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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Kinetics of Several Oxygen-Containing Carbon-Centered Free Radical Reactions with Nitric Oxide
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Kinetics of Several Oxygen-Containing Carbon-Centered Free Radical Reactions with Nitric Oxide

机译：一氧化氮与几个含氧碳中心自由基反应的动力学

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Kinetics of four carbon-centered, oxygen-containing free radical reactions with nitric oxide (NO) were investigated as a function of temperature at a few Torr pressure of helium, employing flow tube reactors coupled to a laser-photolysis/resonance-gas-discharge-lamp photoionization mass spectrometer (LP-RPIMS). Rate coefficients were directly determined from radical (R) decay signals under pseudo-first-order conditions ([R](0) e [NO]). The obtained rate coefficients showed negative temperature dependences, typical for a radical-radical association process, and can be represented by the following parametrizations (all in units of cm(3) molecule(-1) s(-1)): k(CH2OH + NO) = (4.76 x 10(-21)) x (T/300 K)(15.92) x exp[50700/(RT)] (T = 266-363 K, p = 0.79-3.44 Torr); k(CH3CHOH + NO) = (1.27 x 10(-16)) x (T/300 K)(6.81) x exp[28700/(RT)] (T = 241-363 K, p = 0.52-3.43 Torr); k(CH3OCH2 + NO) = (3.58 +/- 0.12) x 10(-12) x (T/300 K)(-3.17)+/-(0.14) (T = 221363 K, p = 0.50-0.80 Torr); k(T)(3) = 9.62 x 10(-11) x (T/300 K)(-5.99) x exp[-7100/(RT)] (T = 221473 K, p = 1.41-2.95 Torr), with the uncertainties given as standard errors of the fits and the overall uncertainties estimated as +/-20%. The rate of CH3OCH2 + NO reaction was measured in two density ranges due to its observed considerable pressure dependence, which was not found in the studied hydroxyalkyl reactions. In addition, the CH3CO + NO rate coefficient was determined at two temperatures resulting in k(298K)(CH3CO + NO) = (5.6 +/- 2.8) x 10(-13) cm(3) molecule(-1) s(-1). No products were found during these experiments, reasons for which are briefly discussed.
机译：利用流管反应器与激光光解/共振气体放电耦合，研究了在几个托尔氦气压力下，与一氧化氮（NO）发生的四个碳中心含氧自由基反应的动力学与温度的关系。灯光电离质谱仪（LP-RPIMS）。速率系数是根据伪一阶条件（[R]（0）e [NO]）的基本（R）衰减信号直接确定的。所获得的速率系数显示出负温度依赖性，这是自由基-自由基缔合过程的典型现象，并且可以由以下参数表示（均以cm（3）分子（-1）s（-1）为单位）：k（CH2OH + NO）=（4.76 x 10（-21））x（T / 300 K）（15.92）x exp [50700 /（RT）]（T = 266-363 K，p = 0.79-3.44 Torr）; k（CH3CHOH + NO）=（1.27 x 10（-16））x（T / 300 K）（6.81）x exp [28700 /（RT）]（T = 241-363 K，p = 0.52-3.43 Torr） ; k（CH 3 OCH 2 + NO）=（3.58 +/- 0.12）x 10（-12）x（T / 300 K）（-3.17）+/-（0.14）（T = 221363 K，p = 0.50-0.80托） ; k（T）（3）= 9.62 x 10（-11）x（T / 300 K）（-5.99）x exp [-7100 /（RT）]（T = 221473 K，p = 1.41-2.95 Torr），不确定性作为拟合的标准误差给出，总体不确定性估计为+/- 20％。由于观察到的显着压力依赖性，在两个密度范围内测量了CH3OCH2 + NO反应的速率，这在所研究的羟烷基反应中没有发现。此外，在两个温度下确定CH3CO + NO速率系数，得出k（298K）（CH3CO + NO）=（5.6 +/- 2.8）x 10（-13）cm（3）分子（-1）s（ -1）。在这些实验中未发现任何产品，简要讨论了其原因。

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