黄伟:金属配位作用设计及其在环境化学中的应用研究论文

黄伟:金属配位作用设计及其在环境化学中的应用研究论文

本文主要研究内容

作者黄伟(2019)在《金属配位作用设计及其在环境化学中的应用研究》一文中研究指出:随着城市化进程的不断加快,污染物的排放量剧增,环境问题日趋加重。不仅包括农业、医疗等人类生产生活导致的病原性污染物,还包括工业化产生的印染废水等难降解污染物,它们以各种方式进入到生态环境体系中。当前,环境污染物的分析检测在很大程度上依赖于复杂的前处理过程,高精端的大型设备进行样品分析,往往难以满足现场的快速检测的要求。并且,野外实验非常容易受到复杂的环境体系和地理环境等干扰,对于痕量物质难以实现高灵敏的选择性识别。而对于环境污染物的处理,也会受到复杂工艺的限制,难以实现对处理材料以及目标污染物的高效回收利用。基于此,开发具有高灵敏度、高分析性能的环境目标物传感平台,设计性能优异、环境友好的环境污染物处理新型材料,逐步建立针对有毒有害难降解环境污染物处理的可持续发展机制,并将其广泛应用在环境化学领域具有重要意义。近年来,金属配位作用的研究在环境化学领域逐渐体现出优势。其金属离子和有机配体不但可以通过各种不同方式进行结合,两者共同作用于环境目标物质,能够产生增强的光学、电化学响应或优异的吸附和催化性能,因此在环境科学领域具有广阔的应用前景。本论文的主要研究内容是基于近几年的研究热点——金属配位化学的几个重要理论基础,包括金属可逆竞争配位调控、金属协调配位调控、金属配位破坏调控。从这三个方面入手,来开展针对环境目标物质的研究。全文共分五个部分,具体如下:第一章绪论本章主要介绍了金属配位化学的背景以及它在环境化学领域的进展。首先,通过其他学者的研究介绍了其在环境目标物质的分析识别和环境污染物后处理上的广泛应用。随后,提出了我们所建立的方法的创新点。第二章基于金属可逆竞争配位设计茜素红(AR)-Tb3+复合物作为比例型比色和荧光双通道探针,结合智能手机检测炭疽生物标志物本章主要基于DPA和茜素红(AR)-Tb3+复合物在硼酸-硼砂盐缓冲溶液中的竞争配位作用,开发了一种新型的比色-荧光双通道探针,检测炭疽生物标志物(吡啶二羧酸,DPA)。通过UV-vis光谱滴定证明AR和Tb3+离子在缓冲液中以3:1的配位形式存在。未添加DPA时,AR-Tb3+复合物的颜色为紫红色并在紫外(UV)灯下显示弱橙色荧光。加入DPA会破坏AR-Tb3+的配位,形成DPA-Tb3+配合物。溶液的颜色从紫红色逐渐变为黄色,同时,在紫外灯照射下DPA-Tb3+发出亮绿色荧光,成功建立比例型比色和荧光双通道检测DPA的平台。与此同时,基于智能手机内置的色彩扫描APP,可将该探针进一步应用于现场快速可视化测定DPA浓度。并且,通过我们开发的新方法可以很便捷地实现对芽孢杆菌释放出的DPA进行快速、灵敏和选择性检测。第三章基于金属协调配位设计可重复利用的磁性无限配位聚合物Fe3O4@Tb/AMP核-壳结构纳米吸附剂用于选择性去除阴离子型染料本章主要基于金属-有机配体和目标物质高度可协调功能,合理地设计出一种可重复利用的新型磁性复合无限配位聚合物Fe3O4@Tb/AMP核-壳结构的纳米吸附剂,开发了一种从有色废水中选择性去除阴离子染料的新技术。将金属离子铽Tb3+用作中心金属节点,腺嘌呤核苷酸AMP作为有机配体与金属节点无限配位形成超分子ICP网络结构壳层;Fe3O4纳米粒子自适应封装在ICP网络中作为核。所制备的磁性核壳结构表现出对阴离子染料的极佳的吸附选择性。最佳吸附条件下,纳米吸附剂表现出极快的吸附性能(5分钟内染料去除率能够达到96%以上),等温线数据与Langmuir模型高度拟合。温度298 K时,最大吸附容量AR(357.14 mg g-1),CR(909.09 mg g-1),且吸附容量随着温度的升高进一步提高。简单的盐/乙醇洗涤就可以使Fe3O4@Tb/AMP核壳纳米粒子再生,并且在5个循环周期内具有很高的重复利用性。磁性Fe3O4@Tb/AMP核壳纳米粒子作为吸附剂,可真正实现有色阴离子染料从有色废水中的选择性去除,这对于染料污染废水处理技术的可持续发展具有重要意义。第四章基于金属配位破坏设计无限配位聚合物{Co(3,5-dbsq)(3,5-dbcat)(bix)}ICP前驱体制备CoOx/GO催化氧化有机难降解废水的机理探究本章主要基于对金属-有机配体破坏调控的原理,电化学极化具有氧化还原活性的{Co(3,5-dbsq)(3,5-dbcat)(bix)}ICP前驱体,在ITO玻璃片层上原位生成CoOx/GO纳米催化剂活化氧化剂Oxone,实时在线监控和处理工业难降解废水。将Co ICP或Co ICP/GO前驱体在0.10 mol L-1的KCl溶液中,-1.1 V电位下极化工作电极1000 s,得到单分散的超小尺寸的CoOx(1.42±0.34 nm)或CoOx/GO(1.21±0.28 nm)纳米粒子,掺杂GO作为载体提供更快的电子传输速率和更强的稳定性。通过对亚甲基蓝(MB)的降解实验证实了CoOx/GO对Oxone的催化活性,并探究其机理。2.0 mL,20 mg L-1的MB溶液在60℃的条件下,4分钟之内就能降解完全,明显优于其他Co催化剂。合成的CoOx/GO有着非常低的活化能,理想的催化和重复利用性能。我们首次以ITO玻璃为原料构建便携式反应池,通过结合紫外/可见光谱仪,可以直接实现对纺织和化妆品工业有色废水催化降解的实时监测。这对于开发在线监测设备,实现工业废水处理过程中的信息采集和过程化控制具有重要意义。

Abstract

sui zhao cheng shi hua jin cheng de bu duan jia kuai ,wu ran wu de pai fang liang ju zeng ,huan jing wen ti ri qu jia chong 。bu jin bao gua nong ye 、yi liao deng ren lei sheng chan sheng huo dao zhi de bing yuan xing wu ran wu ,hai bao gua gong ye hua chan sheng de yin ran fei shui deng nan jiang jie wu ran wu ,ta men yi ge chong fang shi jin ru dao sheng tai huan jing ti ji zhong 。dang qian ,huan jing wu ran wu de fen xi jian ce zai hen da cheng du shang yi lai yu fu za de qian chu li guo cheng ,gao jing duan de da xing she bei jin hang yang pin fen xi ,wang wang nan yi man zu xian chang de kuai su jian ce de yao qiu 。bing ju ,ye wai shi yan fei chang rong yi shou dao fu za de huan jing ti ji he de li huan jing deng gan rao ,dui yu hen liang wu zhi nan yi shi xian gao ling min de shua ze xing shi bie 。er dui yu huan jing wu ran wu de chu li ,ye hui shou dao fu za gong yi de xian zhi ,nan yi shi xian dui chu li cai liao yi ji mu biao wu ran wu de gao xiao hui shou li yong 。ji yu ci ,kai fa ju you gao ling min du 、gao fen xi xing neng de huan jing mu biao wu chuan gan ping tai ,she ji xing neng you yi 、huan jing you hao de huan jing wu ran wu chu li xin xing cai liao ,zhu bu jian li zhen dui you du you hai nan jiang jie huan jing wu ran wu chu li de ke chi xu fa zhan ji zhi ,bing jiang ji an fan ying yong zai huan jing hua xue ling yu ju you chong yao yi yi 。jin nian lai ,jin shu pei wei zuo yong de yan jiu zai huan jing hua xue ling yu zhu jian ti xian chu you shi 。ji jin shu li zi he you ji pei ti bu dan ke yi tong guo ge chong bu tong fang shi jin hang jie ge ,liang zhe gong tong zuo yong yu huan jing mu biao wu zhi ,neng gou chan sheng zeng jiang de guang xue 、dian hua xue xiang ying huo you yi de xi fu he cui hua xing neng ,yin ci zai huan jing ke xue ling yu ju you an kuo de ying yong qian jing 。ben lun wen de zhu yao yan jiu nei rong shi ji yu jin ji nian de yan jiu re dian ——jin shu pei wei hua xue de ji ge chong yao li lun ji chu ,bao gua jin shu ke ni jing zheng pei wei diao kong 、jin shu xie diao pei wei diao kong 、jin shu pei wei po huai diao kong 。cong zhe san ge fang mian ru shou ,lai kai zhan zhen dui huan jing mu biao wu zhi de yan jiu 。quan wen gong fen wu ge bu fen ,ju ti ru xia :di yi zhang xu lun ben zhang zhu yao jie shao le jin shu pei wei hua xue de bei jing yi ji ta zai huan jing hua xue ling yu de jin zhan 。shou xian ,tong guo ji ta xue zhe de yan jiu jie shao le ji zai huan jing mu biao wu zhi de fen xi shi bie he huan jing wu ran wu hou chu li shang de an fan ying yong 。sui hou ,di chu le wo men suo jian li de fang fa de chuang xin dian 。di er zhang ji yu jin shu ke ni jing zheng pei wei she ji qian su gong (AR)-Tb3+fu ge wu zuo wei bi li xing bi se he ying guang shuang tong dao tan zhen ,jie ge zhi neng shou ji jian ce tan ju sheng wu biao zhi wu ben zhang zhu yao ji yu DPAhe qian su gong (AR)-Tb3+fu ge wu zai peng suan -peng sha yan huan chong rong ye zhong de jing zheng pei wei zuo yong ,kai fa le yi chong xin xing de bi se -ying guang shuang tong dao tan zhen ,jian ce tan ju sheng wu biao zhi wu (bi ding er suo suan ,DPA)。tong guo UV-visguang pu di ding zheng ming ARhe Tb3+li zi zai huan chong ye zhong yi 3:1de pei wei xing shi cun zai 。wei tian jia DPAshi ,AR-Tb3+fu ge wu de yan se wei zi gong se bing zai zi wai (UV)deng xia xian shi ruo cheng se ying guang 。jia ru DPAhui po huai AR-Tb3+de pei wei ,xing cheng DPA-Tb3+pei ge wu 。rong ye de yan se cong zi gong se zhu jian bian wei huang se ,tong shi ,zai zi wai deng zhao she xia DPA-Tb3+fa chu liang lu se ying guang ,cheng gong jian li bi li xing bi se he ying guang shuang tong dao jian ce DPAde ping tai 。yu ci tong shi ,ji yu zhi neng shou ji nei zhi de se cai sao miao APP,ke jiang gai tan zhen jin yi bu ying yong yu xian chang kuai su ke shi hua ce ding DPAnong du 。bing ju ,tong guo wo men kai fa de xin fang fa ke yi hen bian jie de shi xian dui ya bao gan jun shi fang chu de DPAjin hang kuai su 、ling min he shua ze xing jian ce 。di san zhang ji yu jin shu xie diao pei wei she ji ke chong fu li yong de ci xing mo xian pei wei ju ge wu Fe3O4@Tb/AMPhe -ke jie gou na mi xi fu ji yong yu shua ze xing qu chu yin li zi xing ran liao ben zhang zhu yao ji yu jin shu -you ji pei ti he mu biao wu zhi gao du ke xie diao gong neng ,ge li de she ji chu yi chong ke chong fu li yong de xin xing ci xing fu ge mo xian pei wei ju ge wu Fe3O4@Tb/AMPhe -ke jie gou de na mi xi fu ji ,kai fa le yi chong cong you se fei shui zhong shua ze xing qu chu yin li zi ran liao de xin ji shu 。jiang jin shu li zi te Tb3+yong zuo zhong xin jin shu jie dian ,xian piao ling he gan suan AMPzuo wei you ji pei ti yu jin shu jie dian mo xian pei wei xing cheng chao fen zi ICPwang lao jie gou ke ceng ;Fe3O4na mi li zi zi kuo ying feng zhuang zai ICPwang lao zhong zuo wei he 。suo zhi bei de ci xing he ke jie gou biao xian chu dui yin li zi ran liao de ji jia de xi fu shua ze xing 。zui jia xi fu tiao jian xia ,na mi xi fu ji biao xian chu ji kuai de xi fu xing neng (5fen zhong nei ran liao qu chu lv neng gou da dao 96%yi shang ),deng wen xian shu ju yu Langmuirmo xing gao du ni ge 。wen du 298 Kshi ,zui da xi fu rong liang AR(357.14 mg g-1),CR(909.09 mg g-1),ju xi fu rong liang sui zhao wen du de sheng gao jin yi bu di gao 。jian chan de yan /yi chun xi di jiu ke yi shi Fe3O4@Tb/AMPhe ke na mi li zi zai sheng ,bing ju zai 5ge xun huan zhou ji nei ju you hen gao de chong fu li yong xing 。ci xing Fe3O4@Tb/AMPhe ke na mi li zi zuo wei xi fu ji ,ke zhen zheng shi xian you se yin li zi ran liao cong you se fei shui zhong de shua ze xing qu chu ,zhe dui yu ran liao wu ran fei shui chu li ji shu de ke chi xu fa zhan ju you chong yao yi yi 。di si zhang ji yu jin shu pei wei po huai she ji mo xian pei wei ju ge wu {Co(3,5-dbsq)(3,5-dbcat)(bix)}ICPqian qu ti zhi bei CoOx/GOcui hua yang hua you ji nan jiang jie fei shui de ji li tan jiu ben zhang zhu yao ji yu dui jin shu -you ji pei ti po huai diao kong de yuan li ,dian hua xue ji hua ju you yang hua hai yuan huo xing de {Co(3,5-dbsq)(3,5-dbcat)(bix)}ICPqian qu ti ,zai ITObo li pian ceng shang yuan wei sheng cheng CoOx/GOna mi cui hua ji huo hua yang hua ji Oxone,shi shi zai xian jian kong he chu li gong ye nan jiang jie fei shui 。jiang Co ICPhuo Co ICP/GOqian qu ti zai 0.10 mol L-1de KClrong ye zhong ,-1.1 Vdian wei xia ji hua gong zuo dian ji 1000 s,de dao chan fen san de chao xiao che cun de CoOx(1.42±0.34 nm)huo CoOx/GO(1.21±0.28 nm)na mi li zi ,can za GOzuo wei zai ti di gong geng kuai de dian zi chuan shu su lv he geng jiang de wen ding xing 。tong guo dui ya jia ji lan (MB)de jiang jie shi yan zheng shi le CoOx/GOdui Oxonede cui hua huo xing ,bing tan jiu ji ji li 。2.0 mL,20 mg L-1de MBrong ye zai 60℃de tiao jian xia ,4fen zhong zhi nei jiu neng jiang jie wan quan ,ming xian you yu ji ta Cocui hua ji 。ge cheng de CoOx/GOyou zhao fei chang di de huo hua neng ,li xiang de cui hua he chong fu li yong xing neng 。wo men shou ci yi ITObo li wei yuan liao gou jian bian xie shi fan ying chi ,tong guo jie ge zi wai /ke jian guang pu yi ,ke yi zhi jie shi xian dui fang zhi he hua zhuang pin gong ye you se fei shui cui hua jiang jie de shi shi jian ce 。zhe dui yu kai fa zai xian jian ce she bei ,shi xian gong ye fei shui chu li guo cheng zhong de xin xi cai ji he guo cheng hua kong zhi ju you chong yao yi yi 。

论文参考文献

论文详细介绍

论文作者分别是来自华东师范大学的黄伟,发表于刊物华东师范大学2019-07-02论文,是一篇关于金属配位化学论文,无限配位聚合物论文,环境分析论文,污染物后处理论文,吡啶二羧酸论文,染料废水论文,华东师范大学2019-07-02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,资料来自华东师范大学2019-07-02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。

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黄伟:金属配位作用设计及其在环境化学中的应用研究论文
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