本文主要研究内容
作者王柄凯（2019）在《稀土复合水滑石基非均相催化剂的设计合成及性质研究》一文中研究指出：在催化科学领域,开发具有高活性,高选择性和长稳定性的催化剂是永恒的主题。由于贵金属（如Pd,Pt,Au,Ir及其合金等）在许多催化反应中表现出优于其它催化剂的性能,因此常被用来驱动非均相催化过程。然而,储量稀少及价格高昂等因素限制了它们在工业生产中的大规模应用。针对这一难题,寻求易操作的解决方案成为当前非均相催化领域内的一大热点。目前主流的两类设计思路:一是优化催化剂载体或引入助催化剂,在性能不受影响（甚至有所增强）的前提下,尽可能减少贵金属用量;二是利用纳米工程设计等策略开发储量丰富的过渡金属催化剂用来取代传统贵金属,达到相同甚至超越的催化性能。无论哪种思路,设计新型催化剂载体,助催化剂和催化剂合成方法对非均相催化的发展具有重要的理论意义和应用价值。水滑石（层状双金属氢氧化物,LDHs）是一类阴离子型二维层状化合物。它是由周期性排布的金属((M2+,M3+)（OH）6)八面体形成带正电荷的主层板,阴离子及水分子构成带负电荷的层间通道。在非均相催化领域,水滑石具有以下优点:（1）主层板阳离子种类比例可调,阴离子可交换使LDHs具有灵活的组成通用性;（2）LDHs的高吸附能力使它们成为表面催化活性成分固定的有效载体;（3）M2+和M3+阳离子在层板上的均匀分散,以及层间阴离子的优选取向,为LDHs作为高度稳定分散的多相催化剂提供了前提;（4）LDHs可以与其它材料结合形成具有分级结构的纳米复合物,通过两种材料之间协同效应,进一步提高催化活性和稳定性。由此可见,合理设计和可控制备LDHs基催化剂使其具有高活性和稳定性,具有重要的应用前景。我们课题组长期致力于稀土功能纳米复合材料的研究工作。稀土元素的4f层电子结构,配位数,高储氧容量等独特性质决定了其在催化方面具有重大应用,素有“工业维生素”的美誉。本论文选用水滑石为纳米材料基质,通过引入稀土元素来调控水滑石结构,详细探讨了材料组装策略,研究了该类纳米复合材料作为非均相催化剂在降解有机污染物以及电催化析氧等领域的应用。该研究工作分别从新型催化剂载体设计,新型助催化剂设计,新型催化剂合成方法三个角度开展非均相催化剂的可控合成,性能调控和催化机理研究,为拓宽稀土复合材料在催化领域的应用提供了新思路。本论文工作分为以下五个部分:第一章:简要介绍稀土元素及水滑石在非均相催化领域的研究进展。第二章:钇掺杂的磁性水滑石核壳结构负载纳米金催化有机污染物降解研究。本部分工作通过简单的共沉淀法制备了稀土钇（Y）掺杂的磁性核壳结构作为催化剂载体,负载金（Au）纳米颗粒后,表现出优秀的催化还原对硝基苯酚的能力。磁性的四氧化三铁（Fe3O4）核使得该催化剂可以通过磁铁方便的与反应体系分离,镁铝水滑石（MgAl-LDH）壳层可以提高Au的负载效率,同时有效避免纳米颗粒团聚。更重要的是,稀土Y的掺杂有效调节了催化活性成分的电子结构,从而提高了催化效率。第三章:氧化石墨烯原位生长二氧化铈作为助催化剂的设计合成及其电催化析氧性能研究。在本章工作中,以氧化石墨烯为前体,成功设计并合成了CeNC结构上均匀分布CeO2纳米颗粒。其与剥离的NiFe-LDH组合后,表现出卓越的电催化OER活性及稳定性。在1 M KOH溶液中,当电流密度为10 mA cm-2时,该催化剂的超电势仅为235 mV,性能远超商用20%Ir/C及其它文章报道的Ni基OER催化剂。CeO2@CeNC作为助催化剂在电催化过程中起到了关键性作用。这部分工作为稀土复合高性能电催化剂的开发提供了新思路。第四章:ZIF-67为模板的二氧化铈-水滑石核壳结构催化剂的设计合成及其电催化析氧性能研究。利用自牺牲模板的合成策略构筑了一种新型CeO2@NC/LDH核壳结构催化剂。该催化剂在碱性电解液中表现出了优异的OER催化活性及稳定性。这种高性能主要受益于稀土CeO2的引入,有效调控了催化剂电子态,并形成了更多的缺陷结构。此外,这种表面原位生长的策略也可以防止LDH片层团聚,增加活性位点数量。更重要的是,这种异质核壳结构的合成策略可以被进一步推广,并应用于其它催化领域。第五章:四氧化三铁稳定的镍(NixFe3-xO4)纳米粒子的设计合成及其电催化5-羟甲基糠醛性能研究探索了不同尺寸镍纳米粒子（Ni NPs）作为5-羟甲基糠醛（HMF）电化学氧化催化剂的活性及选择性,证明催化剂存在尺寸效应。针对Ni NPs稳定性差,催化过程中易团聚的不足,合成了镍掺杂四氧化三铁纳米粒子(NixFe3-xO4NPs),以Fe3-xO4基质稳定活性成分Ni。当Ni/Fe比例为1/1时,该催化剂具有最优的HMF转化率及2,5-呋喃二羧酸（FDCA）法拉第效率,与纯Ni NPs活性相近。鉴于水滑石（LDHs）煅烧失水后形成双金属氧化物,猜想LDHs及稀土复合LDHs材料在HMF催化氧化领域也有着潜在的应用。
Abstract
zai cui hua ke xue ling yu ,kai fa ju you gao huo xing ,gao shua ze xing he chang wen ding xing de cui hua ji shi yong heng de zhu ti 。you yu gui jin shu （ru Pd,Pt,Au,Irji ji ge jin deng ）zai hu duo cui hua fan ying zhong biao xian chu you yu ji ta cui hua ji de xing neng ,yin ci chang bei yong lai qu dong fei jun xiang cui hua guo cheng 。ran er ,chu liang xi shao ji jia ge gao ang deng yin su xian zhi le ta men zai gong ye sheng chan zhong de da gui mo ying yong 。zhen dui zhe yi nan ti ,xun qiu yi cao zuo de jie jue fang an cheng wei dang qian fei jun xiang cui hua ling yu nei de yi da re dian 。mu qian zhu liu de liang lei she ji sai lu :yi shi you hua cui hua ji zai ti huo yin ru zhu cui hua ji ,zai xing neng bu shou ying xiang （shen zhi you suo zeng jiang ）de qian di xia ,jin ke neng jian shao gui jin shu yong liang ;er shi li yong na mi gong cheng she ji deng ce lve kai fa chu liang feng fu de guo du jin shu cui hua ji yong lai qu dai chuan tong gui jin shu ,da dao xiang tong shen zhi chao yue de cui hua xing neng 。mo lun na chong sai lu ,she ji xin xing cui hua ji zai ti ,zhu cui hua ji he cui hua ji ge cheng fang fa dui fei jun xiang cui hua de fa zhan ju you chong yao de li lun yi yi he ying yong jia zhi 。shui hua dan （ceng zhuang shuang jin shu qing yang hua wu ,LDHs）shi yi lei yin li zi xing er wei ceng zhuang hua ge wu 。ta shi you zhou ji xing pai bu de jin shu ((M2+,M3+)（OH）6)ba mian ti xing cheng dai zheng dian he de zhu ceng ban ,yin li zi ji shui fen zi gou cheng dai fu dian he de ceng jian tong dao 。zai fei jun xiang cui hua ling yu ,shui hua dan ju you yi xia you dian :（1）zhu ceng ban yang li zi chong lei bi li ke diao ,yin li zi ke jiao huan shi LDHsju you ling huo de zu cheng tong yong xing ;（2）LDHsde gao xi fu neng li shi ta men cheng wei biao mian cui hua huo xing cheng fen gu ding de you xiao zai ti ;（3）M2+he M3+yang li zi zai ceng ban shang de jun yun fen san ,yi ji ceng jian yin li zi de you shua qu xiang ,wei LDHszuo wei gao du wen ding fen san de duo xiang cui hua ji di gong le qian di ;（4）LDHske yi yu ji ta cai liao jie ge xing cheng ju you fen ji jie gou de na mi fu ge wu ,tong guo liang chong cai liao zhi jian xie tong xiao ying ,jin yi bu di gao cui hua huo xing he wen ding xing 。you ci ke jian ,ge li she ji he ke kong zhi bei LDHsji cui hua ji shi ji ju you gao huo xing he wen ding xing ,ju you chong yao de ying yong qian jing 。wo men ke ti zu chang ji zhi li yu xi tu gong neng na mi fu ge cai liao de yan jiu gong zuo 。xi tu yuan su de 4fceng dian zi jie gou ,pei wei shu ,gao chu yang rong liang deng du te xing zhi jue ding le ji zai cui hua fang mian ju you chong da ying yong ,su you “gong ye wei sheng su ”de mei yu 。ben lun wen shua yong shui hua dan wei na mi cai liao ji zhi ,tong guo yin ru xi tu yuan su lai diao kong shui hua dan jie gou ,xiang xi tan tao le cai liao zu zhuang ce lve ,yan jiu le gai lei na mi fu ge cai liao zuo wei fei jun xiang cui hua ji zai jiang jie you ji wu ran wu yi ji dian cui hua xi yang deng ling yu de ying yong 。gai yan jiu gong zuo fen bie cong xin xing cui hua ji zai ti she ji ,xin xing zhu cui hua ji she ji ,xin xing cui hua ji ge cheng fang fa san ge jiao du kai zhan fei jun xiang cui hua ji de ke kong ge cheng ,xing neng diao kong he cui hua ji li yan jiu ,wei ta kuan xi tu fu ge cai liao zai cui hua ling yu de ying yong di gong le xin sai lu 。ben lun wen gong zuo fen wei yi xia wu ge bu fen :di yi zhang :jian yao jie shao xi tu yuan su ji shui hua dan zai fei jun xiang cui hua ling yu de yan jiu jin zhan 。di er zhang :yi can za de ci xing shui hua dan he ke jie gou fu zai na mi jin cui hua you ji wu ran wu jiang jie yan jiu 。ben bu fen gong zuo tong guo jian chan de gong chen dian fa zhi bei le xi tu yi （Y）can za de ci xing he ke jie gou zuo wei cui hua ji zai ti ,fu zai jin （Au）na mi ke li hou ,biao xian chu you xiu de cui hua hai yuan dui xiao ji ben fen de neng li 。ci xing de si yang hua san tie （Fe3O4）he shi de gai cui hua ji ke yi tong guo ci tie fang bian de yu fan ying ti ji fen li ,mei lv shui hua dan （MgAl-LDH）ke ceng ke yi di gao Aude fu zai xiao lv ,tong shi you xiao bi mian na mi ke li tuan ju 。geng chong yao de shi ,xi tu Yde can za you xiao diao jie le cui hua huo xing cheng fen de dian zi jie gou ,cong er di gao le cui hua xiao lv 。di san zhang :yang hua dan mo xi yuan wei sheng chang er yang hua shi zuo wei zhu cui hua ji de she ji ge cheng ji ji dian cui hua xi yang xing neng yan jiu 。zai ben zhang gong zuo zhong ,yi yang hua dan mo xi wei qian ti ,cheng gong she ji bing ge cheng le CeNCjie gou shang jun yun fen bu CeO2na mi ke li 。ji yu bao li de NiFe-LDHzu ge hou ,biao xian chu zhuo yue de dian cui hua OERhuo xing ji wen ding xing 。zai 1 M KOHrong ye zhong ,dang dian liu mi du wei 10 mA cm-2shi ,gai cui hua ji de chao dian shi jin wei 235 mV,xing neng yuan chao shang yong 20%Ir/Cji ji ta wen zhang bao dao de Niji OERcui hua ji 。CeO2@CeNCzuo wei zhu cui hua ji zai dian cui hua guo cheng zhong qi dao le guan jian xing zuo yong 。zhe bu fen gong zuo wei xi tu fu ge gao xing neng dian cui hua ji de kai fa di gong le xin sai lu 。di si zhang :ZIF-67wei mo ban de er yang hua shi -shui hua dan he ke jie gou cui hua ji de she ji ge cheng ji ji dian cui hua xi yang xing neng yan jiu 。li yong zi xi sheng mo ban de ge cheng ce lve gou zhu le yi chong xin xing CeO2@NC/LDHhe ke jie gou cui hua ji 。gai cui hua ji zai jian xing dian jie ye zhong biao xian chu le you yi de OERcui hua huo xing ji wen ding xing 。zhe chong gao xing neng zhu yao shou yi yu xi tu CeO2de yin ru ,you xiao diao kong le cui hua ji dian zi tai ,bing xing cheng le geng duo de que xian jie gou 。ci wai ,zhe chong biao mian yuan wei sheng chang de ce lve ye ke yi fang zhi LDHpian ceng tuan ju ,zeng jia huo xing wei dian shu liang 。geng chong yao de shi ,zhe chong yi zhi he ke jie gou de ge cheng ce lve ke yi bei jin yi bu tui an ,bing ying yong yu ji ta cui hua ling yu 。di wu zhang :si yang hua san tie wen ding de nie (NixFe3-xO4)na mi li zi de she ji ge cheng ji ji dian cui hua 5-qiang jia ji kang quan xing neng yan jiu tan suo le bu tong che cun nie na mi li zi （Ni NPs）zuo wei 5-qiang jia ji kang quan （HMF）dian hua xue yang hua cui hua ji de huo xing ji shua ze xing ,zheng ming cui hua ji cun zai che cun xiao ying 。zhen dui Ni NPswen ding xing cha ,cui hua guo cheng zhong yi tuan ju de bu zu ,ge cheng le nie can za si yang hua san tie na mi li zi (NixFe3-xO4NPs),yi Fe3-xO4ji zhi wen ding huo xing cheng fen Ni。dang Ni/Febi li wei 1/1shi ,gai cui hua ji ju you zui you de HMFzhuai hua lv ji 2,5-fu nan er suo suan （FDCA）fa la di xiao lv ,yu chun Ni NPshuo xing xiang jin 。jian yu shui hua dan （LDHs）duan shao shi shui hou xing cheng shuang jin shu yang hua wu ,cai xiang LDHsji xi tu fu ge LDHscai liao zai HMFcui hua yang hua ling yu ye you zhao qian zai de ying yong 。
论文参考文献
论文详细介绍
论文作者分别是来自兰州大学的王柄凯，发表于刊物兰州大学2019-07-29论文，是一篇关于稀土元素论文,水滑石论文,核壳结构论文,电催化论文,兰州大学2019-07-29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，资料来自兰州大学2019-07-29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：稀土元素论文; 水滑石论文; 核壳结构论文; 电催化论文; 兰州大学2019-07-29论文;