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题名: Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization
作者: Shen, GC;  Liu, AM;  Ichikawa, M
刊名: INORGANIC CHEMISTRY
发表日期: 1998-10-19
卷: 37, 期:21, 页:5497-5506
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Inorganic & Nuclear
研究领域[WOS]: Chemistry
英文摘要: The synthesis of the intrafaujasite anchoring of ruthenium carbonyl clusters involves the adsorption of metal carbonyl species or metal ion exchange into faujasite cages followed by reductive carbonylation under an atmosphere of CO and H-2. The characterization of the structure and properties of these samples was based on a multianalytical approach, including FT-IR, UV-vis, PXRD, and EXAFS spectroscopies, CO/H-2 gas chemisorption, and (CO)-C-13 isotopic exchange. From this study, several key points emerge. (a) [Ru-3(CO)(12)] clusters thermally diffused into dehydrated faujasite cages. (b) [Ru-3(CO)(12)] guests in Na56Y were thermally activated, in a hydrogen atmosphere, generating intrafaujasite [H4Ru4(CO)(12)]. (c) Hexammineruthenium(III) complexes in Na56X and Na56Y underwent progressive thermal activation, in a CO and H-2 atmosphere. The generation process was considered to occur through conversion of the intermediates [Ru(NH3)(5)(CO)](2+) and Ru-1(CO)(3) to [Ru-6(CO)(18)](2-). (d) A rapid (CO)-C-13/ (CO)-C-12 isotopic exchange was found to reversibly occur for [Ru-6(CO)(18)](2-)/Na56X under H-2 coexistence. (e) Internal and external confinement of ruthenium carbonyl clusters were compared. (f) Oxidation fragmentation under an O-2 atmosphere and reductive regeneration under a CO and H-2 atmosphere were found to reversibly occur for [Ru-6(CO)(18)](2-) guests. (g) Intrafaujasite anchoring of ruthenium carbonyl clusters showed a strong interaction with the extraframework Na+ alpha-cage cations, through involvement of the oxygen end of the bridging or equatorial terminal carbonyl ligands.
关键词[WOS]: METAL-CARBONYLS ;  COBALT CLUSTERS ;  SOLID-STATE ;  ZEOLITES ;  REACTIVITY ;  COMPLEXES ;  HYDROGEN ;  SURFACE ;  H4RU4(CO)12 ;  RU3(CO)12
语种: 英语
WOS记录号: WOS:000076613700018
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/138185
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Univ Toronto, Lash Miller Chem Labs, Dept Chem, Toronto, ON M5S 3H6, Canada
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Hokkaido Univ, Catalysis Res Ctr, Sapporo, Hokkaido 060, Japan

Recommended Citation:
Shen, GC,Liu, AM,Ichikawa, M. Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization[J]. INORGANIC CHEMISTRY,1998,37(21):5497-5506.
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