Photochemical degradation of acrolein using VUV excimer lamp in air at atmospheric pressure
Photochemical degradation of acrolein using VUV excimer lamp in air at atmospheric pressure
复制标题
常压空气中使用 VUV 准分子灯光化学降解丙烯醛
DOI：
10.1007/s13762-019-02404-5
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发表时间：
2019
影响因子：
3.1
通讯作者：
M. Tsuji,M. Miyano,N. Kamo,T. Kawahara,K. Uto,J. Hayashi,T. Tsuji
中科院分区：
文献类型：
--
作者：
Kataoka;Yusuke; Yano;Natsumi; Kohara;Yoshihiro; Tsuji;Takeshi; Inoue;Satoshi; Kawamoto;Tatsuya;M. Tsuji,M. Miyano,N. Kamo,T. Kawahara,K. Uto,J. Hayashi,T. Tsuji
利用172 nm Xe2准分子灯研究了丙烯醛(C2H3CHO)在常压空气中的光化学降解。当用侧式灯分解C2H3CHO时，在FTIR吸收光谱中观察到HCOOH、CO、CO2和O3峰。产物浓度对辐照时间的依赖关系表明，HCOOH和CO中间体最终通过连续反应转化为CO2。当O2浓度从20%降至1%时，间歇体系中C2H3CHO的降解速率系数从8.4min−1增加到19.3min；当氧气室深度从3.0min减小到0.5min时，在20%O2时，−1也从8.4min增加到40.1min。在流动系统中，当氧气浓度为1-20%时，降解C2H3CHO的最佳能效为3.4g/kW−1h−1。除了C2H3CHO的直接真空紫外光解离外，O(3P，1D)与O2光解产生的O(3P，1D)反应也有助于C2H3CHO的初期降解。其中，O(1D)和O_3对C_2H_3CHO脱除量与总压的关系以及O_3+ C_2H_3CHO反应的结果表明，O(1D)和O_3的贡献不显著。结果表明，C2H3CHO首先是通过直接的真空紫外光解离和O(3P) + C2H3CHO反应分解的。O(3P)、OH、O3与HCOOH、CO等中间体发生二次反应，最终氧化成CO2。
The photochemical degradation of acrolein (C2H3CHO) was investigated in air at atmospheric pressure using a 172-nm Xe2excimer lamp. When C2H3CHO was decomposed using the side-on type of lamp, HCOOH, CO, CO2, and O3peaks were observed in FTIR absorption spectra. The dependence of product concentrations on the irradiation time indicated that HCOOH and CO intermediates are finally converted to CO2via consecutive reactions. The degradation rate coefficient of C2H3CHO in the batch system increased from 8.4 to 19.3 min−1, as the O2concentration was decreased from 20 to 1%. It increased also from 8.4 to 40.1 min−1at 20% O2, as the chamber depth was decreased from 3.0 to 0.5 cm. The best energy efficiency of the C2H3CHO degradation was 3.4 g kW−1h−1at 1–20% O2in a flow system. Besides direct VUV photodissociation of C2H3CHO, reactions of O(3P,1D) and O3, produced from photolysis of O2, can contribute to C2H3CHO degradation in the initial stage. Among them, the contribution of O(1D) and O3was found to be insignificant on the basis of the total pressure dependence of removal amount of C2H3CHO and results obtained from the O3+ C2H3CHO reaction. It was concluded that at first C2H3CHO is decomposed by direct VUV photodissociation of C2H3CHO and the O(3P) + C2H3CHO reaction. It was further decomposed by secondary reactions of O(3P), OH, and O3with such intermediates as HCOOH and CO and finally oxidized to CO2.