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基于飞秒再生放大器及飞秒光学参量放大器输出的激光脉冲,搭建了宽带时间分辨相干反斯托克斯拉曼散射(CARS)测试装置,并利用该装置研究了氢气与空气混合气体中氢气的相对含量,探测相对延时与CARS光谱之间的关系.通过调整延时,获得了无非共振背景干扰的氢气CARS信号.实验中测得的CARS信号强度与氢气浓度(分压)的平方呈良好的线性关系,符合CARS理论预测.同时测得的实验数据的信噪比表明:在当前的实验条件下,在氢气与空气混合气的总压为0.1MPa时,该装置可以对氢气的浓度进行测量,且其检测极限可低至0.2%.本文还利用该装置对三联吡啶苯乙炔Pt配合物-Co配合物-三乙醇胺(TEOA)的三元化学催化体系的产氢动力学行为进行了研究,通过改变pH值讨论了该催化体系的产氢动力学机制.结果表明过高的质子浓度会降低体系的产氢效率,这可能是因为在酸性条件下,作为质子和电子供体的三乙醇胺分解被抑制,电子供应中断,导致产氢反应的停止.
Based on the laser pulse output from the femtosecond regenerative amplifier and the femtosecond optical parametric amplifier, a time-resolved wideband time-resolved anti-Stokes Raman scattering (CARS) test set-up was set up and used to study the effect of hydrogen on the mixed gas of hydrogen and air Relative content, the relationship between relative delay and CARS spectra was explored.The hydrogen CARS signal with nonresonant background interference was obtained by adjusting the delay.The square of CARS signal intensity and hydrogen concentration (partial pressure) measured in the experiment was good Linear relationship with the CARS theory.At the same time, the signal-to-noise ratio of the experimental data shows that under the current experimental conditions, when the total pressure of hydrogen and air mixture is 0.1MPa, the device can conduct hydrogen concentration , And its detection limit can be as low as 0.2% .This paper also uses this device to study the hydrogen production kinetics of the ternary chemical catalysis system of terpyridine phenylacetylene Pt complex-Co complex-triethanolamine (TEOA) , The kinetics of hydrogen production in this catalytic system was discussed by changing the pH value.The results show that high proton concentration will reduce the hydrogen production efficiency of the system, which may be because under acidic conditions, Triethanolamine decomposition proton and an electron donor is suppressed, the electron supply interruption, resulting in hydrogen production reaction is stopped.