Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study

	Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study
	Li, Haichao 1; Zhou, Danhong 2; Tian, Dongxu 1; Shi, Chuan 1; Mueller, Ulrich 3; Feyen, Mathias 3; Yilmaz, Bilge 4; Gies, Hermann 5; Xiao, Feng-Shou 6; De Vos, Dirk 7
刊名	chemphyschem
	2014-06-06
卷号	15 期号:8 页码:1700-1707
关键词	Bronsted acidity density functional calculations interlayer pore expansion isomorphously substituted COE-4 lamellar zeolites
通讯作者	weipingzhang
英文摘要	coe-4 zeolites possess a unique two-dimensional ten-ring pore structure with the si(oh)(2) hydroxyl groups attached to the linker position between the ferrierite-type layers, which has been demonstrated through the interlayer-expansion approach in our previous work (h. gies et al. chem. mater. 2012, 24, 1536). herein, density functional theory is used to study the framework stability and bronsted acidity of the zeolite t-coe-4, in which the tetravalent si is isomorphously substituted by a trivalent fe, b, ga, or al heteroatom at the linker position. the influences of substitution energy and equilibrium geometry parameters on the stability of t-coe-4 are investigated in detail. the relative acid strength of the linker position is revealed by the proton affinity, charge analysis, and nh3 adsorption. it is found that the range of the < t-o-si > angles is widened to maintain the stability of isomorphously substituted t-coe-4 zeolites. the smaller the < o1-t-o2 > bond angle is, the more difficult is to form the regular tetrahedral unit. thus, the substitution energies at the linker positions increase in the following sequence: al-coe-4 < ga-coe-4 < fe-coe-4 < b-coe-4. the adsorption of nh3 as a probe molecule indicates that the acidity can affect the hydrogen-bonding interaction between (n-h center dot center dot center dot center dot o2) and (n center dot center dot center dot h- o2). the relative bronsted-acid strength of the interlayer-expanded t-coe-4 zeolite decreases in the order of al-coe-4 > ga-coe-4 > fe-coe-4 > b-coe-4. these findings may be helpful for the structural design and functional modification of interlayer-expanded zeolites.
学科主题	物理化学
WOS标题词	science & technology ; physical sciences
类目[WOS]	chemistry, physical ; physics, atomic, molecular & chemical
研究领域[WOS]	chemistry ; physics
关键词[WOS]	effective core potentials ; ab-initio ; molecular calculations ; catalytic performance ; topotactic conversion ; adsorption properties ; crystal-structure ; layered silicate ; probe molecules ; solid acids
收录类别	SCI
语种	英语
WOS记录号	WOS:000337521700024
公开日期	2016-05-09
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/144230]
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.Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116024, Peoples R China 2.Liaoning Normal Univ, Inst Chem Functionalized Mat, Dalian 116029, Peoples R China 3.BASF SE, Chem Res & Engn, D-67056 Ludwigshafen, Germany 4.BASF Corp, Chem Res & Engn, Iselin, NJ 08830 USA 5.Ruhr Univ Bochum, Inst Geol Mineral & Geophys, Bochum, Germany 6.Zhejiang Univ, Dept Chem, Hangzhou 310028, Peoples R China 7.Katholieke Univ Leuven, Ctr Surface Chem & Catalysis, Leuven, Belgium 8.Tokyo Inst Technol, Chem Resources Lab, Yokohama, Kanagawa 227, Japan 9.Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Li, Haichao,Zhou, Danhong,Tian, Dongxu,et al. Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study[J]. chemphyschem,2014,15(8):1700-1707.
APA	Li, Haichao.,Zhou, Danhong.,Tian, Dongxu.,Shi, Chuan.,Mueller, Ulrich.,...&Zhang, Weiping.(2014).Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study.chemphyschem,15(8),1700-1707.
MLA	Li, Haichao,et al."Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study".chemphyschem 15.8(2014):1700-1707.