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水合氧化钌对铂电催化剂上甲醇电氧化反应的促进作用

Promotion of Platinum Electrocatalyst by Hydrous Ruthenium Oxide for Methanol Oxidation

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【作者】 马俊红余洁赵丹王安杰徐柏庆

【Author】 MA Junhong1,YU Jie2,ZHAO Dan2,WANG Anjie1,XU Boqing2,1 State Key Laboratory of Fine Chemicals,Dalian University of Technology,Dalian 116012,Liaoning,China 2Innovative Catalysis Program,Key Laboratory of Organic Optoelectronics and Molecular Engineering,Department of Chemistry,Tsinghua University,Beijing 100084,China

【机构】 大连理工大学精细化工国家重点实验室清华大学化学系有机光电子与分子工程教育部重点实验室,分子催化与定向转化研究室

【摘要】 以多壁碳纳米管(MWCNTs)为载体,制备了Pt载量为20%的Pt-(RuOxHy)m/MWCNTs催化剂(m为Ru/Pt原子比),在m≤0.4时考察了不同电势区间循环伏安预处理对其催化性能的影响.水合氧化钌(RuOxHy)的存在明显提高了Pt催化剂抗CO毒化的能力,而在甲醇电氧化反应中Pt的质量比活性(MSA)随样品中m值增大呈先升后降趋势.经低电势区间(-0.20-0.46 V vs SCE)预处理稳定的催化剂中,Pt-(RuOxHy)0.10/MWCNTs样品中Pt的甲醇电氧化反应的MSA提高至相应单组分Pt/MWCNTs的9倍.将预处理电势区间扩展到高电势(即-0.20-0.96 v vs SCE)会造成钌组分溶解流失,导致催化剂抗CO毒化能力下降.在经过高电势区间的预处理后,Pt-(RuOxHy)020/MWCNTs对甲醇电氧化反应呈现出最高的催化活性,为单组分Pt催化剂的1.4倍.这些结果证实,水合氧化钉是Pt电催化剂的有效助剂.

【Abstract】 A series of Pt-(RuOxHy)m/MWCNTs catalysts(m being the Ru/Pt atomic ratio) containing 20% Pt were prepared using multi-walled carbon nanotubes(MWCNTs) as the support.The activity towards CO and methanol electro-oxidation of Pt in these catalysts after repeated cyclic voltammetry treatments in low(-0.20-0.46 V vs SCE) and extended(-0.20-0.96 V vs SCE) potential regions was investigated.The results showed that the presence of hydrous ruthenium oxide(RuOxHy) significantly reduced the over-potential of CO electro-oxidation on Pt,and the activity of Pt in Pt-(RuOxHy)m/MWCNTs for methanol electro-oxidation could thus be maximized by proper tuning of m.After the treatment in the low potential region,the mass-specific activity(MSA) of Pt in Pt-(RuOxHy)m/MWCNTs of m = 0.10 for methanol electro-oxidation increased by nearly 9 times that in Pt/MWCNTs.Significant dissolution of RuOxHy species was detected after the pretreatment in the extended potential region,which resulted in reduced CO tolerance and changed the activity order of Pt-(RuOxHy)m/MWCNTs catalysts for methanol electro-oxidation.In this case,Pt in the sample with m = 0.20 showed the highest MSA,which was still 40% higher than that of Pt/MWCNTs.

【基金】 国家自然科学基金(20773074);国家高技术研究发展计划(863计划,2006AA03Z225)
  • 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2009年06期
  • 【分类号】TM911.4
  • 【被引频次】5
  • 【下载频次】228
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