High performance nanosheet-like silicoaluminophosphate molecular sieves: synthesis, 3D EDT structural analysis and MTO catalytic studies

CORC > 武汉物理与数学研究所 > 中国科学院武汉物理与数学研究所 > 磁共振应用研究部

	High performance nanosheet-like silicoaluminophosphate molecular sieves: synthesis, 3D EDT structural analysis and MTO catalytic studies
	Sun, Qiming 1; Ma, Yanhang 2; Wang, Ning 1; Li, Xu 1; Xi, Dongyang 1; Xu, Jun 3; Deng, Feng 3; Yoon, Kyung Byung 4; Oleynikov, Peter 2; Terasaki, Osamu 5,6
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2014-11-14
卷号	2 期号:42 页码:17828-17839
英文摘要	Nanosheet-like silicoaluminophosphate (SAPO) molecular sieves SAPO-34 (CHA-type) and SAPO-18 (AEI-type) with different silicon contents were synthesized under hydrothermal conditions by using tetraethylammonium hydroxide as the template. Three-dimensional electron diffraction tomography (3D EDT) technique was applied for ab initio structure solutions. Electron microscopy observations confirmed the existence of defects, i.e., intergrowth of CHA- and AEI-type frameworks caused by the different stacking manners of double 6-ring layers, but the layers were highly coherent along c direction. Compositions, acidities, chemical environments, and texture properties of all the samples were characterized by ICP, EDS, NH3-TPD, MAS NMR, and N-2 adsorption-desorption measurements. The catalytic performances of methanol-to-olefin (MTO) reactions over nano SAPO catalysts with different silicon contents were systematically studied. All of these catalysts showed excellent catalytic activity, among which SAPO-34 showed superior catalytic performance compared to SAPO-18. DFT calculations were utilized to study the different catalytic performance of CHA and AEI. Significantly to date, SAPO-34 with the lowest silicon content exhibited the longest catalyst lifetime and the lowest coking rate in the MTO reaction than any of the reported catalysts, tested under similar conditions. The straight 8-ring pore channel along the c direction provided the optimum diffusion pathway as well as the shortest diffusion length for reactant and generated olefins, thus significantly reduced the coking rate. This work demonstrates that a 3D EDT approach combined with TEM and EDS analysis from a single nanocrystal can provide a clear crystal structure, crystal orientation and compositional information of nanocrystals, which are useful for the better understanding of the catalytic performance of nanosized crystalline catalysts.
WOS标题词	Science & Technology ; Physical Sciences ; Technology
类目[WOS]	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
研究领域[WOS]	Chemistry ; Energy & Fuels ; Materials Science
关键词[WOS]	METHANOL-TO-OLEFIN ; STATE NMR-SPECTROSCOPY ; BRONSTED ACID SITES ; ZEOLITE STRUCTURES ; SILICON INCORPORATION ; SAPO-34 CATALYSTS ; CONVERSION ; DEACTIVATION ; HYDROCARBONS ; SELECTIVITY
收录类别	SCI
语种	英语
WOS记录号	WOS:000343961300017
公开日期	2015-07-14
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/1361]
专题	武汉物理与数学研究所_磁共振应用研究部
作者单位	1.Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China 2.Stockholm Univ, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden 3.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan Ctr Magnet Resonance, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan 430071, Peoples R China 4.Sogang Univ, Dept Chem, Seoul 121742, South Korea 5.Stockholm Univ, Berzelii Ctr EXSELENT Porous Mat, Dept Mat & Environm Chem, S-10691 Stockholm, Sweden 6.Korea Adv Inst Sci & Technol, Grad Sch EEWS, BK21Plus, Taejon 305701, South Korea
推荐引用方式 GB/T 7714	Sun, Qiming,Ma, Yanhang,Wang, Ning,et al. High performance nanosheet-like silicoaluminophosphate molecular sieves: synthesis, 3D EDT structural analysis and MTO catalytic studies[J]. JOURNAL OF MATERIALS CHEMISTRY A,2014,2(42):17828-17839.
APA	Sun, Qiming.,Ma, Yanhang.,Wang, Ning.,Li, Xu.,Xi, Dongyang.,...&Yu, Jihong.(2014).High performance nanosheet-like silicoaluminophosphate molecular sieves: synthesis, 3D EDT structural analysis and MTO catalytic studies.JOURNAL OF MATERIALS CHEMISTRY A,2(42),17828-17839.
MLA	Sun, Qiming,et al."High performance nanosheet-like silicoaluminophosphate molecular sieves: synthesis, 3D EDT structural analysis and MTO catalytic studies".JOURNAL OF MATERIALS CHEMISTRY A 2.42(2014):17828-17839.