本文主要研究内容
作者孙吉俊(2019)在《溶解性有机物对冰相中蒽和芘光降解的影响》一文中研究指出:随着十八届三中全会的召开,中国正式进入2.0时代,如今的中国以工业产值进行计算,中国已经成为全球最大的工业国。城市汽车尾气、大量化石燃料燃烧及固体废弃物的处理不当等状况,造成了大量的有机废物(HOCs)进入环境介质中,PAHs属于典型有机废物,具有“三致效应”和遗传毒性,并且因其憎水性,能够在环境介质中不断累积,能够对人类造成不可忽视的深远影响。溶解性有机质(Dissolved organic matter,DOM)由动植物残体经过一系列腐烂矿化过程形成的组成和结构非常复杂的有机物质,对于各种生态系统的调节具有不可忽视的作用。研究表明,DOM与HOCs能够产生复杂的结合作用和吸附行为,能够降低HOCs的浓度,同时对PAHs这类有机废物的分布、迁移、转化、光降解和生物降解以及生物毒性等都具有重要作用。目前大部分研究主要集中HOCs在水介质中的光降解,忽略了对冰相条件下的光降解研究。与流动性的大气、水体等环境介质相比较,污染物在冰体内的物理迁移过程、常规化学反应以及微生物作用都相对较弱,反而光化学作用却表现出显著作用。研究冰相中不同来源DOM对PAHs的光降解影响,不仅有助于了解冰相中DOM的光化学性质,而且了解寒冷环境下的碳生物地球化学也具有重要意义。本文通过以来自于水源和陆源两大类的DOM,水源DOM:Suwannee River Fulvic Acid Standard II(SRFA)、Upper Mississippi River NOM(UMRN);来源于陆源DOM:Elliott Soil Humic Acid Standard IV(ESHA)、Leonardite Humic Acid Standard(LHA)以及典型多环芳烃的代表蒽和芘为研究对象,利用125 W自镇流高压汞灯为模拟光源进行室内模拟光解实验,探究冰相下溶解性有机物对蒽和芘光降解的影响。利用高效液相色谱、紫外光谱与荧光光谱以及同步荧光法综合分析,得到溶解性有机物在冰相中对蒽和芘光解影响的相关结论如下:冰相中蒽和芘均可以发生直接光降解,同时当DOM与蒽和芘混合光解时,DOM会对蒽和芘产生光屏蔽效应。水源DOM和陆源DOM的明显区别在于紫外吸收能力方面,尤其在230-500nm区间,陆源DOM的紫外吸收能力强于水源DOM。整体来看,不同来源的天然DOM在冰相中对污染物的影响程度以及作用效果并不相同,水源DOM在冰相中对污染物的影响程度小于陆源DOM在冰相中对污染物的影响程度。在冰相中不同来源DOM对污染物的光解抑制机制整体以光屏蔽效应为主。冰相中不同来源DOM对蒽与芘的光解促进机制中·OH促进效果高于1O2。不同来源DOM的分子结构等不同,直接导致同一活性氧物种在不同DOM中对同一污染物的促进效果存在显著差异,同一活性氧物质在冰相光解过程中对芘的促进效果强于蒽的促进效果。从两种活性氧物质的贡献程度来看,陆源DOM所具有的的发色基团含量明显高于水源DOM。通过考察发现,在冰相中DOM对污染物降解的促进作用机制仍然主要依赖于活性氧物质的贡献程度。在抑制机制中的淬灭作用程度分析中,从荧光光谱图中发现当DOM加入后蒽和芘的荧光强度均发生了降低,但降低程度不同。4种不同来源DOM对蒽和芘均产生了淬灭作用,并且相同DOM对蒽的激发态淬灭程度明显高于对芘的激发态淬灭。当光解过程DOM对污染物的淬灭程度越大时,表观光解常数越小,抑制程度越强。从结合常数角度分析,对于蒽来说,·OH在冰相中对DOM与污染物的结合作用影响并不显著。对于芘来说,由于1O2减弱DOM的芳香性,进而间接减弱分子的极性,所以可以减小DOM与蒽和芘的结合能力,降低淬灭作用效果,其中1O2对水源DOM影响程度稍强于陆源DOM。·OH对于芘在冰相中光解来说,是可以起到很好的促进作用,并且该促进作用强于DOM对其淬灭作用。两种水源DOM在与蒽和芘光解过程中,静态淬灭相较于动态淬灭而言更明显;而对于另外两种陆源DOM,动态淬灭更为突出。整体分析来看,对于多环芳烃这种污染物来说,在冰相中DOM对其光解的淬灭作用应为动静态联合淬灭机制。在紫外指标分析过程中,SUVA与a254和EET/EBZ之间均存在显著相关,其中对于芘来说EET/EBZ和a254存在极显著相关性。由此可见,冰相中DOM对蒽和芘的光解过程,取代程度和自然取代可能性与含C=C和C=O的芳香族化合物含量以及DOM的芳香程度和腐殖化程度具有很好的相关性。与DOM共存条件下冰相中芘的表观光解速率常数与DOM的SUVA值具有极显著正相关性(P<0.01)。冰相中不同来源DOM对芘光解影响过程中,DOM对芘光解影响程度与DOM的碳含量、芳香程度以及腐殖化程度相同,DOM腐殖化程度或者芳香程度越高,DOM对污染物的抑制程度越强。
Abstract
sui zhao shi ba jie san zhong quan hui de shao kai ,zhong guo zheng shi jin ru 2.0shi dai ,ru jin de zhong guo yi gong ye chan zhi jin hang ji suan ,zhong guo yi jing cheng wei quan qiu zui da de gong ye guo 。cheng shi qi che wei qi 、da liang hua dan ran liao ran shao ji gu ti fei qi wu de chu li bu dang deng zhuang kuang ,zao cheng le da liang de you ji fei wu (HOCs)jin ru huan jing jie zhi zhong ,PAHsshu yu dian xing you ji fei wu ,ju you “san zhi xiao ying ”he wei chuan du xing ,bing ju yin ji zeng shui xing ,neng gou zai huan jing jie zhi zhong bu duan lei ji ,neng gou dui ren lei zao cheng bu ke hu shi de shen yuan ying xiang 。rong jie xing you ji zhi (Dissolved organic matter,DOM)you dong zhi wu can ti jing guo yi ji lie fu lan kuang hua guo cheng xing cheng de zu cheng he jie gou fei chang fu za de you ji wu zhi ,dui yu ge chong sheng tai ji tong de diao jie ju you bu ke hu shi de zuo yong 。yan jiu biao ming ,DOMyu HOCsneng gou chan sheng fu za de jie ge zuo yong he xi fu hang wei ,neng gou jiang di HOCsde nong du ,tong shi dui PAHszhe lei you ji fei wu de fen bu 、qian yi 、zhuai hua 、guang jiang jie he sheng wu jiang jie yi ji sheng wu du xing deng dou ju you chong yao zuo yong 。mu qian da bu fen yan jiu zhu yao ji zhong HOCszai shui jie zhi zhong de guang jiang jie ,hu lve le dui bing xiang tiao jian xia de guang jiang jie yan jiu 。yu liu dong xing de da qi 、shui ti deng huan jing jie zhi xiang bi jiao ,wu ran wu zai bing ti nei de wu li qian yi guo cheng 、chang gui hua xue fan ying yi ji wei sheng wu zuo yong dou xiang dui jiao ruo ,fan er guang hua xue zuo yong que biao xian chu xian zhe zuo yong 。yan jiu bing xiang zhong bu tong lai yuan DOMdui PAHsde guang jiang jie ying xiang ,bu jin you zhu yu le jie bing xiang zhong DOMde guang hua xue xing zhi ,er ju le jie han leng huan jing xia de tan sheng wu de qiu hua xue ye ju you chong yao yi yi 。ben wen tong guo yi lai zi yu shui yuan he liu yuan liang da lei de DOM,shui yuan DOM:Suwannee River Fulvic Acid Standard II(SRFA)、Upper Mississippi River NOM(UMRN);lai yuan yu liu yuan DOM:Elliott Soil Humic Acid Standard IV(ESHA)、Leonardite Humic Acid Standard(LHA)yi ji dian xing duo huan fang ting de dai biao en he pi wei yan jiu dui xiang ,li yong 125 Wzi zhen liu gao ya gong deng wei mo ni guang yuan jin hang shi nei mo ni guang jie shi yan ,tan jiu bing xiang xia rong jie xing you ji wu dui en he pi guang jiang jie de ying xiang 。li yong gao xiao ye xiang se pu 、zi wai guang pu yu ying guang guang pu yi ji tong bu ying guang fa zeng ge fen xi ,de dao rong jie xing you ji wu zai bing xiang zhong dui en he pi guang jie ying xiang de xiang guan jie lun ru xia :bing xiang zhong en he pi jun ke yi fa sheng zhi jie guang jiang jie ,tong shi dang DOMyu en he pi hun ge guang jie shi ,DOMhui dui en he pi chan sheng guang bing bi xiao ying 。shui yuan DOMhe liu yuan DOMde ming xian ou bie zai yu zi wai xi shou neng li fang mian ,you ji zai 230-500nmou jian ,liu yuan DOMde zi wai xi shou neng li jiang yu shui yuan DOM。zheng ti lai kan ,bu tong lai yuan de tian ran DOMzai bing xiang zhong dui wu ran wu de ying xiang cheng du yi ji zuo yong xiao guo bing bu xiang tong ,shui yuan DOMzai bing xiang zhong dui wu ran wu de ying xiang cheng du xiao yu liu yuan DOMzai bing xiang zhong dui wu ran wu de ying xiang cheng du 。zai bing xiang zhong bu tong lai yuan DOMdui wu ran wu de guang jie yi zhi ji zhi zheng ti yi guang bing bi xiao ying wei zhu 。bing xiang zhong bu tong lai yuan DOMdui en yu pi de guang jie cu jin ji zhi zhong ·OHcu jin xiao guo gao yu 1O2。bu tong lai yuan DOMde fen zi jie gou deng bu tong ,zhi jie dao zhi tong yi huo xing yang wu chong zai bu tong DOMzhong dui tong yi wu ran wu de cu jin xiao guo cun zai xian zhe cha yi ,tong yi huo xing yang wu zhi zai bing xiang guang jie guo cheng zhong dui pi de cu jin xiao guo jiang yu en de cu jin xiao guo 。cong liang chong huo xing yang wu zhi de gong suo cheng du lai kan ,liu yuan DOMsuo ju you de de fa se ji tuan han liang ming xian gao yu shui yuan DOM。tong guo kao cha fa xian ,zai bing xiang zhong DOMdui wu ran wu jiang jie de cu jin zuo yong ji zhi reng ran zhu yao yi lai yu huo xing yang wu zhi de gong suo cheng du 。zai yi zhi ji zhi zhong de cui mie zuo yong cheng du fen xi zhong ,cong ying guang guang pu tu zhong fa xian dang DOMjia ru hou en he pi de ying guang jiang du jun fa sheng le jiang di ,dan jiang di cheng du bu tong 。4chong bu tong lai yuan DOMdui en he pi jun chan sheng le cui mie zuo yong ,bing ju xiang tong DOMdui en de ji fa tai cui mie cheng du ming xian gao yu dui pi de ji fa tai cui mie 。dang guang jie guo cheng DOMdui wu ran wu de cui mie cheng du yue da shi ,biao guan guang jie chang shu yue xiao ,yi zhi cheng du yue jiang 。cong jie ge chang shu jiao du fen xi ,dui yu en lai shui ,·OHzai bing xiang zhong dui DOMyu wu ran wu de jie ge zuo yong ying xiang bing bu xian zhe 。dui yu pi lai shui ,you yu 1O2jian ruo DOMde fang xiang xing ,jin er jian jie jian ruo fen zi de ji xing ,suo yi ke yi jian xiao DOMyu en he pi de jie ge neng li ,jiang di cui mie zuo yong xiao guo ,ji zhong 1O2dui shui yuan DOMying xiang cheng du shao jiang yu liu yuan DOM。·OHdui yu pi zai bing xiang zhong guang jie lai shui ,shi ke yi qi dao hen hao de cu jin zuo yong ,bing ju gai cu jin zuo yong jiang yu DOMdui ji cui mie zuo yong 。liang chong shui yuan DOMzai yu en he pi guang jie guo cheng zhong ,jing tai cui mie xiang jiao yu dong tai cui mie er yan geng ming xian ;er dui yu ling wai liang chong liu yuan DOM,dong tai cui mie geng wei tu chu 。zheng ti fen xi lai kan ,dui yu duo huan fang ting zhe chong wu ran wu lai shui ,zai bing xiang zhong DOMdui ji guang jie de cui mie zuo yong ying wei dong jing tai lian ge cui mie ji zhi 。zai zi wai zhi biao fen xi guo cheng zhong ,SUVAyu a254he EET/EBZzhi jian jun cun zai xian zhe xiang guan ,ji zhong dui yu pi lai shui EET/EBZhe a254cun zai ji xian zhe xiang guan xing 。you ci ke jian ,bing xiang zhong DOMdui en he pi de guang jie guo cheng ,qu dai cheng du he zi ran qu dai ke neng xing yu han C=Che C=Ode fang xiang zu hua ge wu han liang yi ji DOMde fang xiang cheng du he fu shi hua cheng du ju you hen hao de xiang guan xing 。yu DOMgong cun tiao jian xia bing xiang zhong pi de biao guan guang jie su lv chang shu yu DOMde SUVAzhi ju you ji xian zhe zheng xiang guan xing (P<0.01)。bing xiang zhong bu tong lai yuan DOMdui pi guang jie ying xiang guo cheng zhong ,DOMdui pi guang jie ying xiang cheng du yu DOMde tan han liang 、fang xiang cheng du yi ji fu shi hua cheng du xiang tong ,DOMfu shi hua cheng du huo zhe fang xiang cheng du yue gao ,DOMdui wu ran wu de yi zhi cheng du yue jiang 。
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论文作者分别是来自辽宁大学的孙吉俊,发表于刊物辽宁大学2019-09-05论文,是一篇关于冰相论文,光解论文,抑制机制论文,辽宁大学2019-09-05论文的文章。本文可供学术参考使用,各位学者可以免费参考阅读下载,文章观点不代表本站观点,资料来自辽宁大学2019-09-05论文网站,若本站收录的文献无意侵犯了您的著作版权,请联系我们删除。
标签:冰相论文; 光解论文; 抑制机制论文; 辽宁大学2019-09-05论文;