本文主要研究内容
作者许亚茹（2019）在《可见光响应型金属基纳米催化剂的制备及其在光催化放氢中的应用研究》一文中研究指出：氢气是一种燃烧热值高且环境友好的能源,在实现氢能经济的过程中,氢气的高效存储和温和释放仍然面临挑战。硼烷氨（NH3BH3）和甲酸（HCOOH）分别含19.6 wt%和4.4 wt%的氢,是有应用前景的两种化学储氢材料。为实现温和条件下NH3BH3和HCOOH的高效放氢,新型催化剂的设计是关键。基于此,本论文将可见光引入到NH3BH3和HCOOH的催化放氢体系中,利用可见光能够调节催化剂活性中心的电子密度从而提升其催化活性的特点,设计合成了三类可见光响应催化剂,系统研究了它们光催化NH3BH3和HCOOH的放氢性能。主要结果如下。（1）基于特定金属的表面等离子体共振（SPR）效应和非SPR效应,首先制备了一系列尺寸不同且具有SPR效应的Cu球,然后以它们为载体负载非贵金属Co和Ni纳米粒子,最后研究了负载型催化剂光催化NH3BH3放氢性能。结果表明,所有催化剂的可见光放氢活性都有大幅提高,其中尺寸为190 nm的Cu球负载Co纳米粒子的活性最高,TOF值达164.8 min-1,高于目前所有非贵金属催化剂的TOF。在可见光照射下,Cu因SPR效应所产生的电子转移到活性金属Co、Ni上,同时金属Co、Ni因非SPR效应,受光激发发生带间电子跃迁,于是两种不同来源的电子形成协同增强效应,使得催化剂的光催化放氢活性大幅提升。（2）基于特定金属的非SPR效应,首先采用氨基硅烷修饰在可见区没有光吸收的SiO2、TiO2和TiO2-SiO2,形成NH2功能化载体,然后负载具有非SPR效应的双金属CoPd纳米粒子,最后系统研究了负载型催化剂光催化HCOOH的放氢性能。结果表明,与暗反应相比,所有催化剂的光反应活性都有所提高,说明CoPd的非SPR效应的确对光催化放氢有促进作用。另外,在所有催化剂中,TiO2-SiO2负载的CoPd催化剂具有最高活性,其TOF为888.9 h-1。一系列对比实验表明,催化过程中,NH2能够吸附和活化HCOOH分子;当SiO2与TiO2复合后,可见光的利用率更高,这些有利因素最终促使了HCOOH的高效催化放氢。（3）基于半导体的复合能够改变能带结构的特性,首先合成一系列TiO2-CeO2复合半导体,然后负载双金属CoPd纳米粒子,最后系统研究了负载型催化剂光催化HCOOH的放氢性能。结果表明,在可见光照射下,相较于单一CeO2和TiO2为载体的催化剂,以复合半导体TiO2-CeO2为载体的催化剂光催化放氢活性都有所提升。当CeO2的量为5 wt%时,催化剂活性最高,其TOF值为637.1 h-1。另外,光谱表征结果显示,TiO2与CeO2复合后,它们的能带结构发生明显改变,带隙从3.01 eV减小到2.16 eV,这样的改变最终促使了HCOOH的高效光催化放氢。
Abstract
qing qi shi yi chong ran shao re zhi gao ju huan jing you hao de neng yuan ,zai shi xian qing neng jing ji de guo cheng zhong ,qing qi de gao xiao cun chu he wen he shi fang reng ran mian lin tiao zhan 。peng wan an （NH3BH3）he jia suan （HCOOH）fen bie han 19.6 wt%he 4.4 wt%de qing ,shi you ying yong qian jing de liang chong hua xue chu qing cai liao 。wei shi xian wen he tiao jian xia NH3BH3he HCOOHde gao xiao fang qing ,xin xing cui hua ji de she ji shi guan jian 。ji yu ci ,ben lun wen jiang ke jian guang yin ru dao NH3BH3he HCOOHde cui hua fang qing ti ji zhong ,li yong ke jian guang neng gou diao jie cui hua ji huo xing zhong xin de dian zi mi du cong er di sheng ji cui hua huo xing de te dian ,she ji ge cheng le san lei ke jian guang xiang ying cui hua ji ,ji tong yan jiu le ta men guang cui hua NH3BH3he HCOOHde fang qing xing neng 。zhu yao jie guo ru xia 。（1）ji yu te ding jin shu de biao mian deng li zi ti gong zhen （SPR）xiao ying he fei SPRxiao ying ,shou xian zhi bei le yi ji lie che cun bu tong ju ju you SPRxiao ying de Cuqiu ,ran hou yi ta men wei zai ti fu zai fei gui jin shu Cohe Nina mi li zi ,zui hou yan jiu le fu zai xing cui hua ji guang cui hua NH3BH3fang qing xing neng 。jie guo biao ming ,suo you cui hua ji de ke jian guang fang qing huo xing dou you da fu di gao ,ji zhong che cun wei 190 nmde Cuqiu fu zai Cona mi li zi de huo xing zui gao ,TOFzhi da 164.8 min-1,gao yu mu qian suo you fei gui jin shu cui hua ji de TOF。zai ke jian guang zhao she xia ,Cuyin SPRxiao ying suo chan sheng de dian zi zhuai yi dao huo xing jin shu Co、Nishang ,tong shi jin shu Co、Niyin fei SPRxiao ying ,shou guang ji fa fa sheng dai jian dian zi yue qian ,yu shi liang chong bu tong lai yuan de dian zi xing cheng xie tong zeng jiang xiao ying ,shi de cui hua ji de guang cui hua fang qing huo xing da fu di sheng 。（2）ji yu te ding jin shu de fei SPRxiao ying ,shou xian cai yong an ji gui wan xiu shi zai ke jian ou mei you guang xi shou de SiO2、TiO2he TiO2-SiO2,xing cheng NH2gong neng hua zai ti ,ran hou fu zai ju you fei SPRxiao ying de shuang jin shu CoPdna mi li zi ,zui hou ji tong yan jiu le fu zai xing cui hua ji guang cui hua HCOOHde fang qing xing neng 。jie guo biao ming ,yu an fan ying xiang bi ,suo you cui hua ji de guang fan ying huo xing dou you suo di gao ,shui ming CoPdde fei SPRxiao ying de que dui guang cui hua fang qing you cu jin zuo yong 。ling wai ,zai suo you cui hua ji zhong ,TiO2-SiO2fu zai de CoPdcui hua ji ju you zui gao huo xing ,ji TOFwei 888.9 h-1。yi ji lie dui bi shi yan biao ming ,cui hua guo cheng zhong ,NH2neng gou xi fu he huo hua HCOOHfen zi ;dang SiO2yu TiO2fu ge hou ,ke jian guang de li yong lv geng gao ,zhe xie you li yin su zui zhong cu shi le HCOOHde gao xiao cui hua fang qing 。（3）ji yu ban dao ti de fu ge neng gou gai bian neng dai jie gou de te xing ,shou xian ge cheng yi ji lie TiO2-CeO2fu ge ban dao ti ,ran hou fu zai shuang jin shu CoPdna mi li zi ,zui hou ji tong yan jiu le fu zai xing cui hua ji guang cui hua HCOOHde fang qing xing neng 。jie guo biao ming ,zai ke jian guang zhao she xia ,xiang jiao yu chan yi CeO2he TiO2wei zai ti de cui hua ji ,yi fu ge ban dao ti TiO2-CeO2wei zai ti de cui hua ji guang cui hua fang qing huo xing dou you suo di sheng 。dang CeO2de liang wei 5 wt%shi ,cui hua ji huo xing zui gao ,ji TOFzhi wei 637.1 h-1。ling wai ,guang pu biao zheng jie guo xian shi ,TiO2yu CeO2fu ge hou ,ta men de neng dai jie gou fa sheng ming xian gai bian ,dai xi cong 3.01 eVjian xiao dao 2.16 eV,zhe yang de gai bian zui zhong cu shi le HCOOHde gao xiao guang cui hua fang qing 。
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论文详细介绍
论文作者分别是来自内蒙古大学的许亚茹，发表于刊物内蒙古大学2019-08-13论文，是一篇关于硼烷氨论文,甲酸论文,放氢论文,光催化论文,金属基催化剂论文,复合半导体论文,内蒙古大学2019-08-13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，资料来自内蒙古大学2019-08-13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：硼烷氨论文; 甲酸论文; 放氢论文; 光催化论文; 金属基催化剂论文; 复合半导体论文; 内蒙古大学2019-08-13论文;