活性卤素是大气中的重要物种,它能参与大气中的多种化学过程,对臭氧的损耗有重要影响,影响许多重要物种的源和汇,同时对大气硫循环和汞循环也产生影响,在大气化学中有着十分重要的作用。因此,对活性卤素化学的研究成为近年来国际大气化学研究的重要前沿。本文总结了近年来活性卤素化学实验和理论的研究进展,重点介绍了活性卤素在臭氧损耗中的作用及其大气循环反应过程;综述了重要活性卤素物种的产生和探测、活性卤素光化学反应和非均相反应实验研究;总结了近年来关于活性卤素化学的理论研究,包括活性卤素与水、硫、HO、HO2、烷基氧和烷基过氧自由基、氮氧化物、汞及其它物种的耦合研究。最后,对活性卤素化学的实验和理论研究进行了展望,提出了尚待深入开展研究的一些重要科学问题。
Reactive halogen species are important components in the atmosphere, which can participate in many atmospheric chemical processes, play important role in the ozone depletion, affect sources and sinks of many important compounds and the sulfur and mercury cycle of atmosphere as well. Consequently, reactive halogen chemistry is an important frontier research field in the atmospheric chemistry. In this review, we introduce the recent experimental and theoretical progress of reactive halogen chemistry, review the important role of reactive halogen species in the ozone depletion and their atmospheric cycle reactions, and the production and detection studies of important reactive halogen species and their photochemisty and heterogeneous reactions. The recent theoretical studies of reactive halogen chemistry are summarized, including interactions between reactive halogen species with water, sulfur, OH, HO2, alkyl oxide and alkyl peroxide radicals, nitrogen oxide, mercury and other species. Finally, prospect of reactive halogen chemistry and main scientific problems are put forward.