Grant-in-Aid for Scientific Research (A)
|Allocation Type||Single-year Grants|
|Research Institution||Hokkaido University|
OSAWA Masatoshi Hokkaido University, Catalysis Research Center, Professor, 触媒化学研究センター, 教授 (00108466)
YE Shen Hokkaido University, Catalysis Research Center, Associated Professor, 触媒化学研究センター, 助教授 (40250419)
YAMAKATA Akira Hokkaido University, Catalysis Research Center, Research Associate, 触媒化学研究センター, 助手 (60321915)
|Project Period (FY)
2002 – 2004
Completed(Fiscal Year 2004)
|Budget Amount *help
¥56,030,000 (Direct Cost : ¥43,100,000、Indirect Cost : ¥12,930,000)
Fiscal Year 2004 : ¥5,720,000 (Direct Cost : ¥4,400,000、Indirect Cost : ¥1,320,000)
Fiscal Year 2003 : ¥5,460,000 (Direct Cost : ¥4,200,000、Indirect Cost : ¥1,260,000)
Fiscal Year 2002 : ¥44,850,000 (Direct Cost : ¥34,500,000、Indirect Cost : ¥10,350,000)
|Keywords||Electrochemistry / Surface electrochemistry / Electrode dynamics / Infrared spectroscopy / Electrocatalysis / Self-assembled monolayer / Electrochemical oscillations / Reaction mechanism / 表面反応ダイナミクス / 光電極反応 / 反応中間体 / 燃料電池 / 電子移動 / 表面増強赤外分光 / 水素電極反応 / 自己集積単分子膜 / 核酸塩基対|
This project aimed at to study electrode kinetics and dynamics by using fast time-resolved infrared spectroscopy. The use of surface-enhanced infrared absorption spectroscopy (SEIRAS) enabled ultrafast time-resolved study in the picosecond range. The main achievements are as follows.
1.Ultrafast time-resolved IR spectrscopy
Double-layer charging with a 0.1-1 ms time constant has hampered the study of ultrafast electrode dynamics. This problem was circumvented for the first time by coupling the so-called temperature jump method with picosecond time-resolved SEIRAS. The rapid heating of the interface by a laser pulse results in the sudden change in potential through reorientaion of water.
2.Technical developments in SEIRAS
Simple and cost-effective techniques to prepare very stable SEIRA-active thin metal film electrodes on Si and Ge prisms have been developed. These techniques significantly contributed to the success of the picosecond time-resolved IR studies mentioned above.
le analysis of electrochemical oscillations
A variety of oscillations occur at the electrochemical interface. We investigated potential and current oscillations during formic acid oxidation on Pt by time-resolved SEIRAS and proposed a new concept that explains the oscillations without any assumptions.
Hydrogen evolution, oxygen reduction, and anodic oxidation of C_1 molecules on Pt electrodes that constitute the basis of low temperature fuel cells were examined in detail at the molecular scale. We clearly showed for the first time that all C_1 molecules are oxidized CO_2 via formate, which totally revised the general consensus.
5.Structures and functions of self-assembled monolayers (SAMs)
Hydrogen bond pairing between an adenine derivative self-assembled on an Au electrode and a thimidine derivative were examined by SEIRAS as a model system of molecular recognition system. We also succeeded in fabricating new types of SAMs using triruthenium complexes. Their structures and functions were examined by SEIRAS. Less