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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Temperature and pressure dependent rate coefficients for the reaction of Hg with Br and the reaction of Br with Br: A pulsed laser photolysis-pulsed laser induced fluorescence study
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Temperature and pressure dependent rate coefficients for the reaction of Hg with Br and the reaction of Br with Br: A pulsed laser photolysis-pulsed laser induced fluorescence study

机译：Hg与Br反应以及Br与Br反应的温度和压力相关速率系数：脉冲激光光解脉冲激光诱导的荧光研究

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摘要

A pulsed laser photolysis-pulsed laser induced fluorescence technique has been employed to study the recombination of mercury and bromine atoms, Hg + Br + M -> HgBr + M (1) and the self-reaction of bromine atoms, Br + Br + M -> Br-2 + M (2). Rate coefficients were determined as a function of pressure (200-600 Torr) and temperature (243-293 K) in nitrogen buffer gas and as a function of pressure (200600 Torr) in helium buffer gas at room temperature. For reaction 1, kinetic measurements were performed under conditions in which bromine atoms were the reactant in excess concentration while simultaneously monitoring the concentration of both mercury and bromine. A temperature dependent expression of (1.46 +/- 0.34) x 10(-32) x (T/298)(-(1.86 +/- 1.49)) cm(6) molecule(-2) s(-1) was determined for the third-order recombination rate coefficient in nitrogen buffer gas. The effective second-order rate coefficient for reaction 1 under atmospheric conditions is a factor of 9 smaller than previously determined in a recently published relative rate study. For reaction 2 we obtain a temperature dependent expression of (4.31 +/- 0.21) x 10(-33) x (T/298)(-( 2.77 +/- 0.30)) cm(6) molecule(-2) s(-1) for the third-order recombination rate coefficient in nitrogen buffer gas. The rate coefficients are reported with a 2 sigma error of precision only; however, due to the uncertainty in the determination of absolute bromine atom concentrations and other unidentified systematic errors we conservatively estimate an uncertainty of +/- 50% in the rate coefficients. For both reactions the observed pressure, temperature and buffer gas dependencies are consistent with the expected behavior for three-body recombination.
机译：脉冲激光光解-脉冲激光诱导荧光技术已用于研究汞和溴原子Hg + Br + M-> HgBr + M的重组（1）和溴原子Br + Br + M的自反应-> Br-2 + M（2）。确定速率系数是氮气缓冲气体中压力（200-600 Torr）和温度（243-293 K）的函数，以及室温下氦缓冲气体中压力（200600 Torr）的函数。对于反应1，在其中溴原子是过量浓度的反应物的条件下进行动力学测量，同时监测汞和溴的浓度。确定（1.46 +/- 0.34）x 10（-32）x（T / 298）（-（1.86 +/- 1.49））cm（6）分子（-2）s（-1）的温度依赖性表达氮缓冲气体中的三阶复合率系数。在大气条件下，反应1的有效二阶速率系数比最近发表的相对速率研究中先前确定的小9倍。对于反应2，我们获得（4.31 +/- 0.21）x 10（-33）x（T / 298）（-（2.77 +/- 0.30））cm（6）分子（-2）s（ -1）为氮气缓冲气体中的三阶复合率系数。报告的速率系数仅具有2 sigma的精度误差;但是，由于确定绝对溴原子浓度的不确定性和其他未确定的系统误差，我们保守地估计速率系数的不确定性为+/- 50％。对于这两个反应，观察到的压力，温度和缓冲气体依赖性与三体重组的预期行为一致。

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