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Electrochemical Study on Hydrogen Evolution and CO2 Reduction on Pt Electrode in Acid Solutions with Different pH
Jing Yang,Jie Wei,Wei Chen,Yan-xia Chen*
Author NameAffiliationE-mail
Jing Yang Hefei National Laboratory for Physical Science at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Jie Wei 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  
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:
Hydrogen evolution reaction (HER) is the major cathodic reaction which competes CO2 reduction reaction (CO2 RR) on Pt electrode. Molecular level understanding on how these two reactions interact with each other and what the key factors are of CO2 RR kinetics and selectivity will be of great help in optimizing electrolysers for CO2 reduction. In this work, we report our results of hydrogen evolution and CO2 reduction on Pt(111) and Pt film electrodes in CO2 saturated acid solution by cyclic voltammetry and infrared spectroscopy. In solution with pH>2, the major process is HER and the interfacial pH increases abruptly during HER; COad is the only adsorbed intermediate detected in CO2 reduction by infrared spectroscopy; the rate for COad formation increases with the coverage of UPD-H and reaches maximum at the onset potential for HER; the decrease of COad formation under HER is attributed to the available limited sites and the limited residence time for the reduction intermediate (Had), which is necessary for CO2 adsorption and reduction.
Key words:  Hydrogen evolution reaction, CO2 Reduction, Pt(111), Acidic solution, pH effect, Infrared spectroscopy
FundProject:
不同pH酸性溶液中铂电极上氢析出和二氧化碳还原的电化学研究
杨 晶,魏 杰,陈 微,陈艳霞*
摘要:
本文利用循环伏安法和电化学原位红外光谱的联用,研究了Pt(111)和Pt膜电极在CO2饱和的酸性溶液中氢析出和CO2还原的竞争. 发现:(i)在pH>2的溶液中,主要反应是氢析出,界面pH值随着氢析出突然增加;(ii)通过红外光谱检测,COad是CO2还原过程中唯一的吸附中间体;(iii)COad生成速率随着欠电位沉积氢(UPD-H)覆盖的增加而增大,并在氢析出的起始电位达到最大值;(iv)在氢析出时,COad的减少与CO2吸附和还原所必需的的中间产物(Had)有限的可用位点和停留时间相关.
关键词:  氢析出,二氧化碳还原,Pt(111), 酸性溶液,pH效应,红外光谱
DOI:10.1063/1674-0068/31/cjcp1804057
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