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Study on Methanol Oxidation at Pt and PtRu Electrodes by Combining in situ Infrared Spectroscopy and Di erential Electrochemical Mass Spectrometry
Qian Tao,Wei Chen,Yao Yao,Ammar Bin Yousaf,Yan-xia Chen*
Author NameAffiliationE-mail
Qian Tao Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Wei Chen Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Yao Yao Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Ammar Bin Yousaf Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Yan-xia Chen* Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China yachen@ustc.edu.cn 
Abstract:
Methanol oxidation reaction (MOR) at Pt and Pt electrode surface deposited with various amounts of Ru (denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML) in 0.1 mol/L HClO4+0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that (i) CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V (vs. RHE); (ii) at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; (iii) MOR activity decreases in the order of Pt0.73Ru0.27>Pt0.56Ru0.44>Pt0.83Ru0.17>Pt; (iv) at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/(site sec). Suggestions for further improving of PtRu catalysts for MOR are provided.
Key words:  Differential electrochemical mass spectrometry, Electrochemical in situ in-frared spectroscopy, Methanol oxidation, PtRu electrode, Current efficiency
FundProject:
利用原位红外光谱与微分电化学质谱联用技术研究在Pt以及PtRu电极上发生的甲醇氧化反应
陶骞,陈微,姚瑶,Ammar Bin Yousaf,陈艳霞*
摘要:
利用电化学衰减全反射原位傅里叶变换红外光谱与微分电化学质谱联用技术,在流动电解池环境以及恒电位条件下研究了Pt电极和Pt电极通过表面电沉积Ru形成的PtRu电极(PtxRuy)上发生的甲醇氧化反应(反应电解质溶液为0.1 mol/L HClO4+0.5 mol/L MeOH). 在0.3~0.6 V(参比电极为可逆氢参比)实验用到的所有电极上,CO是唯一能从红外光谱观察到的与甲醇相关的表面吸附物;在Pt0.56Ru0.44电极上可以观察到CO吸附在Ru原子形成的岛上和CO线式吸附在Pt电极表面红外波段,而其他电极上只能观察到Pt表面上线式吸附的CO;甲醇氧化活性按Pt0.73Ru0.27>Pt0.56Ru0.44>Pt0.83Ru0.17>Pt的顺序递减;在0.5 V 时,甲醇在Pt0.73Ru0.27电极上的氧化反应的CO2电流效率达到了50%.
关键词:  微分电化学质谱,电化学衰减全反射原位傅里叶变换红外光谱,甲醇氧化,PtRu电极,CO2电流效率
DOI:10.1063/1674-0068/27/05/541-547
分类号: