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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Fluorescence excitation spectrum of the 2-butoxyl radical and kinetics of its reactions with NO and NO2
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Fluorescence excitation spectrum of the 2-butoxyl radical and kinetics of its reactions with NO and NO2

机译：2-丁氧基自由基的荧光激发光谱及其与NO和NO2反应的动力学

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The ((A) over tilde <-- <(X)over tilde>) fluorescence excitation spectrum of the 2-C4H9O((X) over tilde) (2-butoxyl) radical in the wavelength range 345-390 nm was obtained using a combined laser photolysis/laser-induced fluorescence (LIF) technique following the generation of the radicals by excimer laser photolysis of 2-butylnitrite at lambda =351 nm. The fluorescence excitation spectrum shows 5 vibronic bands, where the dominant progression corresponds to the CO-stretching vibration in the first electronically excited state with (v) over tilde ('CO)=(560 +/- 10) cm(-1). The transition origin was assigned at (v) over tilde (00)=(26768 +/- 10) cm(-1) (lambda (00)=(373.58 +/-0.15) nm). The kinetics of the reactions of the 2-butoxyl radical with NO and NO2 at temperatures between T=223-305 K and pressures between p=6.5-104 mbar have been determined. The rate coefficients for both reactions were found to be independent of total pressure with k(NO)=(3.9 +/-0.3)x10(-11) cm(3) s(-1) and k(NO2)=(3.6 +/-0.3)x10(-11) cm(3) s(-1) at T=295 K. The Arrhenius expressions have been determined to be k(NO)=(9.1 +/-2.7)x10(-12) exp((3.4 +/-0.6) kJ mol(-1)/RT) cm(3) s(-1) and k(NO2)=(8.6 +/-3.3)x10(-12) exp((3.3 +/-0.8) kJ mol(-1)/RT) cm(3) s(-1). In addition, the radiative lifetime of the 2-C4H9O((A) over tilde) radical after excitation at lambda =365.938 nm in the (0,1) band has been determined to be tau (rad)(2-C4H9O((A) over tilde))=(440 +/- 80) ns. Quenching rate constants of the 2-C4H9O((A) over tilde) radical were measured to be k(q)=(4.7 +/-0.3)x10(-10) cm(3) s(-1) and k(q)=(5.0 +/-0.4)x10(-12) cm(3) s(-1) for 2-butylnitrite and nitrogen, respectively. [References: 52]
机译：使用以下方法获得波长范围为345-390 nm的2-C4H9O（（X上的X）（2-丁氧基））的（T上的<（）结合激光光解/激光诱导荧光（LIF）技术，然后通过准分子激光在λ= 351 nm处对2-丁基亚硝酸盐进行自由基解离生成自由基。荧光激发光谱显示了5个振动带，其中主要的进展对应于在第一个电子激发态下CO拉伸振动，其中（v）超过波浪号（'CO）=（560 +/- 10）cm（-1）。将过渡原点指定为波浪号（00）=（26768 +/- 10）cm（-1）的（v）（λ（00）=（373.58 +/- 0.15）nm）。已经确定了2-丁氧基自由基与NO和NO 2在T ＝ 223-305K之间的温度和p ＝ 6.5-104mbar之间的压力下的反应动力学。发现两个反应的速率系数与总压力无关，其中k（NO）=（3.9 +/- 0.3）x10（-11）cm（3）s（-1）和k（NO2）=（3.6 + /-0.3)x10(-11）cm（3）s（-1）在T = 295 K.Arrhenius表达式已确定为k（NO）=（9.1 +/- 2.7）x10（-12）exp （（3.4 +/- 0.6）kJ mol（-1）/ RT）cm（3）s（-1）和k（NO2）=（8.6 +/- 3.3）x10（-12）exp（（3.3 + / -0.8）kJ mol（-1）/ RT）cm（3）s（-1）。此外，在（0,1）波段在λ= 365.938 nm处激发后，2-C4H9O（在波浪线上的（A）在自由基上的辐射寿命已确定为tau（rad）（2-C4H9O（（A ）在波浪号上））=（440 +/- 80）ns。测得2-C4H9O（（A）在波浪号上）的淬灭速率常数为k（q）=（4.7 +/- 0.3）x10（-10）cm（3）s（-1）和k（q ）=（5.0 +/- 0.4）x10（-12）cm（3）s（-1）对于亚硝酸2-丁酯和氮。 [参考：52]

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