多氯联苯在环境凝聚态水中的光致转化机理
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摘要
多氯联苯是一类毒性很强的持久性有机污染物，它们在环境中的转化和去除途径一直是人们所关注的热点问题。环境凝聚态水(如：江、河、湖、海、云、雨、雾、冰雪等)普遍存在于自然环境中。研究环境凝聚态水中联苯和氯代联苯的反应机理，有助于深入了解和全面掌握多氯联苯在自然环境中的转化规律。本文采用纳秒级激光瞬态光谱技术与高效液相色谱、气质联用技术相结合，以联苯和4-氯联苯作为主要研究对象，以N(Ⅲ)作为环境液态水中~·OH的主要来源，H_2O_2作为环境固态水中~·OH的主要来源，考察了环境凝聚态水中联苯(或4-氯联苯)与光诱导产生的~·OH之间的反应过程，并提出了反应机理。
联苯与N(Ⅲ)混合溶液、4-氯联苯与N(Ⅲ)混合溶液光化学反应的主要研究结论如下：
(1)联苯与N(Ⅲ)混合溶液、4-氯联苯与N(Ⅲ)混合溶液在紫外光的作用下均能够发生明显的反应。反应都起始于它们与N(Ⅲ)光解产生的~·OH之间的加成作用。实验测得的二级反应速率常数分别为(9．6±0．1)×10~9L mol~(-1) s~(-1)(298 K)、(8．0±0．5)×10~9 Lmol~(-1)s~(-1)(298 K)。
(2)pH值对于联苯、4-氯联苯的降解效率影响显著，pH值越高，联苯、4-氯联苯的降解速率越慢。
(3)~·OH加合产物Bp…OH加合物、4-PCB…OH加合物的衰减均较为复杂。溶液中存在的H~+、HONO、H_2ONO~+都会对其衰减产生影响。此外，4-PCB…OH加合物还能够发生自身衰减。与H~+、H_2ONO~+的作用将导致羟基化合物的生成，与HONO的作用将导致硝基化合物的生成。
冰相中联苯与H_2O_2光化学反应的主要研究结论如下：
(1)在冰相中联苯与H_2O_2同样能够发生光化学反应。但是，由于联苯被分隔在冰内部的晶界位置，H_2O_2则处于晶格中，两者不能有效的接触，只能通过~·OH在晶格中的扩散才有机会碰撞并发生反应，冰相的反应速率较之液相以及过冷液大幅下降。
(2)冰内部存在的有机物(如：异丙醇、乙酸、丙酮等)主要分布于冰内部的QLL中，因此，对~·OH的淬灭现象不明显。相反，有机物不仅可以与联苯发生传能作用，促进联苯的直接光解，还可导致冰中QLL分数的提高，加速联苯的降解。
以上研究结论将为联苯、4-氯联苯乃至多氯联苯等有机污染物在环境中发生的光化学转化提供重要的参考数据。
The fate of polychlorinated biphenyls in the environment constituted one oftoday's public environmental concerns in respect that they are recognized as one kindof persistent organic pollutants.Condensed water,eg.river,lake,sea,clouds,rain,fog,ice,and snow,is abundant in environment.The study on the reactions ofbiphenyl/4-chlorobiphenyl in environmental condensed water would facilitate thethorough understanding of the sink of polychlorinated biphenyls in environment.Nanosecond laser photolysis/transient absorption spectroscopic technique,togetherwith HPLC-UV and GC-MS, are employed to investigate photo-inducedtransformation mechanism of biphenyl/4-chlorobiphenyl.N(Ⅲ) and H_2O_2 are selectedas ~·OH precusor in liquid phase and in ice phase respectively.According to theassignment of transient species combined with the analysis of products distributions,the biphenyl/4-chlorobiphenyl reaction mechanism is proposed.
Based on the experiment on the photochemical reaction between biphenyl(4-chlorobiphenyl) and N(Ⅲ),the following points could be drawn:
(1) Both biphenyl and 4-chlorobiphenyl would undergo photo-induced reactionin the presence of N(Ⅲ) in aqueous phase.The reactions are initiated by the additionof OH radical,produced from N(Ⅲ) photolysis,to benzene ring.The second-orderreaction rate constants for the reactions of OH radical with biphenyl and4-chlorobiphenyl were determined to be (9.6±0.1)×10~9 L mol~(-1) s~(-1) and (8.0±0.5)×10~9 L mol~(-1) s~(-1) at 298 K,respectively.
(2) It is found that pH value would exert a significant impact on thephotochemical reaction.The decomposition rate of biphenyl and 4-chlorobiphenylslows down with pH.
(3) The decay of Bp…OH adduct and 4-PCB…OH adduct is fairly complicated.H~+,HONO,H_2ONO~+ are found to be capable of reacting with Bp…OH adduct and4-PCB…OH adduct.In addition,4-PCB…OH adduct can also undergo self decay.The reactions of Bp…OH adduct and 4-PCB…OH adduct with H~+,H_2ONO~+ are morelikely to produce hydroxylated compounds,while the reactions with HONO toproduce nitrate ones.
Based on the experiment on the photochemical reaction between biphenyl(4-chlorobiphenyl) and H_2O_2 in ice,following conclusions could be drawn:
(1) The photochemical reaction between biphenyl and H_2O_2 could also take placein ice phase.Since biphenyl is mainly located on grain boundary and H_2O_2 are locatedin bulk ice,the reaction rate is fairly slow as compared with that in liquid phase andsupercooled water.
(2) Co-exist organic pollutants are concentrated in quasi-liquid layer.Therefore,the scavenge of OH radical in ice phase is not significant.On the contrary,becauseorganic pollutants could not only tranfer energy with biphenyl but also increase theQLL fraction in ice,the degradation of biphenyl is acclerated in ice in the presence ofco-exist organic pollutants.
These conclusions will be helpful to the study on photo-induced transformationof organic pollutants like biphenyl and 4-chlorobiphenyl in environment.
联苯与N(Ⅲ)混合溶液、4-氯联苯与N(Ⅲ)混合溶液光化学反应的主要研究结论如下：
(1)联苯与N(Ⅲ)混合溶液、4-氯联苯与N(Ⅲ)混合溶液在紫外光的作用下均能够发生明显的反应。反应都起始于它们与N(Ⅲ)光解产生的~·OH之间的加成作用。实验测得的二级反应速率常数分别为(9．6±0．1)×10~9L mol~(-1) s~(-1)(298 K)、(8．0±0．5)×10~9 Lmol~(-1)s~(-1)(298 K)。
(2)pH值对于联苯、4-氯联苯的降解效率影响显著，pH值越高，联苯、4-氯联苯的降解速率越慢。
(3)~·OH加合产物Bp…OH加合物、4-PCB…OH加合物的衰减均较为复杂。溶液中存在的H~+、HONO、H_2ONO~+都会对其衰减产生影响。此外，4-PCB…OH加合物还能够发生自身衰减。与H~+、H_2ONO~+的作用将导致羟基化合物的生成，与HONO的作用将导致硝基化合物的生成。
冰相中联苯与H_2O_2光化学反应的主要研究结论如下：
(1)在冰相中联苯与H_2O_2同样能够发生光化学反应。但是，由于联苯被分隔在冰内部的晶界位置，H_2O_2则处于晶格中，两者不能有效的接触，只能通过~·OH在晶格中的扩散才有机会碰撞并发生反应，冰相的反应速率较之液相以及过冷液大幅下降。
(2)冰内部存在的有机物(如：异丙醇、乙酸、丙酮等)主要分布于冰内部的QLL中，因此，对~·OH的淬灭现象不明显。相反，有机物不仅可以与联苯发生传能作用，促进联苯的直接光解，还可导致冰中QLL分数的提高，加速联苯的降解。
以上研究结论将为联苯、4-氯联苯乃至多氯联苯等有机污染物在环境中发生的光化学转化提供重要的参考数据。
The fate of polychlorinated biphenyls in the environment constituted one oftoday's public environmental concerns in respect that they are recognized as one kindof persistent organic pollutants.Condensed water,eg.river,lake,sea,clouds,rain,fog,ice,and snow,is abundant in environment.The study on the reactions ofbiphenyl/4-chlorobiphenyl in environmental condensed water would facilitate thethorough understanding of the sink of polychlorinated biphenyls in environment.Nanosecond laser photolysis/transient absorption spectroscopic technique,togetherwith HPLC-UV and GC-MS, are employed to investigate photo-inducedtransformation mechanism of biphenyl/4-chlorobiphenyl.N(Ⅲ) and H_2O_2 are selectedas ~·OH precusor in liquid phase and in ice phase respectively.According to theassignment of transient species combined with the analysis of products distributions,the biphenyl/4-chlorobiphenyl reaction mechanism is proposed.
Based on the experiment on the photochemical reaction between biphenyl(4-chlorobiphenyl) and N(Ⅲ),the following points could be drawn:
(1) Both biphenyl and 4-chlorobiphenyl would undergo photo-induced reactionin the presence of N(Ⅲ) in aqueous phase.The reactions are initiated by the additionof OH radical,produced from N(Ⅲ) photolysis,to benzene ring.The second-orderreaction rate constants for the reactions of OH radical with biphenyl and4-chlorobiphenyl were determined to be (9.6±0.1)×10~9 L mol~(-1) s~(-1) and (8.0±0.5)×10~9 L mol~(-1) s~(-1) at 298 K,respectively.
(2) It is found that pH value would exert a significant impact on thephotochemical reaction.The decomposition rate of biphenyl and 4-chlorobiphenylslows down with pH.
(3) The decay of Bp…OH adduct and 4-PCB…OH adduct is fairly complicated.H~+,HONO,H_2ONO~+ are found to be capable of reacting with Bp…OH adduct and4-PCB…OH adduct.In addition,4-PCB…OH adduct can also undergo self decay.The reactions of Bp…OH adduct and 4-PCB…OH adduct with H~+,H_2ONO~+ are morelikely to produce hydroxylated compounds,while the reactions with HONO toproduce nitrate ones.
Based on the experiment on the photochemical reaction between biphenyl(4-chlorobiphenyl) and H_2O_2 in ice,following conclusions could be drawn:
(1) The photochemical reaction between biphenyl and H_2O_2 could also take placein ice phase.Since biphenyl is mainly located on grain boundary and H_2O_2 are locatedin bulk ice,the reaction rate is fairly slow as compared with that in liquid phase andsupercooled water.
(2) Co-exist organic pollutants are concentrated in quasi-liquid layer.Therefore,the scavenge of OH radical in ice phase is not significant.On the contrary,becauseorganic pollutants could not only tranfer energy with biphenyl but also increase theQLL fraction in ice,the degradation of biphenyl is acclerated in ice in the presence ofco-exist organic pollutants.
These conclusions will be helpful to the study on photo-induced transformationof organic pollutants like biphenyl and 4-chlorobiphenyl in environment.
引文
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