基于拉曼光谱的可视化石英微反应器中间氯甲苯超(亚)临界水氧化研究Study on Supercritical Water Oxidation of 3-Chlorotoluene in a Visible Quartz Microreactor by Raman Spectroscopy
徐明仙,周新凯,甄万顺,贝克,潘志彦,林春绵
摘要(Abstract):
借助可视化石英微反应器和拉曼光谱,探究了间氯甲苯的超临界水氧化过程,实现了对产物CO_2的原位测定。实验观测了间氯甲苯-H_2O/H_2O_2体系在加热冷却过程的相态变化,研究了氧化剂倍数、反应温度、反应时间对有机物去除率的影响,以及反应温度和反应时间对CO_2产率的影响。结果表明:(1)在升温(10℃?min~(-1))与降温(10℃?min~(-1))过程,间氯甲苯-H_2O/H_2O_2体系在加热和冷却过程均发生了明显相态变化,温度升至304.2℃时,油-水相界面消失,到400℃时,相界面消失形成均一相;经升温和降温后,间氯甲苯-H_2O_2体系有机物的体积较为明显减小;(2)随氧化剂(H_2O_2)倍数的增加,有机物去除率的提高呈先快后慢的趋势,适宜氧化剂倍数为1.50;温度越高、反应时间越长,有机物的去除率越高;当温度为340℃、反应时间为8 min时,间氯甲苯的去除率达到99.4%;(3)CO_2的产率随着温度的升高或反应时间的延长而增加,当温度为460℃,反应时间为8 min时,CO_2的产率达到100.0%;间氯甲苯在超临界水中的氧化过程为多步反应。
关键词(KeyWords): 石英微反应器;拉曼光谱;超临界水氧化;间氯甲苯;二氧化碳
基金项目(Foundation): 国家自然科学基金(2137716)
作者(Author): 徐明仙,周新凯,甄万顺,贝克,潘志彦,林春绵
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