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Anodic oxidation of formic acid on PdAuIr /C-Sb_2O_5·SnO_2 electrocatalysts prepared by borohydride reduction
引用本文:A. O. Neto,J. Nandenha,R. F. B. De Souza,G. S Buzzo,J. C. M . Silva,E. V. Spinacé,M . H. M . T. Assumpo. Anodic oxidation of formic acid on PdAuIr /C-Sb_2O_5·SnO_2 electrocatalysts prepared by borohydride reduction[J]. 燃料化学学报, 2014, 42(7): 851-857
作者姓名:A. O. Neto  J. Nandenha  R. F. B. De Souza  G. S Buzzo  J. C. M . Silva  E. V. Spinacé  M . H. M . T. Assumpo
作者单位:Instituto de Pesquisas Energéticas e Nucleares-IPEN-CNEN/SP, Cidade Universitária, São Paulo 05508-900, Brazil
基金项目:the Laboratório de Microscopia do Centro de Ciências e Tecnologia de Materiais(CCTM) by TEM measurements,FAPESP(2011/18246-0,2012/03516-5) and CNPQ(150639/2013-9)for the financial support
摘    要:PdAuIr/C-Sb2O5·SnO2electrocatalysts with Pd∶Au∶Ir molar ratios of 90∶5∶5,70∶20∶10 and 50∶45∶5 were prepared by borohydride reduction method.These electrocatalysts were characterized by EDX,X-ray diffraction,transmission electron microscopy and the catalytic activity toward formic acid electro-oxidation in acid medium investigated by cyclic voltammetry(CV),chroamperometry(CA)and tests on direct formic acid fuel cell(DFAFC)at 100℃.X-ray diffractograms of PdAuIr/C-Sb2O5·SnO2electrocatalysts showed the presence of Pd fcc phase,Pd-Au fcc alloys,carbon and ATO phases,while Ir phases were not observed.TEM micrographs and histograms indicated that the nanoparticles were not well dispersed on the support and some agglomerates.The cyclic voltammetry and chroamperometry studies showed that PdAuIr/C-Sb2O5·SnO2(50∶45∶5)had superior performance toward formic acid electro-oxidation at 25℃compared to PdAuIr/C-Sb2O5·SnO2(70∶20∶10),PdAuIr/C-Sb2O5·SnO2(90∶5∶5)and Pd/C-Sb2O5·SnO2electrocatalysts.The experiments in a single DFAFC also showed that all PdAuIr/C-Sb2O5·SnO2electrocatalysts exhibited higher performance for formic acid oxidation in comparison with Pd/C-Sb2O5·SnO2electrocatalysts,however PdAuIr/C-Sb2O5·SnO2(90∶5∶5)had superior performance.These results indicated that the addition of Au and Ir to Pd favor the electro-oxidation of formic acid,which could be attributed to the bifunctional mechanism(the presence of ATO,Au and Ir oxides species)associated to the electronic effect(Pd-Au fcc alloys).

关 键 词:PdAuIr/C-Sb2O5·  SnO2electrocatalysts  formicacidoxidation  fuelcell  borohydridereductionprocess  
收稿时间:2013-12-06

Anodic oxidation of formic acid on PdAuIr/C-Sb2O5·SnO2 electrocatalysts prepared by borohydride reduction
A. O. Neto,J. Nandenha,R. F. B. De Souza,G. S Buzzo,J. C. M. Silva,E. V. Spinac,#,M. H. M. T. Assump,#,,#,o. Anodic oxidation of formic acid on PdAuIr/C-Sb2O5·SnO2 electrocatalysts prepared by borohydride reduction[J]. Journal of Fuel Chemistry and Technology, 2014, 42(7): 851-857
Authors:A. O. Neto  J. Nandenha  R. F. B. De Souza  G. S Buzzo  J. C. M. Silva  E. V. Spinac&#  M. H. M. T. Assump&#  &#  o
Affiliation:Instituto de Pesquisas Energéticas e Nucleares-IPEN-CNEN/SP, Cidade Universitária, São Paulo 05508-900, Brazil
Abstract:PdAuIr/C-Sb2O5·SnO2 electrocatalysts with Pd:Au:Ir molar ratios of 90:5:5, 70:20:10 and 50:45:5 were prepared by borohydride reduction method. These electrocatalysts were characterized by EDX, X-ray diffraction, transmission electron microscopy and the catalytic activity toward formic acid electro-oxidation in acid medium investigated by cyclic voltammetry (CV), chroamperometry (CA) and tests on direct formic acid fuel cell (DFAFC) at 100℃. X-ray diffractograms of PdAuIr/C-Sb2O5·SnO2 electrocatalysts showed the presence of Pd fcc phase, Pd-Au fcc alloys, carbon and ATO phases, while Ir phases were not observed. TEM micrographs and histograms indicated that the nanoparticles were not well dispersed on the support and some agglomerates. The cyclic voltammetry and chroamperometry studies showed that PdAuIr/C-Sb2O5·SnO2 (50:45:5) had superior performance toward formic acid electro-oxidation at 25℃ compared to PdAuIr/C-Sb2O5·SnO2 (70:20:10), PdAuIr/C-Sb2O5·SnO2 (90:5:5) and Pd/C-Sb2O5·SnO2 electrocatalysts. The experiments in a single DFAFC also showed that all PdAuIr/C-Sb2O5·SnO2 electrocatalysts exhibited higher performance for formic acid oxidation in comparison with Pd/C-Sb2O5·SnO2 electrocatalysts, however PdAuIr/C-Sb2O5·SnO2 (90:5:5) had superior performance. These results indicated that the addition of Au and Ir to Pd favor the electro-oxidation of formic acid, which could be attributed to the bifunctional mechanism (the presence of ATO, Au and Ir oxides species) associated to the electronic effect (Pd-Au fcc alloys).
Keywords:PdAuIr/C-Sb2O5·  SnO2 electrocatalysts  formic acid oxidation  fuel cell  borohydride reduction process  
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