本文主要研究内容
作者明淑君,庞磊,范驰,郭文,董亚浩,刘鹏,陈真,李涛(2019)在《柴油机尾气中的碱性无机污染物引起Cu-SAPO-18脱硝催化剂的化学失活(英文)》一文中研究指出:选择性催化还原NOx(NH3-SCR)已是柴油机尾气处理系统中有效的NOx减排技术.铜基分子筛催化剂作为潜在的NH3-SCR催化剂已被广泛研究,其中具有AEI结构的Cu-SAPO-18分子筛表现出优异的脱硝活性和水热稳定性,成为柴油机尾气后处理系统潜在的替代品.然而在实际的后处理应用中,生物柴油污染物、发动机润滑剂和燃料添加剂中的一些无机组分(K, Na, S, P, Ca和Mg等)可逐渐聚集在催化剂表面,导致催化剂孔道堵塞和活性位点丢失,最终导致SCR催化剂失活.由于碱金属和碱土金属在柴油衍生物中含量较高,因而其对SCR催化剂的影响引起了人们更多的关注.本文采用浸渍法制备了掺杂不同含量碱性无机污染物(K, Na, Ca和Mg)的Cu-SAPO-18催化剂,以阐明这些污染物对Cu-SAPO-18结构、酸性位点和铜物种的影响.XRD和氮吸附实验结果表明,低含量污染物的掺入造成催化剂孔道堵塞和比表面积下降,而高含量污染物引入导致催化剂部分结构被破坏,其中高含量Na的引入造成催化剂结构破坏最为严重.H2-TPR和EPR结果表明,污染物引入Cu-SAPO-18后,催化剂的Cu2+数目减少,这是由于Cu2+被K+, Na+, Ca2+和Mg2+取代造成的.被取代的Cu2+由于无法位于离子交换位点上会在煅烧过程中转变成CuO和CuAl2O4, CuO的产生会造成催化剂孔道堵塞甚至部分骨架结构坍塌.另外,NH3-TPD结果表明,与新鲜催化剂相比,被污染的Cu-SAPO-18催化剂总酸性位点减少,这是由于H+和Cu2+被K+, Na+, Ca2+和Mg2+取代造成Br?nsted酸和Lewis酸减少造成的.催化剂比表面积的降低、Cu2+数目以及酸含量的减少最终造成催化剂失活,且催化剂失活程度随无机污染物含量的增加而增大.但不同无机组分造成催化剂的失活程度不同,其中K, Na, Ca和Mg造成Cu-SAPO-18催化剂失活程度为K> Na> Ca> Mg.此外, K, Na, Ca和Mg造成Cu-SAPO-18催化剂比表面积、Cu2+含量以及酸含量的减少程度分别为Na> K> Ca> Mg, Na> K> Mg> Ca和K> Na> Ca> Mg.其中酸含量下降程度与催化剂失活程度一致,表明在某种程度上,酸含量对催化剂NH3-SCR活性的影响高于催化剂结构和Cu2+对活性的影响.最后,我们还通过NH3-SCR动力学测试研究了K, Na, Ca和Mg对Cu-SAPO-18催化NH3-SCR反应机理的影响,结果显示新鲜催化剂和被污染催化剂具有相近的活化能,表明无机污染物对Cu-SAPO-18催化NH3-SCR反应机理没有影响.
Abstract
shua ze xing cui hua hai yuan NOx(NH3-SCR)yi shi chai you ji wei qi chu li ji tong zhong you xiao de NOxjian pai ji shu .tong ji fen zi shai cui hua ji zuo wei qian zai de NH3-SCRcui hua ji yi bei an fan yan jiu ,ji zhong ju you AEIjie gou de Cu-SAPO-18fen zi shai biao xian chu you yi de tuo xiao huo xing he shui re wen ding xing ,cheng wei chai you ji wei qi hou chu li ji tong qian zai de ti dai pin .ran er zai shi ji de hou chu li ying yong zhong ,sheng wu chai you wu ran wu 、fa dong ji run hua ji he ran liao tian jia ji zhong de yi xie mo ji zu fen (K, Na, S, P, Cahe Mgdeng )ke zhu jian ju ji zai cui hua ji biao mian ,dao zhi cui hua ji kong dao du sai he huo xing wei dian diu shi ,zui zhong dao zhi SCRcui hua ji shi huo .you yu jian jin shu he jian tu jin shu zai chai you yan sheng wu zhong han liang jiao gao ,yin er ji dui SCRcui hua ji de ying xiang yin qi le ren men geng duo de guan zhu .ben wen cai yong jin zi fa zhi bei le can za bu tong han liang jian xing mo ji wu ran wu (K, Na, Cahe Mg)de Cu-SAPO-18cui hua ji ,yi chan ming zhe xie wu ran wu dui Cu-SAPO-18jie gou 、suan xing wei dian he tong wu chong de ying xiang .XRDhe dan xi fu shi yan jie guo biao ming ,di han liang wu ran wu de can ru zao cheng cui hua ji kong dao du sai he bi biao mian ji xia jiang ,er gao han liang wu ran wu yin ru dao zhi cui hua ji bu fen jie gou bei po huai ,ji zhong gao han liang Nade yin ru zao cheng cui hua ji jie gou po huai zui wei yan chong .H2-TPRhe EPRjie guo biao ming ,wu ran wu yin ru Cu-SAPO-18hou ,cui hua ji de Cu2+shu mu jian shao ,zhe shi you yu Cu2+bei K+, Na+, Ca2+he Mg2+qu dai zao cheng de .bei qu dai de Cu2+you yu mo fa wei yu li zi jiao huan wei dian shang hui zai duan shao guo cheng zhong zhuai bian cheng CuOhe CuAl2O4, CuOde chan sheng hui zao cheng cui hua ji kong dao du sai shen zhi bu fen gu jia jie gou tan ta .ling wai ,NH3-TPDjie guo biao ming ,yu xin xian cui hua ji xiang bi ,bei wu ran de Cu-SAPO-18cui hua ji zong suan xing wei dian jian shao ,zhe shi you yu H+he Cu2+bei K+, Na+, Ca2+he Mg2+qu dai zao cheng Br?nstedsuan he Lewissuan jian shao zao cheng de .cui hua ji bi biao mian ji de jiang di 、Cu2+shu mu yi ji suan han liang de jian shao zui zhong zao cheng cui hua ji shi huo ,ju cui hua ji shi huo cheng du sui mo ji wu ran wu han liang de zeng jia er zeng da .dan bu tong mo ji zu fen zao cheng cui hua ji de shi huo cheng du bu tong ,ji zhong K, Na, Cahe Mgzao cheng Cu-SAPO-18cui hua ji shi huo cheng du wei K> Na> Ca> Mg.ci wai , K, Na, Cahe Mgzao cheng Cu-SAPO-18cui hua ji bi biao mian ji 、Cu2+han liang yi ji suan han liang de jian shao cheng du fen bie wei Na> K> Ca> Mg, Na> K> Mg> Cahe K> Na> Ca> Mg.ji zhong suan han liang xia jiang cheng du yu cui hua ji shi huo cheng du yi zhi ,biao ming zai mou chong cheng du shang ,suan han liang dui cui hua ji NH3-SCRhuo xing de ying xiang gao yu cui hua ji jie gou he Cu2+dui huo xing de ying xiang .zui hou ,wo men hai tong guo NH3-SCRdong li xue ce shi yan jiu le K, Na, Cahe Mgdui Cu-SAPO-18cui hua NH3-SCRfan ying ji li de ying xiang ,jie guo xian shi xin xian cui hua ji he bei wu ran cui hua ji ju you xiang jin de huo hua neng ,biao ming mo ji wu ran wu dui Cu-SAPO-18cui hua NH3-SCRfan ying ji li mei you ying xiang .
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论文作者分别是来自催化学报的明淑君,庞磊,范驰,郭文,董亚浩,刘鹏,陈真,李涛,发表于刊物催化学报2019年04期论文,是一篇关于催化剂论文,碱性无机污染物论文,选择性催化还原论文,酸性位点论文,铜离子论文,催化学报2019年04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04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:催化剂论文; 碱性无机污染物论文; 选择性催化还原论文; 酸性位点论文; 铜离子论文; 催化学报2019年04期论文;