本文主要研究内容
作者惠兰(2019)在《石墨炔基电催化剂的可控制备及催化性能研究》一文中研究指出:石墨炔(graphdiyne,GDY)是一种由sp和sp2两种杂化碳构成的新型碳同素异形体。在石墨炔结构中,1,3-二炔键通过共价链接苯环形成单原子层厚度的二维平面网络结构。基于其特殊的化学结构和电子结构,石墨炔展现出诸多奇特性质,例如,丰富的碳化学键、天然的孔洞结构、高共轭性、天然带隙、以及化学和热稳定性等。这些独特性质使石墨炔在催化、能源、电子等领域展现出巨大的应用潜力和广阔的应用前景。本论文以二维石墨炔为中心,利用石墨炔独特的化学结构和电子结构性质、及其可以在任意基底表面可控合成的性质,从石墨炔的可控合成出发,通过合理设计和精细调控,发展了可控制备石墨炔基异质结构材料的新方法,制备了多种形貌结构可调的石墨炔基异质结构材料,解决了电催化过程中无机纳米催化剂本征活性差、稳定性差等问题,并成功将所制备的石墨炔基异质结构催化剂应用于电催化产氢、电催化产氧等领域中。同时,结合理论计算,重点详细地研究了其电化学性质和电催化反应机理。本论文主要包括以下几个部分内容:第一章,着重阐述了石墨炔的发展历史。从石墨炔的化学结构到电子结构出发,讲述了石墨炔的基本性质;随后重点讲述了石墨炔的合成,并概述了石墨炔基新材料在催化、能源转化和存储材料研究方面取得的重要研究成果。第二章,成功制备出具有多活性中心、多功能的单晶类水滑石材料,对其形貌和结构性质进行了详细的表征。通过电催化解水,对其电催化性能进行了评价。研究表明,对活性中心元素种类及含量的调控,可以对催化剂的形貌以及结构进行有效调节,从而使其性能得到显著改善。此外,通过实验和理论计算相结合明确了其催化水解的机理。第三章,通过对纯类水滑石结构可控地进行非金属元素掺杂的策略,实现了对催化剂结构、形貌的进一步精确调控,显著提升其催化活性和稳定性。详细的XPS、XRD等结构分析结果和密度泛函理论计算结果共同显示,非金属元素的掺杂可以显着提高催化剂的电荷转移能力,从而增强其反应活性,同时增加其反应稳定性。最佳比例得到的材料表现出优异的性能,例如,电流密度10 mA cm-2时的析氢为68 mV,析氧电位为208 mV。被用作全水解的双功能电极时,在1.44V的极低电池电压下电流密度即达到10 mA cm-2,在100 mA cm-2下稳定长达80小时而无衰减。第四章,利用石墨炔可在任意基底表面原位生长的特性,发展了一种原位插层-剥离类水滑石纳米片的方法,首次实现了对自支撑类水滑石纳米片的原位插层—剥离,并构筑了三维“石墨炔—层状双金属氢氧化物—石墨炔”三明治结构纳米片阵列电极(e-ICLDH@GDY/NF)。研究表明,相对于单独的LDH和GDY催化剂,e-ICLDH@GDY/NF具有更为优异的电催化HER、OER和全水解反应活性和稳定性,并通过对复合材料结构的可控调控实现了对电极性能的调控。第五章,成功地在泡沫镍集流体上构筑了超薄石墨炔(GDY)包覆的碱式碳酸铁(FeCH)纳米片阵列电极。研究结果显示,作为三维集成电极,其在碱性电解液中表现出优秀的析氢反应(HER)、析氧反应(OER)活性和稳定性。同时,基于该催化剂的全水解电解池展现出良好的反应活性(仅需1.49 V电池电压即可驱动10 mA cm-2的全水解电流密度)和稳定性。第六章,发展了一种调控二硫化钼晶相的方法,通过在硫化钼纳米片表面原位生长石墨炔纳米片结构,实现了二硫化钼从2H到1T相的转变,显著增加了体系导电性,降低了氢吸附自由能,进而提升了其本征催化活性。电化学研究结果显示,所制备的石墨炔包覆二硫化钼纳米片阵列电极,在全pH(014)范围内都有优异的HER活性和稳定性。尤其是在碱性(pH=14)条件下,该电极的HER活性超过20 wt.%Pt/C;同时瞬态光电流是纯二硫化钼的45.7倍。第七章,本论文的总结与展望。
Abstract
dan mo gui (graphdiyne,GDY)shi yi chong you sphe sp2liang chong za hua tan gou cheng de xin xing tan tong su yi xing ti 。zai dan mo gui jie gou zhong ,1,3-er gui jian tong guo gong jia lian jie ben huan xing cheng chan yuan zi ceng hou du de er wei ping mian wang lao jie gou 。ji yu ji te shu de hua xue jie gou he dian zi jie gou ,dan mo gui zhan xian chu zhu duo ji te xing zhi ,li ru ,feng fu de tan hua xue jian 、tian ran de kong dong jie gou 、gao gong e xing 、tian ran dai xi 、yi ji hua xue he re wen ding xing deng 。zhe xie du te xing zhi shi dan mo gui zai cui hua 、neng yuan 、dian zi deng ling yu zhan xian chu ju da de ying yong qian li he an kuo de ying yong qian jing 。ben lun wen yi er wei dan mo gui wei zhong xin ,li yong dan mo gui du te de hua xue jie gou he dian zi jie gou xing zhi 、ji ji ke yi zai ren yi ji de biao mian ke kong ge cheng de xing zhi ,cong dan mo gui de ke kong ge cheng chu fa ,tong guo ge li she ji he jing xi diao kong ,fa zhan le ke kong zhi bei dan mo gui ji yi zhi jie gou cai liao de xin fang fa ,zhi bei le duo chong xing mao jie gou ke diao de dan mo gui ji yi zhi jie gou cai liao ,jie jue le dian cui hua guo cheng zhong mo ji na mi cui hua ji ben zheng huo xing cha 、wen ding xing cha deng wen ti ,bing cheng gong jiang suo zhi bei de dan mo gui ji yi zhi jie gou cui hua ji ying yong yu dian cui hua chan qing 、dian cui hua chan yang deng ling yu zhong 。tong shi ,jie ge li lun ji suan ,chong dian xiang xi de yan jiu le ji dian hua xue xing zhi he dian cui hua fan ying ji li 。ben lun wen zhu yao bao gua yi xia ji ge bu fen nei rong :di yi zhang ,zhao chong chan shu le dan mo gui de fa zhan li shi 。cong dan mo gui de hua xue jie gou dao dian zi jie gou chu fa ,jiang shu le dan mo gui de ji ben xing zhi ;sui hou chong dian jiang shu le dan mo gui de ge cheng ,bing gai shu le dan mo gui ji xin cai liao zai cui hua 、neng yuan zhuai hua he cun chu cai liao yan jiu fang mian qu de de chong yao yan jiu cheng guo 。di er zhang ,cheng gong zhi bei chu ju you duo huo xing zhong xin 、duo gong neng de chan jing lei shui hua dan cai liao ,dui ji xing mao he jie gou xing zhi jin hang le xiang xi de biao zheng 。tong guo dian cui hua jie shui ,dui ji dian cui hua xing neng jin hang le ping jia 。yan jiu biao ming ,dui huo xing zhong xin yuan su chong lei ji han liang de diao kong ,ke yi dui cui hua ji de xing mao yi ji jie gou jin hang you xiao diao jie ,cong er shi ji xing neng de dao xian zhe gai shan 。ci wai ,tong guo shi yan he li lun ji suan xiang jie ge ming que le ji cui hua shui jie de ji li 。di san zhang ,tong guo dui chun lei shui hua dan jie gou ke kong de jin hang fei jin shu yuan su can za de ce lve ,shi xian le dui cui hua ji jie gou 、xing mao de jin yi bu jing que diao kong ,xian zhe di sheng ji cui hua huo xing he wen ding xing 。xiang xi de XPS、XRDdeng jie gou fen xi jie guo he mi du fan han li lun ji suan jie guo gong tong xian shi ,fei jin shu yuan su de can za ke yi xian zhao di gao cui hua ji de dian he zhuai yi neng li ,cong er zeng jiang ji fan ying huo xing ,tong shi zeng jia ji fan ying wen ding xing 。zui jia bi li de dao de cai liao biao xian chu you yi de xing neng ,li ru ,dian liu mi du 10 mA cm-2shi de xi qing wei 68 mV,xi yang dian wei wei 208 mV。bei yong zuo quan shui jie de shuang gong neng dian ji shi ,zai 1.44Vde ji di dian chi dian ya xia dian liu mi du ji da dao 10 mA cm-2,zai 100 mA cm-2xia wen ding chang da 80xiao shi er mo cui jian 。di si zhang ,li yong dan mo gui ke zai ren yi ji de biao mian yuan wei sheng chang de te xing ,fa zhan le yi chong yuan wei cha ceng -bao li lei shui hua dan na mi pian de fang fa ,shou ci shi xian le dui zi zhi cheng lei shui hua dan na mi pian de yuan wei cha ceng —bao li ,bing gou zhu le san wei “dan mo gui —ceng zhuang shuang jin shu qing yang hua wu —dan mo gui ”san ming zhi jie gou na mi pian zhen lie dian ji (e-ICLDH@GDY/NF)。yan jiu biao ming ,xiang dui yu chan du de LDHhe GDYcui hua ji ,e-ICLDH@GDY/NFju you geng wei you yi de dian cui hua HER、OERhe quan shui jie fan ying huo xing he wen ding xing ,bing tong guo dui fu ge cai liao jie gou de ke kong diao kong shi xian le dui dian ji xing neng de diao kong 。di wu zhang ,cheng gong de zai pao mo nie ji liu ti shang gou zhu le chao bao dan mo gui (GDY)bao fu de jian shi tan suan tie (FeCH)na mi pian zhen lie dian ji 。yan jiu jie guo xian shi ,zuo wei san wei ji cheng dian ji ,ji zai jian xing dian jie ye zhong biao xian chu you xiu de xi qing fan ying (HER)、xi yang fan ying (OER)huo xing he wen ding xing 。tong shi ,ji yu gai cui hua ji de quan shui jie dian jie chi zhan xian chu liang hao de fan ying huo xing (jin xu 1.49 Vdian chi dian ya ji ke qu dong 10 mA cm-2de quan shui jie dian liu mi du )he wen ding xing 。di liu zhang ,fa zhan le yi chong diao kong er liu hua mu jing xiang de fang fa ,tong guo zai liu hua mu na mi pian biao mian yuan wei sheng chang dan mo gui na mi pian jie gou ,shi xian le er liu hua mu cong 2Hdao 1Txiang de zhuai bian ,xian zhe zeng jia le ti ji dao dian xing ,jiang di le qing xi fu zi you neng ,jin er di sheng le ji ben zheng cui hua huo xing 。dian hua xue yan jiu jie guo xian shi ,suo zhi bei de dan mo gui bao fu er liu hua mu na mi pian zhen lie dian ji ,zai quan pH(014)fan wei nei dou you you yi de HERhuo xing he wen ding xing 。you ji shi zai jian xing (pH=14)tiao jian xia ,gai dian ji de HERhuo xing chao guo 20 wt.%Pt/C;tong shi shun tai guang dian liu shi chun er liu hua mu de 45.7bei 。di qi zhang ,ben lun wen de zong jie yu zhan wang 。
论文参考文献
论文详细介绍
论文作者分别是来自新疆大学的惠兰,发表于刊物新疆大学2019-07-23论文,是一篇关于石墨炔论文,二维碳材料论文,电催化论文,能量转换论文,析氢反应论文,析氧反应论文,新疆大学2019-07-23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,资料来自新疆大学2019-07-23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:石墨炔论文; 二维碳材料论文; 电催化论文; 能量转换论文; 析氢反应论文; 析氧反应论文; 新疆大学2019-07-23论文;