Molecular structural and morphological characterization of polymer-supported Mo(VI) alkene epoxidation catalysts

被引:50
作者
Leinonen, S
Sherrington, DC
Sneddon, A
McLoughlin, D
Corker, J
Canevali, C
Morazzoni, F
Reedijk, J
Spratt, SBD
机构
[1] Univ Strathclyde, Dept Pure & Appl Chem, Glasgow G1 1XL, Lanark, Scotland
[2] Univ Strathclyde, Dept Biosci, Glasgow G1 1XW, Lanark, Scotland
[3] Univ Southampton, Dept Chem, Southampton SO9 5NH, Hants, England
[4] Univ Milan, Dept Mat Sci, Milan, Italy
[5] Leiden Univ, Leiden Inst Chem, Gorlaeus Labs, NL-2300 RA Leiden, Netherlands
[6] Johnston Matthey Technol Ctr, Reading, Berks, England
基金
英国工程与自然科学研究理事会;
关键词
D O I
10.1006/jcat.1999.2399
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Heterogeneous alkene epoxidation catalysts prepared by immobilization of species derived from MoO2(acac)(2) on two polymers, a polystyrene N-hydroxypropyl aminomethylpyridine resin and a polybenzimidazole resin, are known to behave differently. The two catalyst species have now been characterized extensively in terms of both the molecular structure of the Mo(VI) centers and the resin morphologies, and significant differences have been demonstrated in both aspects. Molecular structural characterization has involved elemental analysis and FTIR, electronic, and X-ray photoelectron spectroscopies, together with EXAFS analysis and associated modeling. Morphological studies have employed high-resolution transmission electron microscopy with Mo mapping, N-2 sorption, and Hg intrusion porosimetry and solvent imbibition measurements. The differences observed account for the observed variation in catalytic behavior, and these structural and morphological differences are discussed in detail. (C) 1999 Academic Press.
引用
收藏
页码:251 / 266
页数:16
相关论文
共 23 条
[11]   ALKENE EPOXIDATIONS CATALYZED BY MO(VI) SUPPORTED ON IMIDAZOLE-CONTAINING POLYMERS .1. SYNTHESIS, CHARACTERIZATION, AND ACTIVITY OF CATALYSTS IN THE EPOXIDATION OF CYCLOHEXENE [J].
MILLER, MM ;
SHERRINGTON, DC .
JOURNAL OF CATALYSIS, 1995, 152 (02) :368-376
[12]   ALKENE EPOXIDATIONS CATALYZED BY MOLYBDENUM(VI) SUPPORTED ON IMIDAZOLE-CONTAINING POLYMERS .3. EPOXIDATION OF OCT-1-ENE AND PROPENE [J].
MILLER, MM ;
SHERRINGTON, DC ;
SIMPSON, S .
JOURNAL OF THE CHEMICAL SOCIETY-PERKIN TRANSACTIONS 2, 1994, (10) :2091-2096
[13]   ROLE OF PEROXYMETALLATION IN SELECTIVE OXIDATIVE PROCESSES [J].
MIMOUN, H .
JOURNAL OF MOLECULAR CATALYSIS, 1980, 7 (01) :1-29
[14]   OXO-SPECIES OF MOLYBDENUM-(V) AND -(6) [J].
MITCHELL, PC .
QUARTERLY REVIEWS, 1966, 20 (01) :103-&
[15]   SPECTROSCOPIC INVESTIGATION OF THE MOLYBDENUM ACTIVE-SITES ON MO-VI HETEROGENEOUS CATALYSTS FOR ALKENE EPOXIDATION [J].
MORAZZONI, F ;
CANEVALI, C ;
DAPRILE, F ;
BIANCHI, CL ;
TEMPESTI, E ;
GIUFFRE, L ;
AIROLDI, G .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (21) :3969-3974
[16]   VARIABLE-TEMPERATURE INFRARED SPECTROSCOPIC STUDY OF SOME MOLYBDENUM BRONZES - EVIDENCE FOR ELECTRON-PHONON COUPLING [J].
MORTIMER, R ;
POWELL, JG ;
GREENBLATT, M ;
MCCARROLL, WH ;
RAMANUJACHARY, KV .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1993, 89 (19) :3603-3609
[17]   Efficient epoxidation of terminal and internal alkenes using t-butylhydroperoxide catalysed by polybenzimidazole-supported Mo(VI)•(PBI•Mo) [J].
Olason, G ;
Sherrington, DC .
MACROMOLECULAR SYMPOSIA, 1998, 131 :127-146
[18]  
Sharpless K.B., 1979, ALDRICHIM ACTA, V12, P63
[19]   MECHANISM OF EPOXIDATION OF OLEFINS BY COVALENT PEROXIDES OF MOLYBDENUM(VI) [J].
SHARPLESS, KB ;
WILLIAMS, DR ;
TOWNSEND, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1972, 94 (01) :295-+
[20]   Preparation, structure and morphology of polymer supports [J].
Sherrington, DC .
CHEMICAL COMMUNICATIONS, 1998, (21) :2275-2286