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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2011,Vol.27>> Issue(08)>> 1868-1874     doi: 10.3866/PKU.WHXB20110803         中文摘要
ELECTROCHEMISTRY AND NEW ENERGY
Preparation of ‘Sandwich-Like’ Au/Pt Composite Multilayer Films for Methanol Electrooxidation
ZHAO Jing, SUN Yue, LI Yong-Jun, LIANG Ren
Department of Chemisty, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, P. R. China
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Pt/Au composite monolayer films were fabricated by combining interfacial assembly and under-potential deposition (UPD) with redox replacement. Based on the Pt/Au composite monolayers, an organic linker-free method was proposed for the fabrication of sandwich-like Pt/Au composite multilayer films: (Pt/Au)n, Ptm/Au, and (Pt3/Au)k (n, m, or k represents the layer number). Electron microscopy was used to characterize the morphologies of the Au monolayer films and the Pt/Au composite multilayer films. For each type of composite multilayer films, a common characteristic was that the effective electroactive areas increased with an increase in the layer number. Additionally, the electrocatalytic activities of the composite multilayer films for methanol electrooxidation are systematically discussed by examining the catalytic current densities and its tolerance toward carbonaceous species. For the same series of composite multilayer films (Pt/Au)3, Pt3/Au, and (Pt3/Au)2 showed a higher catalytic current density than bulk Pt (Ptbulk). Among the three composite multilayer films, (Pt/Au)3 showed the best catalytic performance in terms of the current density and tolerance toward carbonaceous species. The tolerance of (Pt/Au)3 to carbonaceous species was found to be better than that of the commercial Pt/C catalyst. This better electrocatalytic activity may be attributed to the maximum synergistic effect between Au and Pt, which depends on the Pt:Au atomic ratio and also the arrangement of Pt and Au nanoparticles.



Keywords: Interfacial self-assembly   Under-potential deposition   Au/Pt composite multilayer film   Electrooxidation   Methanol  
Received: 2011-04-11 Accepted: 2011-05-31 Publication Date (Web): 2011-06-08
Corresponding Authors: LI Yong-Jun Email: liyongjunef@gmail.com

Fund: The project was supported by the National Natural Science Foundation of China (20703016), Scientific and Technological Projects of Hunan Province, China (2010FJ6030) and State Key Laboratory for Physical Chemistry of Solid Surface (Xiamen University), China.

Cite this article: ZHAO Jing, SUN Yue, LI Yong-Jun, LIANG Ren. Preparation of ‘Sandwich-Like’ Au/Pt Composite Multilayer Films for Methanol Electrooxidation[J]. Acta Phys. -Chim. Sin., 2011,27 (08): 1868-1874.    doi: 10.3866/PKU.WHXB20110803

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64. MAO Dong-Sen, GUO Qiang-Sheng, MENG Tao.Effect of Magnesium Oxide Modification on the Catalytic Performance of Nanoscale HZSM-5 Zeolite for the Conversion of Methanol to Propylene[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2242-2248
65. ZHAO Yan-Chun, LAN Huang-Xian, DENG Bin-Bin, TIAN Jian-Niao, YANG Xiu-Lin, WANG Feng-Yang.Electrocatalytic Oxidation of Methanol with Poly Functionalized Multiwalled Carbon Nanotubes Supported Pt Catalysts[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2255-2260
66. ZHAO Rong-Li, LIN Ke, ZHOU Xiao-Guo, LIU Shi-Lin.Solubility of Poly(N-isopropylacrylamide) in Aqueous Methanol from Raman Spectroscopy[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1915-1922
67. ZHANG Sheng-Hong, ZHANG Hong-Peng, LI Wei-Zhen, ZHANG Wei, HUANG Hua, LIU Hai-Chao.Effects of Zirconia Crystallite Phases on the Structures of MoOx/ZrO2 Catalysts and Their Properties in the Selective Oxidation of Methanol[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1879-1886
68. LI Yong-Jun, ZHOU You-Chen, SUN Shi-Gang.Preparation of Core-Shell SiO2/Pt Particles via Layer-by-Layer Assembly and Their Electrooxidation and In-situ Electrochemical FTIR Spectra for CO[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1773-1778
69. AN Xiao-Sha, CHEN De-Jun, ZHOU Zhi-You, WANG Qiang, FAN You-Jun, SUN Shi-Gang.Rare Earth Eu Doped PtRu/C Catalysts and Their Properties for Methanol Electrooxidation[J]. Acta Phys. -Chim. Sin., 2010,26(05): 1207-1213
70. LIU Bo-Jie, LI Xue-Yi, CHEN Wei, LIU Ren-Xiao, GE Guang-Lu.Surface Ligand Exchange and Phase Transfer of Iron Oxide Magnetic Nanoparticles[J]. Acta Phys. -Chim. Sin., 2010,26(03): 784-788
71. WU Yan-Ni, LIAO Shi-Jun.Shortened Carbon Nanotubes as Supports to Prepare High-Performance Pt/SCNT and PtRu/SCNT Catalysts for Fuel Cells[J]. Acta Phys. -Chim. Sin., 2010,26(03): 669-674
72. MAO Dong-Sen, GUO Qiang-Sheng, MENG Tao, LU Guan-Zhong.Effect of Hydrothermal Treatment on the Acidity and Catalytic Performance of Nanosized HZSM-5 Zeolites for the Conversion of Methanol to Propene[J]. Acta Phys. -Chim. Sin., 2010,26(02): 338-344
73. ZHAO Yan-Chun, LAN Huang-Xian, TIAN Jian-Niao, YANG Xiu-Lin, WANG Feng-Yang.Electrocatalytic Oxidation of Methanol on Pt Nanoparticles Supported on Porous Poly(N-acetylaniline) Nanofibrils[J]. Acta Phys. -Chim. Sin., 2009,25(10): 2050-2054
74. FANG Xiang, SHEN Pei-Kang.Mechanism of Ethanol Electrooxidation on Pd Electrode[J]. Acta Phys. -Chim. Sin., 2009,25(09): 1933-1938
75. GAO Yun-Fang, YU Li-Li| LU Qing-Qing, MA Chun-An.Electrochemical Oxidation Behavior of Iodide on Platinum Electrode in Acid Solution[J]. Acta Phys. -Chim. Sin., 2009,25(07): 1421-1426
76. NI Zhe-Ming, MAO Jiang-Hong, PAN Guo-Xiang, XU Qian, LI Xiao-Nian.Mechanism of Palladium-Catalyzed Methanol Decomposition for Hydrogen Production[J]. Acta Phys. -Chim. Sin., 2009,25(05): 876-882
77. YANG Hong-Yan, GUO Pan-Pan, LI Wei-Shan.Electrodeposition Preparation and Activity of CO-Resistant Catalyst Pt-HxWO3 for Methanol Oxidation[J]. Acta Phys. -Chim. Sin., 2009,25(04): 719-723
78. WANG Jian-She, GUO Xun, SONG Cheng-Ying, WANG Liu-Cheng, ZHAO Jian-Hong, QIU Xin-Ping.Promoting Methanol Electro-Oxidation through Fabricating Pore Structure in Pt/CNTs Catalyst Layer by Dissolving Away Premixed La2O3 Particles[J]. Acta Phys. -Chim. Sin., 2009,25(04): 767-772
79. XU Lei; WU Shu-Jie; ZHANG Wen-Xiang; JIA Ming-Jun; LIU Gang.Vapour Phase ortho-Selective Alkylation of Phenol with Methanol over Fe-Zr Oxide Catalysts[J]. Acta Phys. -Chim. Sin., 2009,25(02): 242-246
80. LI Lai-Cai; WANG Yi-Wei; TIAN An-Min.Adsorption of Methanol on the Pt-Mo(111)/C Surface[J]. Acta Phys. -Chim. Sin., 2008,24(11): 2013-2018
81. PAN Lei-Ming, ZHOU Zhi-You, CHEN De-Hun, SUN Shi-Gang.Electrochemical and In Situ FTIR Studies of Adsorption and Oxidation of Dimethyl Ether on Platinum Electrode[J]. Acta Phys. -Chim. Sin., 2008,24(10): 1739-1744
82. CHANG Xiao-Tu, WANG Jian-Ming, SHAO Hai-Bo, WANG Jun-Bo, ZENG Xiao-Xu, ZHANG Jian-Qing, CAO Chu-Nan.Corrosion and Anodic Behaviors of Pure Aluminumin a Novel Alkaline Electrolyte[J]. Acta Phys. -Chim. Sin., 2008,24(09): 1620-1624
83. ZHENG Bo; LI He-Xian; WANG Guo-Chang; LIU Kun; YUAN Wei; LI He; LIANG Bo.Supramolecular Complexation in Water-Methanol Mixtures[J]. Acta Phys. -Chim. Sin., 2008,24(08): 1503-1506
84. ZHENG Gen-Wen; GONG Chun-Li; WEN Sheng; XIE Xiao-Lin.Preparation and Performances of Sulfonated Poly(ether imide) and Poly (ether sulfone) Blends for Proton Exchange Membrane[J]. Acta Phys. -Chim. Sin., 2008,24(05): 855-860
85. LIANG Ying; LIAO Dai-Wei.Effects of pH on the PtRu/C Catalyst Prepared by Microwave-assisted Ethylene Glycol Process[J]. Acta Phys. -Chim. Sin., 2008,24(02): 317-322
86. DENG Hui-Ning; WANG Yu-Xin.Preparation and Properties of Proton Conducting Composite Membranes from Sulfonated Poly(phthalazinone ether keton) and Phosphotungstic Acid[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1235-1240
87. XU Hui-Yuan; CHU Wei; CI Zhi-Min.Effect of Glow Discharge Plasma on Copper-based Catalysts for Methanol Synthesis[J]. Acta Phys. -Chim. Sin., 2007,23(07): 1042-1046
88. ZHENG Hai-Tao; LI Yong-Liang; LIANG Jian-Ying; SHEN Pei-Kang.Methanol Oxidation on Pd-based Electrocatalysts[J]. Acta Phys. -Chim. Sin., 2007,23(07): 993-996
89. YAN Zong-Cheng; CHEN Li; WANG Hong-Lin.Glow Discharge Plasma Electrolysis of Methanol Solutions[J]. Acta Phys. -Chim. Sin., 2007,23(06): 835-840
90. LI Lan-Lan; WEI Zi-Dong; YAN Can; LUO Yi-Hui; YIN Guang-Zhi; SUN Cai-Xin.Methanol Oxidation on a Pt ElectrodeModified by Underpotential Deposition of Ru[J]. Acta Phys. -Chim. Sin., 2007,23(05): 723-727
91. ZHAO Wen-Xia; HU Man-Cheng; LI Shu-Ni; JIANG Yu-Cheng; ZHANG Xiao-Lei; HU Lei; CHEN Huai-Jun.The Solubility of Ternary SystemRbBr/CsBr-CH3OH/C2H5OH-H2O at Different Temperatures[J]. Acta Phys. -Chim. Sin., 2007,23(05): 695-700
92. WU Wei; CAO Jie-Ming; CHEN Yu; LU Tian-Hong.Preparation of High-alloying Pt-Ru/CMK-3 Catalysts in THF-H2O-EtOH Ternary Solution System[J]. Acta Phys. -Chim. Sin., 2007,23(04): 559-564
93. ZHANG Cheng-Gen;LI Wen-Zuo;HUANG Ming-Bao.Reaction of Methyl Alcohol with Thionyl Chloride in Solution[J]. Acta Phys. -Chim. Sin., 2007,23(03): 399-403
94. ZHANG Shu-Dong;ZHU Xiang-Jun;WANG Yan;KONG Xiang-He.Multiphoton Ionization Mass Spectrum of Methanol Clusters and Ab Initio Calculations[J]. Acta Phys. -Chim. Sin., 2007,23(03): 379-383
95. DENG Hui-Ning;WANG Yu-Xin .Sulfonated Poly(phthalazinones) Membranes For Direct Methanol Fuel Cell[J]. Acta Phys. -Chim. Sin., 2007,23(02): 187-191
96. HUANG Mian-Yan;CHEN Hua-Yan;GUO Jian-Zhao;WANG Zhi-Tao;XU Li;WANG Yu-Xin.Methanol Resistant Poly(Ether Sulfone)/Sulfonated Poly(Ether Ether Ketone) Blend Proton Exchange Membrane for DMFC[J]. Acta Phys. -Chim. Sin., 2007,23(01): 44-49
97. SHEN Pei-Kang;WANG Sheng-Long;HU Zhi-Yi;LI Yong-Liang;ZENG Rong;HUANG Yue-Qiang.Hydrogen Production by Alcohol Electrolysis[J]. Acta Phys. -Chim. Sin., 2007,23(01): 107-110
98. CHU Dao-Bao;YIN Xiao-Juan;FENG De-Xiang;LIN Hua-Shui;TIAN Zhao-Wu.Electrocatalytic Oxidation of Ethanol on Pt/nanoTiO2-CNT Complex Catalysts[J]. Acta Phys. -Chim. Sin., 2006,22(10): 1238-1242
99. ZHANG Xue-Hong;TANG Xing-Hua;CHENG Xin-Sun.Synthesis and Application of Ce-doped Mesoporous TiO2[J]. Acta Phys. -Chim. Sin., 2006,22(05): 532-537
100. LI Li;WU Gang;YE Qing;DENG Wei;XU Bo-Qing.Electrochemical Modification of Pt/C Catalyst by Silicomolybdic Acid[J]. Acta Phys. -Chim. Sin., 2006,22(04): 419-423
101. CHEN Ling; WANG Xin-dong; GUO Min.The Effect of NdOx as Co-catalyst for the Electro-oxidation of Methanol on PtRu/C[J]. Acta Phys. -Chim. Sin., 2006,22(02): 141-145
102. CHEN Yu; TANG Ya-wen; Kong Ling-yong; LIU Chang-peng; XING Wei; LU Tianhong.Effect of Surface Modification Extent of Carbon Nanotubes on Electrocatalytic Performance of Carbon Nanotubes Supported Pt catalyst[J]. Acta Phys. -Chim. Sin., 2006,22(01): 119-123
103. LIN Heng; CHEN Guo-liang; ZHENG Zi-shan; ZHOU Jian-zhang; CHEN Sheng-pei; LIN Zhong-hua.The Adsorption and Oxidation of Isopropanol at Platinum Electrode in Alkaline Media[J]. Acta Phys. -Chim. Sin., 2005,21(11): 1280-1284
104. ZHONG Qi-ling ; ZHANG Xiao-hong; ZHOU Hai-Hui; WEN Zu-biao; YANG Xiong-yuan; HUANG Peng; REN Bin; TIAN Zhong-qun.In-situ SERS of Piperonal and Isosafrole Electrooxidation on Pt Electrode[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1182-1185
105. WANG Zhen-bo; YIN Ge-ping; SHI Peng-fei.The Influence of Three Groups of Pt-Ru/C Catalyst’s Precursors on Its Performance for Direct Methanol Fuel Cell[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1156-1160
106. LI Li; XU Bo-qing.Electrooxidation of CO Adsorbed on PtMo/C Catalyst:Effect of Catalyst Preparation[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1132-1137
107. QU Wei-li; WU Bing; SUN Fang; GAO Ying; LU Tian-hong; LIU Chang-peng; XING Wei.Electrocatalytic Oxidation of Ethylene Glycol at Pt-WO3/C Electrode[J]. Acta Phys. -Chim. Sin., 2005,21(07): 804-807
108. ZHANG Wen-yu; DONG Qing-nian; ZHAO Ning; WEI Wei; SUN Yu-han.The Reaction Mechanism for the Synthesis of 1-methoxy-2-propanol on MgO Catalyst[J]. Acta Phys. -Chim. Sin., 2005,21(06): 653-657
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110. JIA Yu-Xiang; GUO Xiang-Yun.Monte Carlo Simulation of Adsorption Process of CO and H2 in Supercritical Fluids[J]. Acta Phys. -Chim. Sin., 2005,21(03): 306-309
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112. Zhong Qi-Ling;Zhang Bin;Zhang Lei;Yang Xiong-Yuan;Huang Peng.In-situ SERS of Dissociative Adsorption and Oxidation of Ethanol on Roughed Platinum Electrodes[J]. Acta Phys. -Chim. Sin., 2004,20(09): 1163-1166
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114. Hu Ji-Ming;Zhang Jian-Qing;Zhang Jin-Tao;Cao Chu-Nan.Electrochemical Activities of IrO2 Electrodes in Small Organic Molecules Containing Aqueous Solutions[J]. Acta Phys. -Chim. Sin., 2004,20(07): 740-744
115. Yun Hong;Chen Jian-Hua;Zhang Hui;Lin Jing-Dong;Chen Hong-Bo;Lin Chang-Jian.The Effects of ZrO2 on Cu-ZnO-ZrO2 Catalysts for Hydrogen Generation by Steam Reforming of Methanol[J]. Acta Phys. -Chim. Sin., 2004,20(05): 550-553
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130. Yang Cheng;Dong Qing-Nian;Zhang Jing;Ren Jie;Sun Yu-Han;Xie Ya-Ning;Hu Tian-Dou.The Structural Effect of CeO2 and La2O3 Modified Pd/γ-Al2O3 Catalysts[J]. Acta Phys. -Chim. Sin., 2002,18(02): 170-174
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