本文主要研究内容
作者付文洋（2019）在《Pd基纳米材料电催化脱氯反应决速步骤识别及效能调控研究》一文中研究指出：氯酚是一种持久性的有机污染物,具有毒性,致癌性,生物富集性等特点。常用作杀虫剂,除草剂以及除菌剂。人们在生产生活中大量使用氯酚,使其在环境中迁移富集污染水体,导致严重的水环境污染问题,对生态环境和人类健康造成危害。所以,发展高效、对环境友好的处理氯酚的技术很有必要。目前,电催化脱氯技术是比较新兴的处理氯酚的有效技术。相比于传统的处理氯酚的技术,电催化脱氯技术具有高效,二次污染风险小,操作简单的特点,是一种比较有发展前景的新技术。金属钯(Pd)对氢具有较强的束缚作用,能产生强还原性的活性氢(H~*)物种,所以Pd常被用做电催化脱氯技术的催化剂。根据Pd基纳米材料电催化脱氯反应中效能较低的问题,本文重点对Pd基纳米材料电催化脱氯反应中决速步骤的识别和反应效能的优化进行了研究。首先,通过研究比较TiN-Pd和C-Pd电极上电催化脱氯(EHDC)反应,发现苯酚(P)的脱附是Pd基纳米材料EHDC反应的决速步骤。本文选取的典型氯酚污染物是2,4-二氯苯酚(2,4-DCP)。通过实验和DFT计算相结合的方法考察比较了TiN-Pd和C-Pd的EHDC效率,H*的产生量以及对2,4-DCP和P的吸附行为,发现P通过与2,4-DCP竞争吸附位点导致催化剂中毒,从而确定了P的脱附是EHDC反应的决速步骤。另外,与碳黑(C)载体相比,氮化钛(TiN)通过降低Pd的d band centre,削弱其与P的吸附强度,P更容易脱附,减轻Pd的中毒现象,提高EHDC效率。因此,Pd的d band centre具有作为描述EHDC效率的潜力,并且利用d band centre综合考虑2,4-DCP吸附和P脱附是增强EHDC效率的有效策略。但是,TiN-Pd上的EHDC电流效率比C-Pd略低,说明虽然TiN-Pd缓解了P的毒化作用,增强了EHDC效率,但是没有降低能耗。针对Pd基纳米材料EHDC反应的能耗问题,本文研究利用载体的协同作用,来提高电催化脱氯反应的效能。首先,研究了制备MgAlLDH-Pd电催化剂的方法。探究了不同pH对MgAlLDH-Pd和C-Pd电催化脱氯反应的影响,发现MgAlLDH利用静电作用和络合作用协同吸附2,4-DCP,增强了Pd纳米颗粒(Pd NPs)对2,4-DCP的有效吸附,提高了EHDC反应效能。其次,探究了不同电压对MgAlLDH-Pd和C-Pd电催化脱氯反应的影响,发现MgAlLDH利用自身带正电的特性,减弱了阴极电场线对离子化的2,4-DCP的排斥作用,加快了2,4-DCP的传质,增强了Pd NPs对2,4-DCP的有效吸,提升了MgAlLDH-Pd的EHDC反应效能。最后,比较MgAlLDH-Pd和C-Pd电极上HER副反应的影响,其结果显示MgAlLDH-Pd削弱了HER副反应,这对提升电流效率,减少能耗有贡献。因此,证明利用载体的协同效应能达到提高Pd NPs电催化脱氯效能的目的。本文通过对Pd基纳米材料电催化脱氯反应中决速步骤识别和效能调控进行研究得到的结论,有助于其他研究者研发性能优异的电催化脱氯催化剂,实现电催化脱氯技术在废水处理中的高效应用。
Abstract
lv fen shi yi chong chi jiu xing de you ji wu ran wu ,ju you du xing ,zhi ai xing ,sheng wu fu ji xing deng te dian 。chang yong zuo sha chong ji ,chu cao ji yi ji chu jun ji 。ren men zai sheng chan sheng huo zhong da liang shi yong lv fen ,shi ji zai huan jing zhong qian yi fu ji wu ran shui ti ,dao zhi yan chong de shui huan jing wu ran wen ti ,dui sheng tai huan jing he ren lei jian kang zao cheng wei hai 。suo yi ,fa zhan gao xiao 、dui huan jing you hao de chu li lv fen de ji shu hen you bi yao 。mu qian ,dian cui hua tuo lv ji shu shi bi jiao xin xing de chu li lv fen de you xiao ji shu 。xiang bi yu chuan tong de chu li lv fen de ji shu ,dian cui hua tuo lv ji shu ju you gao xiao ,er ci wu ran feng xian xiao ,cao zuo jian chan de te dian ,shi yi chong bi jiao you fa zhan qian jing de xin ji shu 。jin shu ba (Pd)dui qing ju you jiao jiang de shu fu zuo yong ,neng chan sheng jiang hai yuan xing de huo xing qing (H~*)wu chong ,suo yi Pdchang bei yong zuo dian cui hua tuo lv ji shu de cui hua ji 。gen ju Pdji na mi cai liao dian cui hua tuo lv fan ying zhong xiao neng jiao di de wen ti ,ben wen chong dian dui Pdji na mi cai liao dian cui hua tuo lv fan ying zhong jue su bu zhou de shi bie he fan ying xiao neng de you hua jin hang le yan jiu 。shou xian ,tong guo yan jiu bi jiao TiN-Pdhe C-Pddian ji shang dian cui hua tuo lv (EHDC)fan ying ,fa xian ben fen (P)de tuo fu shi Pdji na mi cai liao EHDCfan ying de jue su bu zhou 。ben wen shua qu de dian xing lv fen wu ran wu shi 2,4-er lv ben fen (2,4-DCP)。tong guo shi yan he DFTji suan xiang jie ge de fang fa kao cha bi jiao le TiN-Pdhe C-Pdde EHDCxiao lv ,H*de chan sheng liang yi ji dui 2,4-DCPhe Pde xi fu hang wei ,fa xian Ptong guo yu 2,4-DCPjing zheng xi fu wei dian dao zhi cui hua ji zhong du ,cong er que ding le Pde tuo fu shi EHDCfan ying de jue su bu zhou 。ling wai ,yu tan hei (C)zai ti xiang bi ,dan hua tai (TiN)tong guo jiang di Pdde d band centre,xiao ruo ji yu Pde xi fu jiang du ,Pgeng rong yi tuo fu ,jian qing Pdde zhong du xian xiang ,di gao EHDCxiao lv 。yin ci ,Pdde d band centreju you zuo wei miao shu EHDCxiao lv de qian li ,bing ju li yong d band centrezeng ge kao lv 2,4-DCPxi fu he Ptuo fu shi zeng jiang EHDCxiao lv de you xiao ce lve 。dan shi ,TiN-Pdshang de EHDCdian liu xiao lv bi C-Pdlve di ,shui ming sui ran TiN-Pdhuan jie le Pde du hua zuo yong ,zeng jiang le EHDCxiao lv ,dan shi mei you jiang di neng hao 。zhen dui Pdji na mi cai liao EHDCfan ying de neng hao wen ti ,ben wen yan jiu li yong zai ti de xie tong zuo yong ,lai di gao dian cui hua tuo lv fan ying de xiao neng 。shou xian ,yan jiu le zhi bei MgAlLDH-Pddian cui hua ji de fang fa 。tan jiu le bu tong pHdui MgAlLDH-Pdhe C-Pddian cui hua tuo lv fan ying de ying xiang ,fa xian MgAlLDHli yong jing dian zuo yong he lao ge zuo yong xie tong xi fu 2,4-DCP,zeng jiang le Pdna mi ke li (Pd NPs)dui 2,4-DCPde you xiao xi fu ,di gao le EHDCfan ying xiao neng 。ji ci ,tan jiu le bu tong dian ya dui MgAlLDH-Pdhe C-Pddian cui hua tuo lv fan ying de ying xiang ,fa xian MgAlLDHli yong zi shen dai zheng dian de te xing ,jian ruo le yin ji dian chang xian dui li zi hua de 2,4-DCPde pai chi zuo yong ,jia kuai le 2,4-DCPde chuan zhi ,zeng jiang le Pd NPsdui 2,4-DCPde you xiao xi ,di sheng le MgAlLDH-Pdde EHDCfan ying xiao neng 。zui hou ,bi jiao MgAlLDH-Pdhe C-Pddian ji shang HERfu fan ying de ying xiang ,ji jie guo xian shi MgAlLDH-Pdxiao ruo le HERfu fan ying ,zhe dui di sheng dian liu xiao lv ,jian shao neng hao you gong suo 。yin ci ,zheng ming li yong zai ti de xie tong xiao ying neng da dao di gao Pd NPsdian cui hua tuo lv xiao neng de mu de 。ben wen tong guo dui Pdji na mi cai liao dian cui hua tuo lv fan ying zhong jue su bu zhou shi bie he xiao neng diao kong jin hang yan jiu de dao de jie lun ,you zhu yu ji ta yan jiu zhe yan fa xing neng you yi de dian cui hua tuo lv cui hua ji ,shi xian dian cui hua tuo lv ji shu zai fei shui chu li zhong de gao xiao ying yong 。
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论文作者分别是来自重庆工商大学的付文洋，发表于刊物重庆工商大学2019-06-28论文，是一篇关于电催化脱氯论文,决速步骤识别论文,效能优化论文,重庆工商大学2019-06-28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，资料来自重庆工商大学2019-06-28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：电催化脱氯论文; 决速步骤识别论文; 效能优化论文; 重庆工商大学2019-06-28论文;