本文主要研究内容
作者张岩,吕元,王玉清,李存耀,姜淼,丁云杰（2019）在《多孔聚合物催化剂高效催化甲酸分解制氢（英文）》一文中研究指出：氢能作为一种新型能源被认为是未来最理想的二次能源,与传统能源相比,具有能量密度高、热效率高、零污染的特点.然而,通常状态下氢能以低密度的气体形式存在,易燃易爆,给储存和运输带来诸多困难.因此,研发出安全高效的储氢方法尤为重要.甲酸在室温下为液体,无毒,挥发性低,方便储存和运输;而且甲酸的体积储氢量高达53 g/L,并能够通过催化甲酸分解反应释放出氢气和催化二氧化碳加氢反应将氢气转化成甲酸,因而甲酸被认为是理想的氢能载体.对于甲酸分解反应,制备出高活性的催化剂是关键,常用的催化剂包括均相催化剂和多相催化剂两类.均相催化剂主要是有机膦、有机胺等有机配体与金属离子（Ru、Ir、Rh、Fe等）配位得到的配合物,多相催化剂主要是多孔材料（活性炭、分子筛、二氧化硅等）负载的Au、Pd、Pt等单金属或其合金.均相催化剂具有高活性、高选择性的优点,而多相催化剂易于分离.为了结合均相催化剂和多相催化剂的优点,本文基于均相催化剂和多孔聚合物材料的发展,将均相催化剂锚定在多孔有机聚合物载体上,制备出Ru@POPs-PPh3及Ru@POPs-TPP催化剂.首先,对制备的催化剂进行了一系列表征.通过13C和31P固体核磁谱图证实了催化剂的结构;热重分析结果显示催化剂的分解温度高于400 oC,表明此催化剂具有优良的热稳定性;N2物理吸附结果表明该催化剂具有非常高的比表面积和丰富的孔道结构;原位一氧化碳吸附红外光谱结果表明聚合物配体对中心金属离子的电子态具有重要影响.随后,对制备的催化剂进行了活性评价实验.结果显示, Ru@POPs-PPh3及Ru@POPs-TPP催化剂均能催化甲酸分解脱氢,并通过热过滤实验证明催化过程是多相催化过程.使用前后催化剂的透射电子显微镜表征显示,使用前Ru@POPs-PPh3及Ru@POPs-TPP催化剂上均未发现Ru纳米粒子,在使用后的Ru@POPs-TPP催化剂上发现了Ru纳米颗粒,而Ru@POPs-PPh3上的Ru仍然是高分散状态,没有团聚成纳米颗粒,表明Ru@POPs-PPh3具有更高的稳定性.对Ru@POPs-PPh3催化剂的进一步研究发现,在三乙胺参与下, 140 oC条件下,其催化甲酸分解脱氢的TOF值可达55855 h–1,该催化活性可与均相催化剂相媲美;稳定性实验结果表明该催化剂具有非常高的稳定性,能够连续使用5次而活性没有明显降低.催化剂的高活性和稳定性归因于特定的聚合物配体,以及载体的高比表面积和高的膦配体浓度.本工作可为甲酸分解催化剂的设计提供带来启发.
Abstract
qing neng zuo wei yi chong xin xing neng yuan bei ren wei shi wei lai zui li xiang de er ci neng yuan ,yu chuan tong neng yuan xiang bi ,ju you neng liang mi du gao 、re xiao lv gao 、ling wu ran de te dian .ran er ,tong chang zhuang tai xia qing neng yi di mi du de qi ti xing shi cun zai ,yi ran yi bao ,gei chu cun he yun shu dai lai zhu duo kun nan .yin ci ,yan fa chu an quan gao xiao de chu qing fang fa you wei chong yao .jia suan zai shi wen xia wei ye ti ,mo du ,hui fa xing di ,fang bian chu cun he yun shu ;er ju jia suan de ti ji chu qing liang gao da 53 g/L,bing neng gou tong guo cui hua jia suan fen jie fan ying shi fang chu qing qi he cui hua er yang hua tan jia qing fan ying jiang qing qi zhuai hua cheng jia suan ,yin er jia suan bei ren wei shi li xiang de qing neng zai ti .dui yu jia suan fen jie fan ying ,zhi bei chu gao huo xing de cui hua ji shi guan jian ,chang yong de cui hua ji bao gua jun xiang cui hua ji he duo xiang cui hua ji liang lei .jun xiang cui hua ji zhu yao shi you ji lin 、you ji an deng you ji pei ti yu jin shu li zi （Ru、Ir、Rh、Fedeng ）pei wei de dao de pei ge wu ,duo xiang cui hua ji zhu yao shi duo kong cai liao （huo xing tan 、fen zi shai 、er yang hua gui deng ）fu zai de Au、Pd、Ptdeng chan jin shu huo ji ge jin .jun xiang cui hua ji ju you gao huo xing 、gao shua ze xing de you dian ,er duo xiang cui hua ji yi yu fen li .wei le jie ge jun xiang cui hua ji he duo xiang cui hua ji de you dian ,ben wen ji yu jun xiang cui hua ji he duo kong ju ge wu cai liao de fa zhan ,jiang jun xiang cui hua ji mao ding zai duo kong you ji ju ge wu zai ti shang ,zhi bei chu Ru@POPs-PPh3ji Ru@POPs-TPPcui hua ji .shou xian ,dui zhi bei de cui hua ji jin hang le yi ji lie biao zheng .tong guo 13Che 31Pgu ti he ci pu tu zheng shi le cui hua ji de jie gou ;re chong fen xi jie guo xian shi cui hua ji de fen jie wen du gao yu 400 oC,biao ming ci cui hua ji ju you you liang de re wen ding xing ;N2wu li xi fu jie guo biao ming gai cui hua ji ju you fei chang gao de bi biao mian ji he feng fu de kong dao jie gou ;yuan wei yi yang hua tan xi fu gong wai guang pu jie guo biao ming ju ge wu pei ti dui zhong xin jin shu li zi de dian zi tai ju you chong yao ying xiang .sui hou ,dui zhi bei de cui hua ji jin hang le huo xing ping jia shi yan .jie guo xian shi , Ru@POPs-PPh3ji Ru@POPs-TPPcui hua ji jun neng cui hua jia suan fen jie tuo qing ,bing tong guo re guo lv shi yan zheng ming cui hua guo cheng shi duo xiang cui hua guo cheng .shi yong qian hou cui hua ji de tou she dian zi xian wei jing biao zheng xian shi ,shi yong qian Ru@POPs-PPh3ji Ru@POPs-TPPcui hua ji shang jun wei fa xian Runa mi li zi ,zai shi yong hou de Ru@POPs-TPPcui hua ji shang fa xian le Runa mi ke li ,er Ru@POPs-PPh3shang de Rureng ran shi gao fen san zhuang tai ,mei you tuan ju cheng na mi ke li ,biao ming Ru@POPs-PPh3ju you geng gao de wen ding xing .dui Ru@POPs-PPh3cui hua ji de jin yi bu yan jiu fa xian ,zai san yi an can yu xia , 140 oCtiao jian xia ,ji cui hua jia suan fen jie tuo qing de TOFzhi ke da 55855 h–1,gai cui hua huo xing ke yu jun xiang cui hua ji xiang pi mei ;wen ding xing shi yan jie guo biao ming gai cui hua ji ju you fei chang gao de wen ding xing ,neng gou lian xu shi yong 5ci er huo xing mei you ming xian jiang di .cui hua ji de gao huo xing he wen ding xing gui yin yu te ding de ju ge wu pei ti ,yi ji zai ti de gao bi biao mian ji he gao de lin pei ti nong du .ben gong zuo ke wei jia suan fen jie cui hua ji de she ji di gong dai lai qi fa .
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论文作者分别是来自催化学报的张岩,吕元,王玉清,李存耀,姜淼,丁云杰，发表于刊物催化学报2019年02期论文，是一篇关于多相催化论文,多孔聚合物论文,甲酸论文,分解论文,氢能论文,催化学报2019年02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，资料来自催化学报2019年02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。