Stability of Extraframework Iron-Containing Complexes in ZSM-5 Zeolite

	Stability of Extraframework Iron-Containing Complexes in ZSM-5 Zeolite
	Li, Guanna 1,2; Pidko, Evgeny A.1; van Santen, Rutger A.1; Li, Can 2; Hensen, Emiel J. M.1
刊名	journal of physical chemistry c
	2013-01-10
卷号	117 期号:1 页码:413-426
通讯作者	李灿 ; emiel j. m. hensen
产权排序	待补充
合作状况	英
英文摘要	the stability of oxygenated and hydroxylated iron complexes in fe/zsm-5 is studied by periodic dft calculations. the reaction paths for the interconversion of various potential iron-containing complexes confined in the zeolite matrix are discussed. it is demonstrated that the distribution of mononuclear [feo](+) species depends only slightly on the specific local zeolite environment. for all binuclear complexes considered, a notable preference for the location at the larger eight-membered ring gamma site in the sinusoidal channel is observed. nevertheless, the formation of the mononuclear species [feo](+) in realistic systems is very unlikely. irrespective of their location inside the zeolite matrix, such species show a strong tendency toward self-organization into binuclear oxygen-bridged [fe(mu-o)(2)fe](2+) complexes. using ab initio thermodynamic analysis of the stability of different fe complexes in zsm-5, it is demonstrated that two distinct extraframework cationic complexes can be present in the fe/zsm-5 catalyst, namely, [fe-iii(mu-o)(2)fe-iii](2+) and [fe-ii(mu-o)fe-ii](2+). the [fe-ii(mu-o)fe-ii](2+)complexes containing bivalent iron centers are mainly present in the fe/zsm-5 catalyst activated at low oxygen chemical potential and h2o-free conditions, whereas the formation of its fe3+-containing counterpart [fe-iii(mu-o)(2)fe-iii](2+) is favored upon the high-temperature calcination in an o-2-rich environment.
学科主题	物理化学
WOS标题词	science & technology ; physical sciences ; technology
类目[WOS]	chemistry, physical ; nanoscience & nanotechnology ; materials science, multidisciplinary
研究领域[WOS]	chemistry ; science & technology - other topics ; materials science
关键词[WOS]	nitrous-oxide decomposition ; over-exchanged fe/zsm5 ; chemical-vapor-deposition ; selective catalytic-reduction ; high-temperature treatment ; initio molecular-dynamics ; density-functional theory ; total-energy calculations ; direct n2o decomposition ; situ xafs spectroscopy
收录类别	SCI
资助信息	2，1
原文出处	426
语种	英语
WOS记录号	WOS:000313220700054
公开日期	2014-09-11
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/119227]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	1.Eindhoven Univ Technol, Inorgan Mat Chem Grp, NL-5600 MB Eindhoven, Netherlands 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian, Peoples R China
推荐引用方式 GB/T 7714	Li, Guanna,Pidko, Evgeny A.,van Santen, Rutger A.,et al. Stability of Extraframework Iron-Containing Complexes in ZSM-5 Zeolite[J]. journal of physical chemistry c,2013,117(1):413-426.
APA	Li, Guanna,Pidko, Evgeny A.,van Santen, Rutger A.,Li, Can,&Hensen, Emiel J. M..(2013).Stability of Extraframework Iron-Containing Complexes in ZSM-5 Zeolite.journal of physical chemistry c,117(1),413-426.
MLA	Li, Guanna,et al."Stability of Extraframework Iron-Containing Complexes in ZSM-5 Zeolite".journal of physical chemistry c 117.1(2013):413-426.