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標題: 添加金屬氧化物於質子交換膜燃料電池中之陽極鉑觸媒以提升對CO之容忍度
Adding metal oxides in Pt anode electrocatalysts for enhancing CO tolerance in proton exchange membrane fuel cells
作者: 郭蔓嬋
Guo, Mann-Charn
關鍵字: 質子交換膜燃料電池;PEMFC;前處理;CO容忍度;金屬氧化物;Pretreatment;CO tolerance;Metal oxides
出版社: 環境工程學系所
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本研究將先探討質子交換膜燃料電池(PEMFC)膜電極組(MEA)的製備條件,再對近年來較新穎之奈米碳管(CNTs)碳擔體進行改質,比較經不同硝酸前處理程序後之擔體製備之觸媒催化活性之影響,最後選用添加CeO2、ZrO2、SnO2金屬氧化物(MOx)於鉑觸媒測試活性大小,並探討不同濃度CO對質子交換膜燃料電池的影響。將利用FESEM、TEM、XRD、BET及ESCA 進行觸媒特性分析。研究結果顯示,膜電極組經135 oC、240秒壓著後具有較佳的電化學活性。在擔體前處理方面,以硝酸在50 oC下處理兩天之奈米碳管擔體(CNTs-50oC-2d)製備之電極觸媒擁有較高的活性,推測其改質後擔體比表面積增加,有利於氣體分子擴散進入孔洞內與活性相反應。比較添加MOx結果顯示,在相同電壓操作下,以5%SnO2-5%Pt/C及5%ZrO2-5%Pt/C皆比未添加MOx具較佳之電化學活性,顯示添加MOx具催化效果,其中5%SnO2-5%Pt/C具較高的電流密度,有較佳之電化學效能。在CO毒化的部分,本研究以5%MOx-5%Pt/C、5%Pt/C與10%Pt/C電極觸媒進行100 ppm CO活性測試,研究結果顯示,添加SnO2及ZrO2具有提升電極觸媒對CO的容忍度,依序為5%ZrO2-5%Pt/C > 5%SnO2-5%Pt/C > 5%Pt/C > 5%CeO2-5%Pt/C;探討在不同CO濃度(0、25、50及100 ppm)於陽極燃料之容忍度測試,以5%ZrO2-5%Pt/C擁有較高之抗CO的能力。整體而言,添加MOx於Pt電極觸媒會提升電催化效果及CO容忍度。

The aim of this study is to discuss the preparation of the membrane-electrode assembly (MEA) by using carbon nanotubes (CNTs) in proton exchange membrane fuel cell (PEMFC). Different pretreatment procedures of carbon supports are also considered to evaluate the catalytic activity with various catalysts. Besides, the addition of metal oxides such as CeO2、ZrO2 and SnO2 are investigated to enhance the electrocatalytic activity and the tolerance of different CO concentrations. All catalysts are characterized by means of FESEM, TEM, XRD, BET and ESCA.
The experimental results show that the effects of various preparation methods on the MEA to determine the best operating parameters. The 240 seconds hot-press with temperature is 135 oC has been selected for further experiments. Additionally, the investigation of the catalytic activity compared with different pretreatment procedures for catalyst support indicates that CNTs pretreated with nitric acid at 50 oC for two days (CNTs-50 oC-2d) that are supported active metals has higher catalytic activity than others. It is supposed that CNTs-50oC-2d supports have higher surface area provided more active sites and the gas molecules may easily diffuse into the pores to be reacted. Moreover, the electrocatalytic activities by using several catalysts included 5%SnO2-5%Pt/C, 5%ZrO2-5%Pt/C at the same voltage are higher than those without adding any MOx, and 5%SnO2-5%Pt/C is the effectiveness catalyst found after testing .On the other hand, it was reported that the CO tolerance of electrocatalyst was also enhanced by the addition of SnO2 and ZrO2 under the CO concentration is 100 ppm. The CO tolerance are in the following order as 5%ZrO2-5%Pt/C > 5%SnO2-5%Pt/C > 5%Pt/C > 5%CeO2-5%Pt/C. The effect of various concentrations of CO (0、50 and 100 ppm) shows that 5%ZrO2-5%Pt/C catalyst displays a better CO tolerance than the others. Consequently, the electrocatalytic activity and CO tolerance of catalysts are both enhanced while MOx added with Pt.
其他識別: U0005-1407201220465500
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