本文主要研究内容
作者王昊,刘小好,许光月,郭子薇,张颖(2019)在《纤维素原位合成Fe-N-C催化加氢硝基苯到苯胺(英文)》一文中研究指出:贵金属被广泛用作各种反应的催化剂,然而它们高昂的价格和有限的来源引起了人们对于开发非贵金属催化剂的浓厚兴趣.因此,寻找一种丰富而有效的催化剂来代替贵金属已成为催化领域最重要的任务之一.铁是地球上最丰富、最廉价的过渡金属,同时铁基催化剂在合成氨,费托合成和选择性还原氮氧化物等方面表现出优异的活性.近年来,廉价高效的氮掺杂碳负载铁催化剂在各种典型的铂催化反应中表现出良好的催化性能,尤其在催化加氢反应中的应用引起了研究人员的关注.本文通过在氨气氛围下共热解纤维素和氯化铁制备了一系列氮掺杂碳负载铁催化剂,并通过元素分析、原子吸收光谱、透射电子显微镜、X射线衍射和X射线光电子能谱等表征方法,探索了催化剂的物理化学性质.同时以硝基苯加氢制备苯胺为模型反应,探究了催化剂制备条件和反应条件对于催化剂活性的影响.其中Fe-N-C-700(通过在氨气氛围下700°C共热解纤维素和氯化铁制备)表现出最佳活性,在5 MPa氢气和120℃的条件下反应12 h,硝基苯被完全转化,苯胺的收率可达98.0%,同时,该催化剂还显示出良好的可再循环性, 5次运行后未见催化活性的显著降低.BET和元素分析结果表明,在热解温度为700℃的条件下制备的催化剂具有最高的比表面积,并且随着热解温度的升高,催化剂中碳元素和铁元素的含量升高,而氢、氮、氧元素的含量都随之下降.根据TEM图像,当热解温度升至600℃时,在碳材料上可以观察到平均尺寸为5.1 nm的金属颗粒,分散性较好.进一步将温度升至700℃,观察到平均尺寸为9.1 nm的金属颗粒,并且碳材料的形态结构转变为卷曲的层状.在XRD分析中, 600℃时催化剂的衍射峰归因于正交晶系的Fe2N,随着温度升至700℃, Fe2N相消失同时出现了Fe3C相.在HRTEM的图谱中,可以清晰地看到Fe3C相的(031)面的衍射条纹,并且在颗粒周围有约5.2nm厚的石墨碳层包裹.XPS结果表明,当温度达到700℃时,形成石墨化的氮掺杂碳,提高了催化剂活性.结合催化剂表征结果和对比实验,催化剂中铁物种的转变和氮掺杂碳尤其是石墨化的氮掺杂碳的生成可能是影响催化剂活性的主要因素.根据动力学实验,当使用Fe-N-C-700催化剂时,硝基苯加氢反应表观活化能为31.53 kJ/mol(报道为91.5 kJ/mol),这表明Fe-N-C-700催化剂可以有效地降低反应活化能.
Abstract
gui jin shu bei an fan yong zuo ge chong fan ying de cui hua ji ,ran er ta men gao ang de jia ge he you xian de lai yuan yin qi le ren men dui yu kai fa fei gui jin shu cui hua ji de nong hou xing qu .yin ci ,xun zhao yi chong feng fu er you xiao de cui hua ji lai dai ti gui jin shu yi cheng wei cui hua ling yu zui chong yao de ren wu zhi yi .tie shi de qiu shang zui feng fu 、zui lian jia de guo du jin shu ,tong shi tie ji cui hua ji zai ge cheng an ,fei tuo ge cheng he shua ze xing hai yuan dan yang hua wu deng fang mian biao xian chu you yi de huo xing .jin nian lai ,lian jia gao xiao de dan can za tan fu zai tie cui hua ji zai ge chong dian xing de bo cui hua fan ying zhong biao xian chu liang hao de cui hua xing neng ,you ji zai cui hua jia qing fan ying zhong de ying yong yin qi le yan jiu ren yuan de guan zhu .ben wen tong guo zai an qi fen wei xia gong re jie qian wei su he lv hua tie zhi bei le yi ji lie dan can za tan fu zai tie cui hua ji ,bing tong guo yuan su fen xi 、yuan zi xi shou guang pu 、tou she dian zi xian wei jing 、Xshe xian yan she he Xshe xian guang dian zi neng pu deng biao zheng fang fa ,tan suo le cui hua ji de wu li hua xue xing zhi .tong shi yi xiao ji ben jia qing zhi bei ben an wei mo xing fan ying ,tan jiu le cui hua ji zhi bei tiao jian he fan ying tiao jian dui yu cui hua ji huo xing de ying xiang .ji zhong Fe-N-C-700(tong guo zai an qi fen wei xia 700°Cgong re jie qian wei su he lv hua tie zhi bei )biao xian chu zui jia huo xing ,zai 5 MPaqing qi he 120℃de tiao jian xia fan ying 12 h,xiao ji ben bei wan quan zhuai hua ,ben an de shou lv ke da 98.0%,tong shi ,gai cui hua ji hai xian shi chu liang hao de ke zai xun huan xing , 5ci yun hang hou wei jian cui hua huo xing de xian zhe jiang di .BEThe yuan su fen xi jie guo biao ming ,zai re jie wen du wei 700℃de tiao jian xia zhi bei de cui hua ji ju you zui gao de bi biao mian ji ,bing ju sui zhao re jie wen du de sheng gao ,cui hua ji zhong tan yuan su he tie yuan su de han liang sheng gao ,er qing 、dan 、yang yuan su de han liang dou sui zhi xia jiang .gen ju TEMtu xiang ,dang re jie wen du sheng zhi 600℃shi ,zai tan cai liao shang ke yi guan cha dao ping jun che cun wei 5.1 nmde jin shu ke li ,fen san xing jiao hao .jin yi bu jiang wen du sheng zhi 700℃,guan cha dao ping jun che cun wei 9.1 nmde jin shu ke li ,bing ju tan cai liao de xing tai jie gou zhuai bian wei juan qu de ceng zhuang .zai XRDfen xi zhong , 600℃shi cui hua ji de yan she feng gui yin yu zheng jiao jing ji de Fe2N,sui zhao wen du sheng zhi 700℃, Fe2Nxiang xiao shi tong shi chu xian le Fe3Cxiang .zai HRTEMde tu pu zhong ,ke yi qing xi de kan dao Fe3Cxiang de (031)mian de yan she tiao wen ,bing ju zai ke li zhou wei you yao 5.2nmhou de dan mo tan ceng bao guo .XPSjie guo biao ming ,dang wen du da dao 700℃shi ,xing cheng dan mo hua de dan can za tan ,di gao le cui hua ji huo xing .jie ge cui hua ji biao zheng jie guo he dui bi shi yan ,cui hua ji zhong tie wu chong de zhuai bian he dan can za tan you ji shi dan mo hua de dan can za tan de sheng cheng ke neng shi ying xiang cui hua ji huo xing de zhu yao yin su .gen ju dong li xue shi yan ,dang shi yong Fe-N-C-700cui hua ji shi ,xiao ji ben jia qing fan ying biao guan huo hua neng wei 31.53 kJ/mol(bao dao wei 91.5 kJ/mol),zhe biao ming Fe-N-C-700cui hua ji ke yi you xiao de jiang di fan ying huo hua neng .
论文参考文献
论文详细介绍
论文作者分别是来自Chinese Journal of Catalysis的王昊,刘小好,许光月,郭子薇,张颖,发表于刊物Chinese Journal of Catalysis2019年10期论文,是一篇关于共热解论文,氮掺杂论文,碳材料论文,氢化反应论文,Chinese Journal of Catalysis2019年10期论文的文章。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Chinese Journal of Catalysis2019年10期论文网站,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:共热解论文; 氮掺杂论文; 碳材料论文; 氢化反应论文; Chinese Journal of Catalysis2019年10期论文;