In situ growth-etching approach to the preparation of hierarchically macroporous zeolites with high MTO catalytic activity and selectivity

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

	In situ growth-etching approach to the preparation of hierarchically macroporous zeolites with high MTO catalytic activity and selectivity
	Xi, Dongyang 1; Sun, Qiming 1; Xu, Jun 2; Cho, Minhyung 3; Cho, Hae Sung 3; Asahina, Shunsuke 4; Li, Yi 1; Deng, Feng 2; Terasaki, Osamu 3; Yu, Jihong 1
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2014-11-14
卷号	2 期号:42 页码:17994-18004
英文摘要	Silicoaluminophosphate zeolite SAPO-34 with CHA topology is known as one of the best catalysts for methanol-to-olefin (MTO) conversion. In this work, we demonstrate a facile one-step hydrothermal synthesis of hierarchically macroporous SAPO-34 through the etching effect of hydrofluoric acid. The highly crystalline hierarchically macroporous SAPO-34 is prepared as central-holed rhombohedral crystals with particle size of ca. 5-10 mu m that comprise intracrystalline parallel macrochannels of ca. 100 nm. The formation of macroporous structures via in situ growth-etching can be directly imaged by SEM. Strikingly, a particular crystal configuration consisting of eight pyramidal parts has been first observed during the zeolite crystal growth process, which eventually grows to form a perfect rhombohedral shape. The HF etching effect is further elucidated by the analysis of changes of pH values as well as of solid and liquid compositions following the evolution of crystallization. The texture properties, chemical environments of framework atoms, and acidity of the synthesized SAPO-34 are characterized by N-2 adsorption/desorption, MAS NMR and NH3-TPD measurements. The hierarchically macroporous SAPO-34 shows larger micropore volume, slightly stronger acid strength, and lower external surface acidity than its conventional counterpart synthesized without using HF. Consequently, the hierarchically macroporous SAPO-34 exhibits excellent MTO catalytic performance, showing much higher selectivity to ethylene and propylene as well as longer lifetime than the conventional counterpart. In comparison with previously reported methods for the generation of hierarchical porosity, this one-step HF-assisted in situ growth-etching synthetic route is simple, straightforward and cost-effective, which offers a new approach to prepare hierarchically porous zeolites with improved catalytic activity.
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]	SURFACTANT-DIRECTED SYNTHESIS ; MICROPOROUS MATERIALS ; SAPO-34 CATALYSTS ; NMR-SPECTROSCOPY ; SINGLE-CRYSTALS ; COKE FORMATION ; METHANOL ; OLEFINS ; CRYSTALLIZATION ; MESOPOROSITY
收录类别	SCI
语种	英语
WOS记录号	WOS:000343961300037
公开日期	2015-07-14
内容类型	期刊论文
源URL	[http://ir.wipm.ac.cn/handle/112942/1334]
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.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Wuhan 430071, Peoples R China 3.Korea Adv Inst Sci & Technol, Grad Sch EEWS, Taejon 305701, South Korea 4.JEOL, SMBU, Tokyo 1968558, Japan
推荐引用方式 GB/T 7714	Xi, Dongyang,Sun, Qiming,Xu, Jun,et al. In situ growth-etching approach to the preparation of hierarchically macroporous zeolites with high MTO catalytic activity and selectivity[J]. JOURNAL OF MATERIALS CHEMISTRY A,2014,2(42):17994-18004.
APA	Xi, Dongyang.,Sun, Qiming.,Xu, Jun.,Cho, Minhyung.,Cho, Hae Sung.,...&Yu, Jihong.(2014).In situ growth-etching approach to the preparation of hierarchically macroporous zeolites with high MTO catalytic activity and selectivity.JOURNAL OF MATERIALS CHEMISTRY A,2(42),17994-18004.
MLA	Xi, Dongyang,et al."In situ growth-etching approach to the preparation of hierarchically macroporous zeolites with high MTO catalytic activity and selectivity".JOURNAL OF MATERIALS CHEMISTRY A 2.42(2014):17994-18004.