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学科主题: 物理化学
题名: Framework Stability and Bronsted Acidity of Isomorphously Substituted Interlayer-Expanded Zeolite COE-4: A Density Functional Theory Study
作者: Li, Haichao1;  Zhou, Danhong2;  Tian, Dongxu1;  Shi, Chuan1;  Mueller, Ulrich3;  Feyen, Mathias3;  Yilmaz, Bilge4;  Gies, Hermann5;  Xiao, Feng-Shou6;  De Vos, Dirk7;  Yokoi, Toshiyuki8;  Tatsumi, Takashi8;  Bao, Xinhe9;  Zhang, Weiping1
通讯作者: WeipingZhang
关键词: Bronsted acidity ;  density functional calculations ;  interlayer pore expansion ;  isomorphously substituted COE-4 ;  lamellar zeolites
刊名: CHEMPHYSCHEM
发表日期: 2014-06-06
DOI: 10.1002/cphc.201301033
卷: 15, 期:8, 页:1700-1707
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
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.
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
语种: 英语
WOS记录号: WOS:000337521700024
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/144230
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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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

Recommended Citation:
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.
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