Improving Stability of Zeolites in Aqueous Phase via Selective Removal of Structural Defects

被引:86
作者
Prodinger, Sebastian [1 ]
Derewinski, Miroslaw A. [1 ]
Vjunov, Aleksei [1 ]
Burton, Sarah D. [1 ]
Arslan, Ilke [1 ]
Lercher, Johannes A. [1 ,2 ,3 ]
机构
[1] Pacific NW Natl Lab, Inst Integrated Catalysis, POB 999, Richland, WA 99352 USA
[2] Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85748 Garching, Germany
[3] Tech Univ Munich, Catalysis Res Inst, Lichtenbergstr 4, D-85748 Garching, Germany
关键词
NUCLEAR-MAGNETIC-RESONANCE; HYDROPHOBIC ZEOLITES; HYDROXYL-GROUPS; SURFACE-AREA; NMR; SPECTRA; IMPACT; SITES; BETA; FTIR;
D O I
10.1021/jacs.5b12785
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Missing silicon oxygen bonds in zeolites are shown to be the cause for structural instability of zeolites in hot liquid water. Their selective removal drastically improved their structural stability as demonstrated using zeolite beta as example. The defects in the siloxy bonds were capped by reaction with trimethylchlorosilane, and Si-O-Si bonds were eventually formed. Hydrolysis of Si-O-Si bonds of the parent materials and dissolution of silica-oxygen tetrahedra in water causing a decrease in sorption capacity by reprecipitation of dissolved silica and pore blocking was largely mitigated by the treatment. The stability of the modified molecular sieves was monitored by Si-29-MAS NMR, transmission electron micrographs, X-ray diffraction, and adsorption isotherms. The microporosity, sorption capacity, and long-range order of the stabilized material were fully retained even after prolonged exposure to hot liquid water.
引用
收藏
页码:4408 / 4415
页数:8
相关论文
共 43 条
[1]  
Baerlocher Ch., Database of zeolite structures
[2]   The hydrothermal synthesis of zeolites: History and development from the earliest days to the present time [J].
Cundy, CS ;
Cox, PA .
CHEMICAL REVIEWS, 2003, 103 (03) :663-701
[3]   HYDROXYL-GROUPS AND ACID SITES IN NA-ZSM-5 ZEOLITES STUDIES BY IR SPECTROSCOPY [J].
DATKA, J ;
TUZNIK, E .
ZEOLITES, 1985, 5 (04) :230-232
[4]  
DEREWINSKI M, 1991, STUD SURF SCI CATAL, V69, P127
[5]   SYNTHESIS OF MOLECULAR-SIEVE [B]-BEA AND MODIFICATION OF THE BORON SITE [J].
DERUITER, R ;
PAMIN, K ;
KENTGENS, APM ;
JANSEN, JC ;
VANBEKKUM, H .
ZEOLITES, 1993, 13 (08) :611-621
[6]   CALCINATION AND DEBORONATION OF [B]-MFI SINGLE-CRYSTALS [J].
DERUITER, R ;
KENTGENS, APM ;
GROOTENDORST, J ;
JANSEN, JC ;
VANBEKKUM, H .
ZEOLITES, 1993, 13 (02) :128-138
[7]   ON THE INCORPORATION MECHANISM OF B AND AL IN MFI-TYPE ZEOLITE FRAMEWORKS [J].
DERUITER, R ;
JANSEN, JC ;
VANBEKKUM, H .
ZEOLITES, 1992, 12 (01) :56-62
[8]   HIGH-RESOLUTION SI-29 NMR OF DEALUMINATED AND ULTRASTABLE Y-ZEOLITES [J].
ENGELHARDT, G ;
LOHSE, U ;
SAMOSON, A ;
MAGI, M ;
TARMAK, M ;
LIPPMAA, E .
ZEOLITES, 1982, 2 (01) :59-62
[9]   HYDROUS SODIUM SILICATES FROM LAKE MAGADI KENYA - PRECURSORS OF BEDDED CHERT [J].
EUGSTER, HP .
SCIENCE, 1967, 157 (3793) :1177-&
[10]   Cation-induced transformation of boron-coordination in zeolites [J].
Fild, C ;
Shantz, DF ;
Lobo, RF ;
Koller, H .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (13) :3091-3098