직접 에탄올 연료전지용 백금합금촉매의 합성과 특성 분석
Synthesis and Characterization of Pt based Alloy Catalysts for Direct Ethanol Fuel Cell
0
조회
0
다운로드
1
인용
0
참고문헌
키워드
초록
에탄올이 이산화탄소가 생성되는 경로로 반응할 경우 12개의 전자를 발생시키게 되지만 실제로는 두 개의 탄소 원자사 이의 결합력 때문에 완전 산화시키는 것이 쉽지 않다. 따라서 고성능 에탄올 산화촉매의 개발은 에탄올 연료전지 실용 화에 필수적이다. 본 연구는 Pt에 Sn, Au을 첨가하여 이원계, 삼원계 촉매를 제조하여 에탄올에서의 활성과 촉매의 특 성에 대한 분석을 수행하였다. 촉매합성은 modified polyol 방법을 이용하였으며 Vulcan XC-72R 담지체를 사용하여 20 wt%로 담지하였다. PtSn/C 합금촉매는 Pt : Sn의 비율이 1 : 0, 4 : 1, 3 : 1, 2 : 1, 1.5 : 1, 1 : 1, 1 : 1.5 으로 합성하였으며, PtSnAu/C 합금촉매는 Pt : Sn :Au의 비율을 5 : 5 : 0, 5 : 4 : 1, 5 : 3 : 2, 5 : 2 : 3 으로 합성하였다. 촉매특성은 XRD, TEM 분석을 통해 분석한 결과 1.9~2.4 nm 정도의 입자의 크기와 면심입방구조의 구조를 가지는 것으로 확인하였다. 에탄올 산화에 대한 합금촉매의 활성은 순환전류전압법으로 실험하였고, 그 중 가장 높은 성능을 가진 PtSn(1.5 : 1)/C 와 PtSnAu(5 : 2 : 3)/C 합금촉매를 단위전지 성능평가를 통해 실제 연료전지 구동환경에서 촉매의 활성을 측정하였다. 그 결과 에탄올 산화에 가장 높은 성능을 나타낸 촉매는 PtSn/C(1.5 : 1)이었고, 촉매의 안정성은 PtSnAu/C(5 : 2 : 3)에 서 높게 나타났다
Abstract
Though ethanol can theoretically generate 12 electrons during oxidation to carbon dioxide, the complete oxidationopment of high activity catalyst for ethanol oxidation is necessary for the commercialization of direct ethanol fuel cel.In this study, some binary and ternary electrocatalysts of PtSn/C and PtSnAu/C have been synthesized and characterized.The catalysts were fabricated with modified polyol method with the amounts of 20 wt%, where the Pt:Sn ratios inthe PtSn/C were 1 : 0, 4 : 1, 3 : 1, 2 : 1, 1.5 : 1, 1 : 1, 1 : 1.5 and Pt:Sn:Au ratios in the PtSnAu/C were 5 : 5 : 0, 5 : 4 : 1,5 : 3 : 2, 5 : 2 : 3. From the XRD and TEM analysis results, the catalysts were found to have face centered cubic structurewith particle size of around 1.9~2.4 nm. The activity in the ethanol oxidation was examined with cyclic voltammetryand the results indicated that PtSn(1.5 : 1)/C and PtSnAu(5:2:3)/C had the highest activity in each catalyst system. Fur-formance while the long term stability of PtSnAu/C(5:2:3) is beter than PtSn/C(1.5 : 1).
참고문헌 (21)
- J. Larminie, "Fuel cell systems explained", pp.28~ (2003), John Wiley & Sons
- N. R. de Tacconi, "Insitu FTIR study of the electrocatalytic oxidation of ethanol at iridium and rhodium electrodes", J. Electroanal. Chem, 379, pp.329~ (1994)
- G. A. Camara, "Parallel pathways of ethanol oxidation: The effect of ethanol concentration", J. Electroanal. Chem, 578, pp.315~ (2005)
- S. Song, "The effect of methanol and ethanol cross-over on the performance of PtRu", C-based anode DAFCs, 2005, pp.55, 65~
- S. S. Gupta, "A comparative study on ethanol oxidation behavior at Pt and PtRh electrodeposits", J. Electroanal. Chem, 594, pp.65~ (2006)
- C. Lamy, "Electrocatalytic oxidation of aliphatic alcohols: Application to the direct alcohol fuel cell(DAFC)", J. Appl. Electrochem, 31, pp.799~ (2001)
- W. J. Zhou, "Direct ethanol fuel cells based on PtSn anodes: the effect of Sn content on the fuel cell performance", J. Power Sources, 140, pp.50~ (2005)
- S. W. Ho, "Effects of ethanol impregnation on the properties of silica-supported cobalt catalysts", J. Catalysis, 168, pp.51~ (1997)
- T. S. Ahmadi, "Shape-controlled synthesis of colloidal platinum nanoparticles", Science, 272, pp.1924~ (1996)
- W. Zhoua, "Pt based anode catalysts for direct ethanol fuel cells", Appl. catal. B: Envir, 46, pp.273~ (2003)
- Z. Zhou, "Novel synthesis of highly active Pt", C cathode electrocatalyst for direct methanol fuel cell, 2003, pp.394, ~
- S. C. Chang, "Metal crystallinity effects in electrocatalysis as probed by real-time FTIR spectroscopy: electrooxidation of formic acid, methanol, and ethanol on ordered low-index platinum surfaces", J. Phys. Chem, 94, pp.6013~ (1990)
- S. Rousseau, "Direct ethanol fuel cell(DEFC): electrical performances and reaction products distribution under operating conditions with different Ptbased anodes", J. Power Sources, 158, pp.18~ (2006)
- J. H. Choi, "Electro-oxidation of methanol and formic acid on PtRu and PtAu for direct liquid fuel cells", J. Power Sources, 163, pp.71~ (2006)
- J. Riberio, "Carbonsupported ternary PtSnIr catalysts for direct ethanol fuel cell", Electrochimica Acta, 52, pp.6997~ (2007)
- F. Vigier, "Development of anode catalysts for a direct ethanol fuel cell", J. Appl. electrochem, 34, pp.439~ (2004)
- H. Tsaprailis, "Sol-gel derived Pt-Ir mixed catalysts for DMFC applications", Electrochem. Solid-State Lett, 7, pp.A348~ (2004)
- H. S. Oh, "Investigation of carbon-supported Pt nanocatalyst preparation by the polyol process for fuel cell performances", Electrochimica Acta, 52, pp.7278~ (2007)
- L. H. Jiang, "Effect of treatment in different atmosphere on Pt3Sn", C electrocatalysts for ethanol electrooxidation, 2004, pp.18, 866~
- V. Radmilovic, "Structure and chemical composition of a supported Pt-Ru electrocatalyst for methanol oxidation", J. Catalysis, 154, pp.98~ (1995)
- Z. Liu, "Preparation and characterization of Pt", C and Pt-Ru, J. Power Sources, pp.2005, 149[DOI]