,2004,275(1):214-224.
[24]Zhang Z C,Beard B C.Agglomeration of Pt particles in the presence of chlorides[J].Applied Catalysis A,General,1999,188:229-240.
[25]Liu J,Makwana V,Cai J,et al.Effects of alkali metal and ammonium cation templates on nanofibrous cryptomelane-type manganese oxide octahedral molecular sieves(OMS-2)[J].Journal of Physics Chemistry B,2003,107(35):9185-9194.
[26]Jothiramalingam R,Wang M K.Synthesis,characterization and photocatalytic activity of porous manganese oxide doped titania for toluene decomposition[J].Journal of Hazardous Materials,2007,147(1-2):562-569.
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