Single Fe Site on the Surface of gamma-Al2O3: Insights from Density Functional Theory Periodic Boundary Approach

doi:10.1021/acs.jpcc.0c05401

	Single Fe Site on the Surface of gamma-Al2O3: Insights from Density Functional Theory Periodic Boundary Approach
	Gu, Jiande 1,2; Wang, Jing 1; Leszczynski, Jerzy 1
刊名	JOURNAL OF PHYSICAL CHEMISTRY C
	2020-09-24
卷号	124 期号:38 页码:20931-20941
ISSN号	1932-7447
DOI	10.1021/acs.jpcc.0c05401
通讯作者	Gu, Jiande(jiande@icnanotox.org) ; Leszczynski, Jerzy(jerzy@icnanotox.org)
英文摘要	Tri-coordinated Fe single sites on the (111)(n) surface of gamma-alumina have been investigated by the carefully calibrated density functional methods (M12-L/SV) using periodic boundary conditions. For all three different Al sites available on the (111)(n) surface, the most stable replacement has been found to be FeI substitution. The low spin state (doublet) has been found to be the ground state for the replacements of Fe on Al-I and Al-III sites on the (111)n surface of gamma-Al2O3. Al-II replacement results in the quadruplet as the ground state. The replacement of Al by Fe on the (111)(n) surface leads to elongations of metal-O distances. The substitution of the tri-coordinated Fe on the surface also leads to charge redistributions of the surrounding O atoms. The direct band gap is predicted to be close to that of the unsubstituted (111)(n) surface of gamma-Al2O3. The Al2O3 moiety is the main electron donor and the tri-coordinated Fe-I acts as an electron acceptor on the (111)(n) surface of gamma-Al2O3. However, in the cases of the substitution of Fe on the II and III positions, both tri-coordinated Fe and Al2O3 might act as the electron donor and acceptor on the (111)(n) surface of gamma-Al2O3.
资助项目	ONR[N00014171306] ; National Science Foundation[OCI-1053575] ; XSEDE award[DMR110088] ; Mississippi Center for Supercomputer Research
WOS关键词	TOTAL-ENERGY CALCULATIONS ; GAUSSIAN-BASIS SETS ; GAMMA-ALUMINA ; CO OXIDATION ; CATALYTIC PERFORMANCE ; EXCHANGE-REACTION ; SUPPORTED SINGLE ; HYDROXYL-GROUPS ; ATOMS LI ; REDUCTION
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000575823600031
内容类型	期刊论文
源URL	[http://119.78.100.183/handle/2S10ELR8/291333]
专题	中国科学院上海药物研究所
通讯作者	Gu, Jiande; Leszczynski, Jerzy
作者单位	1.Jackson State Univ, Dept Chem, Interdisciplinary Nanotox Ctr, Jackson, MS 39217 USA 2.Chinese Acad Sci, Shanghai Inst Mat Med, Drug Design & Discovery Ctr, State Key Lab Drug Res, Shanghai 201203, Peoples R China
推荐引用方式 GB/T 7714	Gu, Jiande,Wang, Jing,Leszczynski, Jerzy. Single Fe Site on the Surface of gamma-Al2O3: Insights from Density Functional Theory Periodic Boundary Approach[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2020,124(38):20931-20941.
APA	Gu, Jiande,Wang, Jing,&Leszczynski, Jerzy.(2020).Single Fe Site on the Surface of gamma-Al2O3: Insights from Density Functional Theory Periodic Boundary Approach.JOURNAL OF PHYSICAL CHEMISTRY C,124(38),20931-20941.
MLA	Gu, Jiande,et al."Single Fe Site on the Surface of gamma-Al2O3: Insights from Density Functional Theory Periodic Boundary Approach".JOURNAL OF PHYSICAL CHEMISTRY C 124.38(2020):20931-20941.