Citation: LV Yong-Gang, LI Zhi-Jun, WU Li-Zhu, WANG Peng, FU Li-Min, ZHANG Jian-Ping. Application of Time-Resolved Coherent Anti-Stokes Raman Scattering Technique on the Study of Photocatalytic Hydrogen Production Kinetics[J]. Acta Physico-Chimica Sinica, ;2013, 29(08): 1632-1638. doi: 10.3866/PKU.WHXB201304281 shu

Application of Time-Resolved Coherent Anti-Stokes Raman Scattering Technique on the Study of Photocatalytic Hydrogen Production Kinetics

1.
1 Department of Chemistry, Renmin University of China, Beijing 100872, P. R. China;
2 Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China;
3 School of Physics, Peking University, Beijing 100871, P. R. China

Received Date: 31 January 2013
Available Online: 28 April 2013
Fund Project: 国家重点基础研究发展规划项目(973) (2009CB220008)资助 (973) (2009CB220008)

Based on the laser pulse output from a femtosecond regenerative amplifier and optical parametric amplifier (OPA), a broadband time-resolved coherent anti-Stokes Raman scattering (CARS) setup was assembled. Using this setup, the relationship of hydrogen CARS spectra to its amount in a mixture with air and the relevant detection time-delay were studied. Hydrogen CARS spectra without nonresonant background interference were obtained by adjusting the detection time-delay. The observed CARS intensity exhibited a linear relationship with the square of hydrogen concentration, which is consistent with the theoretical prediction. The signal-to-noise ratio showed that when the pressure of hydrogen-air mixed gas was 0.1 MPa, the detection limit of our setup was less than 0.2%. Using this setup, the hydrogen production kinetics of a platinum(II) terpyridyl acetylide molecular-cobalt catalysttriethanolamine (TEOA) system was studied. The kinetic mechanism of hydrogen production was discussed by considering the effect of changing pH. The results indicate that a high proton concentration will reduce the hydrogen production efficiency. This can be attributed to the inhibition of hydrolysis of TEOA under acidic conditions, because it is the electron and proton donor in this hydrogen production system.
- Coherent anti-Stokes Raman scattering,
- Nonresonant background,
- Time-resolved spectrum,
- Photo-catalysis,
- Kinetics
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