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dc.contributor.authorYuan, Ru-Ming
dc.contributor.authorFu, Gang
dc.contributor.author傅钢
dc.contributor.authorXu, Xin
dc.contributor.author徐昕
dc.contributor.authorWan, Hui-Lin
dc.contributor.author万惠霖
dc.date.accessioned2012-04-08T08:52:17Z
dc.date.available2012-04-08T08:52:17Z
dc.date.issued2010-10-29
dc.identifier.citationPHYSICAL CHEMISTRY CHEMICAL PHYSICS,2011,13(2):453-460zh_CN
dc.identifier.issn1463-9076
dc.identifier.urihttp://dx.doi.org/doi:10.1039/c0cp00256a
dc.identifier.uriWOS:000285390400012
dc.identifier.urihttps://dspace.xmu.edu.cn/handle/2288/12005
dc.description.abstractThe selective catalytic reduction (SCR) of NO by NH(3) over V(2)O(5)-based catalysts is used worldwide to control NO(x) emission. Understanding the mechanisms involved is vital for the rational design of more effective catalysts. Here, we have performed a systematic density functional theory (DFT) study of a SCR reaction by using cluster models. Three possible mechanisms have been considered, namely (i) a Lewis acid mechanism, (ii) a Bronsted acid mechanism and (iii) a nitrite mechanism. Our calculations down-play the significance of mechanism (i) due to its high barrier as well as the incorrect reaction order. On the other hand, our calculations demonstrate that both mechanisms (ii) and (iii) can lead to a first order reaction with respect to NO with the predicted barriers being consistent with the experimental observations. Thus, we conclude: there exists two competitive pathways for SCR. Mechanism (ii) is dominant when the Bronsted acidity of the catalysts is relatively strong, while mechanism (iii) becomes important when Bronsted acidity is weak or absent. Importantly, we demonstrate that the latter two mechanisms share a common feature where N-N bond formation is ahead of N-H bond cleavage, in contrast to that in mechanism (i). Such a sequence provides an effective way to reduce the side reaction of ammonia combustion since the relatively strong N-N bond has already been formed.zh_CN
dc.description.sponsorshipNational Natural Science Foundation of China[20525311, 20503022, 20433030, 20973139]; Ministry of Science and Technology[2005CB221408, 2007CB815206]; Key Science & Technology Specific Projects of Fujian Province[2009HZ0002-1]; Natural Science Foundation of Fujian Province of China[2009J05035]zh_CN
dc.language.isoenzh_CN
dc.publisherROYAL SOC CHEMISTRYzh_CN
dc.titleBronsted-NH(4)(+) mechanism versus nitrite mechanism: new insight into the selective catalytic reduction of NO by NH(3)zh_CN
dc.typeArticlezh_CN


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