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Role of Bridge-bonded Formate in Formic Acid Dehydration to CO at Pt Electrode: Electrochemial in-situ Infrared Spectroscopic Study
Zun-biao Zhang,Jie Xu,Jing Kang,Yan-xia Chen*
Author NameAffiliationE-mail
Zun-biao Zhang Hefei National Laboratory for Physical Science at Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Jie Xu Hefei National Laboratory for Physical Science at Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China  
Jing Kang Hefei National Laboratory for Physical Science at 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 Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China yachen@ustc.edu.cn 
Abstract:
Formic acid (HCOOH) decomposition at Pt film electrode has been studied by electrochem- ical in situ FTIR spectroscopy under attenuated-total-reflection configuration, in order to clarify whether bridge-bonded formate (HCOOb) is the reactive intermediate for COad for-mation from HCOOH molecules. When switching from HCOOH-free solution to HCOOH-containing solution at constant potential (E=0.4 V vs. RHE), we found that immediately upon solution switch COad formation rate is the highest, while surface coverage of formate is zero, then after COad formation rate decreases, while formate coverage reaches a steady state coverage quickly within ca. 1 s. Potential step experiment from E=0.75 V to 0.35 V, reveals that formate band intensity drops immediately right after the potential step, while the COad signal develops slowly with time. Both facts indicate that formate is not the reactive intermediate for formic acid dehydration to CO.
Key words:  Mechanism for formic acid dehydration, Formate intermediate, CO pathway, Pt electrode, Infrared spectroscopic studies under attenuated total reflection configuration
FundProject:
电化学红外光谱研究铂电极上甲酸分解成CO的反应中桥式吸附甲酸根的作用
张尊彪,徐杰,康婧,陈艳霞*
摘要:
采用电化学原位红外光谱技术研究了多晶Pt电极上甲酸的分解反应. 研究发现,在恒电位下(0.4 V vs. RHE)从不含甲酸的支持电解质溶液切换到含甲酸的溶液时,COad的生成速率在切换的最初也就是甲酸根的覆盖度为零最大,切换后的1 s内甲酸根的覆盖度达到平衡,而COad的生成速率逐步降低. E由0.75 V变至0.35 V的电位阶跃实验显示:电位阶跃后的瞬间,甲酸根的红外光谱强度迅速降低,而COad的生成强度随时间缓慢增加. 实验表明甲酸根不是甲酸脱水生成CO的反应活性中间体.
关键词:  甲酸脱水机理,CO路径,铂电极,甲酸根中间物
DOI:10.1063/1674-0068/26/04/471-476
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