Synthesis of 3D Large-Pore Germanosilicate Zeolites Using Imidazolium-Based Long Dications

doi:10.1021/acs.chemmater.9b00959

	Synthesis of 3D Large-Pore Germanosilicate Zeolites Using Imidazolium-Based Long Dications
	Lu, Peng 1,2,3,6; Mayoral, Alvaro 4; Gomez-Hortiguela, Luis 5; Zhang, Yaping 4; Camblor, Miguel A.1
刊名	CHEMISTRY OF MATERIALS
	2019-08-13
卷号	31 期号:15 页码:5484-5493
ISSN号	0897-4756
DOI	10.1021/acs.chemmater.9b00959
通讯作者	Camblor, Miguel A.(macamblor@icmm.csic.es)
英文摘要	Introduction of small molar fractions of Ge in a synthesis system otherwise yielding the monodimensional large-pore zeolite MTW produced three 3D large-pore materials as the Ge fraction increased: BEA, HPM-8, and HPM-7. HPM-8 is a zeolite consisting of an intergrowth of polymorphs D and E of the zeolite Beta family with a large predominance (>80%) of polymorph D, according to DIFFaX simulations and high-resolution scanning transmission electron microscopy analysis. After calcination, HPM-8 becomes remarkably stable upon contact with ambient air. HPM-7 likely possesses the POS topology, which is related to polymorph C. The density of double 4-ring (D4R) units in the crystallized materials increases from BEA to HPM-8 to HPM-7, that is, as the Ge fraction increases. Interestingly, molecular mechanics show that in both HPM-7 and HPM-8, the organic dications prefer to site with their imidazolium rings in close contact with the D4R units as a consequence of a stronger confinement in this position. Indeed, the structure-directing role of these long dications can be explained as a consequence of the appropriate distance match between adjacent D4R units in both zeolite frameworks (and hence the negative charges associated with the occluded fluoride) and the imidazolium rings of these organic dications (and hence the positive charges), which is dictated by the length of the alkyl spacers, thus driving the crystallization pathway toward these particular germanosilicate zeolites.
资助项目	Spanish Ministry of Science, Innovation and Universities[MAT2016-77496-R] ; Spanish Ministry of Science, Innovation and Universities[MAT2015-71117-R] ; National Natural Science Foundation of China[NSFC-21850410448] ; National Natural Science Foundation of China[NSFC-21835002] ; China Scholarship Council (CSC) ; SPST of ShanghaiTech University[EM02161943]
WOS关键词	SILICA ; CRYSTAL ; GE
WOS研究方向	Chemistry ; Materials Science
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000480826900016
资助机构	Spanish Ministry of Science, Innovation and Universities ; Spanish Ministry of Science, Innovation and Universities ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; China Scholarship Council (CSC) ; China Scholarship Council (CSC) ; SPST of ShanghaiTech University ; SPST of ShanghaiTech University ; Spanish Ministry of Science, Innovation and Universities ; Spanish Ministry of Science, Innovation and Universities ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; China Scholarship Council (CSC) ; China Scholarship Council (CSC) ; SPST of ShanghaiTech University ; SPST of ShanghaiTech University ; Spanish Ministry of Science, Innovation and Universities ; Spanish Ministry of Science, Innovation and Universities ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; China Scholarship Council (CSC) ; China Scholarship Council (CSC) ; SPST of ShanghaiTech University ; SPST of ShanghaiTech University ; Spanish Ministry of Science, Innovation and Universities ; Spanish Ministry of Science, Innovation and Universities ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; China Scholarship Council (CSC) ; China Scholarship Council (CSC) ; SPST of ShanghaiTech University ; SPST of ShanghaiTech University
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/173658]
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
通讯作者	Camblor, Miguel A.
作者单位	1.CSIC, ICMM, C Sor Juana Ines de la Cruz 3, Madrid 28049, Spain 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.ShanghaiTech Univ, Sch Phys Sci & Technol, Ctr High Resolut Electron Microscopy ChEM, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China 5.CSIC, ICP, Madrid 28049, Spain 6.Johns Hopkins Univ, Inst Nanobiotechnol WSE, 3400 Charles St, Baltimore, MD 21218 USA
推荐引用方式 GB/T 7714	Lu, Peng,Mayoral, Alvaro,Gomez-Hortiguela, Luis,et al. Synthesis of 3D Large-Pore Germanosilicate Zeolites Using Imidazolium-Based Long Dications[J]. CHEMISTRY OF MATERIALS,2019,31(15):5484-5493.
APA	Lu, Peng,Mayoral, Alvaro,Gomez-Hortiguela, Luis,Zhang, Yaping,&Camblor, Miguel A..(2019).Synthesis of 3D Large-Pore Germanosilicate Zeolites Using Imidazolium-Based Long Dications.CHEMISTRY OF MATERIALS,31(15),5484-5493.
MLA	Lu, Peng,et al."Synthesis of 3D Large-Pore Germanosilicate Zeolites Using Imidazolium-Based Long Dications".CHEMISTRY OF MATERIALS 31.15(2019):5484-5493.