本文主要研究内容
作者王文峰(2019)在《基于金属有机框架的氧还原反应与析氢反应催化剂的制备及性能表征研究》一文中研究指出:本文研究了一种简单而有效的策略,用于实现稳定的Fe和Co单原子锚定在氮掺杂多孔碳((Fe,Co)SACs/N-C)上,其具有很大的比表面积(764.7 m2g-1)和较高的金属负载量(1.6 wt.%)。首先,Fe(III)通过一步共同成核法与预先设计的双金属Zn/Co金属有机框架形成Fe(acac)3@ZnCo-BMOF,然后通过高温热解和顺序还原过程获得(Fe,Co)SACs/N-C催化剂。(Fe,Co)SACs/N-C表现出优良的电催化氧还原反应(ORR)性能,其半波电位在0.1 M HClO4中为0.72 V,比商业Pt/C(0.81 V)略小,在0.1 M PBS中,半波电位为0.81 V,更重要的是,在0.1 M KOH中,该催化剂的半波电位为0.85 V,比商业Pt/C(0.83 V)还要高20 mV。同时,我们还探讨了酸性和碱性条件下的活性差异可归因于吡啶-N的质子化作用。动力学研究发现,(Fe,Co)SACs/N-C在酸性、中性和碱性电解质中都是一个快速的4电子过程,这说明其具有高效ORR催化性能。研究发现,经过3000个周期的伏安循环扫描,(Fe,Co)SACs/N-C的半波电位在酸性和碱性电解质中也仅仅降低了13 mV和7mV,这证明了其优越的稳定性。最后还证实了,(Fe,Co)SACs/N-C在酸性和碱性电解质中对甲醇均具有良好的耐受性。总之,该催化剂展示了可与商用Pt/C催化剂相媲美的ORR性能,在燃料电池方面具有潜在的应用前景,而且,所建立的简单一步共同成核方法可对制备其他双金属单原子催化剂起到示范作用。另外,本文以UIO-66为载体,先后经过FeCl3化学气相沉积、原位碳化和磷化以及HF刻蚀等步骤制备了多孔FeP@PC催化剂。采用X射线衍射(XRD)、场发射透射电子显微镜(FE-TEM)、X射线光电子能谱(XPS)和气体吸附仪(BET)等对该催化剂的晶型结构、形貌、化学价态和比表面积等物理性质进行了表征;也采用线性扫描伏安法和电化学阻抗谱等对其电催化析氢反应性能进行了考察。结果表明,FeP@PC保持了原UIO-66的八面体多孔结构,比表面积为83 m2g-1;仅需过电位为156 mV,就可以驱动电流密度达到10 mA cm-2,塔菲尔斜率为84 mV dec-1,电荷转移电阻为44Ω,电化学活性表面积为13.9 mF cm-2。而且计时电流法持续测试12 h和循环伏安法测试1000次之后,催化剂的活性几乎没有衰减,这表现出与许多已经报道的非贵金属相媲美的电催化析氢反应性能。其优良的催化活性以及稳定性不仅是因为高的比表面积能暴露更多的析氢活性位点,而且金属有机框架稳定的纳米八面体多孔碳骨架包覆也起到重要作用。FeP@PC是一种价格低廉,催化活性以及稳定性优良的析氢催化剂,而且这种在MOFs基载体中引入新金属中心的策略为合成其它同类型材料提供了新的思路。
Abstract
ben wen yan jiu le yi chong jian chan er you xiao de ce lve ,yong yu shi xian wen ding de Fehe Cochan yuan zi mao ding zai dan can za duo kong tan ((Fe,Co)SACs/N-C)shang ,ji ju you hen da de bi biao mian ji (764.7 m2g-1)he jiao gao de jin shu fu zai liang (1.6 wt.%)。shou xian ,Fe(III)tong guo yi bu gong tong cheng he fa yu yu xian she ji de shuang jin shu Zn/Cojin shu you ji kuang jia xing cheng Fe(acac)3@ZnCo-BMOF,ran hou tong guo gao wen re jie he shun xu hai yuan guo cheng huo de (Fe,Co)SACs/N-Ccui hua ji 。(Fe,Co)SACs/N-Cbiao xian chu you liang de dian cui hua yang hai yuan fan ying (ORR)xing neng ,ji ban bo dian wei zai 0.1 M HClO4zhong wei 0.72 V,bi shang ye Pt/C(0.81 V)lve xiao ,zai 0.1 M PBSzhong ,ban bo dian wei wei 0.81 V,geng chong yao de shi ,zai 0.1 M KOHzhong ,gai cui hua ji de ban bo dian wei wei 0.85 V,bi shang ye Pt/C(0.83 V)hai yao gao 20 mV。tong shi ,wo men hai tan tao le suan xing he jian xing tiao jian xia de huo xing cha yi ke gui yin yu bi ding -Nde zhi zi hua zuo yong 。dong li xue yan jiu fa xian ,(Fe,Co)SACs/N-Czai suan xing 、zhong xing he jian xing dian jie zhi zhong dou shi yi ge kuai su de 4dian zi guo cheng ,zhe shui ming ji ju you gao xiao ORRcui hua xing neng 。yan jiu fa xian ,jing guo 3000ge zhou ji de fu an xun huan sao miao ,(Fe,Co)SACs/N-Cde ban bo dian wei zai suan xing he jian xing dian jie zhi zhong ye jin jin jiang di le 13 mVhe 7mV,zhe zheng ming le ji you yue de wen ding xing 。zui hou hai zheng shi le ,(Fe,Co)SACs/N-Czai suan xing he jian xing dian jie zhi zhong dui jia chun jun ju you liang hao de nai shou xing 。zong zhi ,gai cui hua ji zhan shi le ke yu shang yong Pt/Ccui hua ji xiang pi mei de ORRxing neng ,zai ran liao dian chi fang mian ju you qian zai de ying yong qian jing ,er ju ,suo jian li de jian chan yi bu gong tong cheng he fang fa ke dui zhi bei ji ta shuang jin shu chan yuan zi cui hua ji qi dao shi fan zuo yong 。ling wai ,ben wen yi UIO-66wei zai ti ,xian hou jing guo FeCl3hua xue qi xiang chen ji 、yuan wei tan hua he lin hua yi ji HFke shi deng bu zhou zhi bei le duo kong FeP@PCcui hua ji 。cai yong Xshe xian yan she (XRD)、chang fa she tou she dian zi xian wei jing (FE-TEM)、Xshe xian guang dian zi neng pu (XPS)he qi ti xi fu yi (BET)deng dui gai cui hua ji de jing xing jie gou 、xing mao 、hua xue jia tai he bi biao mian ji deng wu li xing zhi jin hang le biao zheng ;ye cai yong xian xing sao miao fu an fa he dian hua xue zu kang pu deng dui ji dian cui hua xi qing fan ying xing neng jin hang le kao cha 。jie guo biao ming ,FeP@PCbao chi le yuan UIO-66de ba mian ti duo kong jie gou ,bi biao mian ji wei 83 m2g-1;jin xu guo dian wei wei 156 mV,jiu ke yi qu dong dian liu mi du da dao 10 mA cm-2,da fei er xie lv wei 84 mV dec-1,dian he zhuai yi dian zu wei 44Ω,dian hua xue huo xing biao mian ji wei 13.9 mF cm-2。er ju ji shi dian liu fa chi xu ce shi 12 hhe xun huan fu an fa ce shi 1000ci zhi hou ,cui hua ji de huo xing ji hu mei you cui jian ,zhe biao xian chu yu hu duo yi jing bao dao de fei gui jin shu xiang pi mei de dian cui hua xi qing fan ying xing neng 。ji you liang de cui hua huo xing yi ji wen ding xing bu jin shi yin wei gao de bi biao mian ji neng bao lou geng duo de xi qing huo xing wei dian ,er ju jin shu you ji kuang jia wen ding de na mi ba mian ti duo kong tan gu jia bao fu ye qi dao chong yao zuo yong 。FeP@PCshi yi chong jia ge di lian ,cui hua huo xing yi ji wen ding xing you liang de xi qing cui hua ji ,er ju zhe chong zai MOFsji zai ti zhong yin ru xin jin shu zhong xin de ce lve wei ge cheng ji ta tong lei xing cai liao di gong le xin de sai lu 。
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论文作者分别是来自合肥工业大学的王文峰,发表于刊物合肥工业大学2019-10-22论文,是一篇关于单原子论文,磷化铁论文,金属有机框架论文,氧还原反应论文,析氢反应论文,合肥工业大学2019-10-22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,资料来自合肥工业大学2019-10-22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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