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题名: Comprehensive structural and spectroscopic study of intrazeolite anchoring of ruthenium carbonyl clusters
作者: Shen, GC;  Liu, AM;  Ichikawa, M
刊名: JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS
发表日期: 1998-05-07
卷: 94, 期:9, 页:1353-1362
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
英文摘要: [Ru-3(CO)(12)] guests in Na56Y were thermally activated from 298 to 363 K, in a hydrogen atmosphere, generating intrazeolitic [H4Ru4(CO)(12)]. Hexaammineruthenium(III) complexes in Na56X have been thermally activated progressively from 298 to 393 K, in CO and H-2 atmospheres. The generation process is via conversion of the intermediate [Ru(NK3)(5)(CO)](2+), Ru-1(CO)(3) to [Ru-6(CO)(18)](2-). The characterization of the structure and properties of these samples used a multi-analytical approach based on FTIR, UV-VIS, EXAFS spectroscopies and CO and H-2 gas chemiscrption. The research encompassed several key points as follows: (i) kinetics of the intrazeolitic diffusion of [Ru-3(CO)(12)] clusters; (ii) oxidation fragmentation under O-2 atmosphere and reductive regeneration under CO and H-2 chemisorption with temperature-programmed heating for the intrazeolite anchoring of [Ru-6(CO)(18)](2-); (iii) internal vs. external confinement of ruthenium carbonyl clusters; (iv) intrazeolite anchoring of ruthenium carbonyl clusters shows a strong reaction with the extraframework Na+ alpha-cage cations, through involvement of the oxygen end of the bridging or equatorial terminal carbonyl ligands; (v) comparison of orbitally degenerate ground-state for free Ru carbonyl clusters vs. the intrazeolitic anchoring site provides a theoretical indication of the symmetry distortion.
关键词[WOS]: NAY ZEOLITE CAGES ;  METAL-CARBONYLS ;  SOLID-STATE ;  CHEMISTRY ;  REACTIVITY ;  SURFACE ;  RU3(CO)12 ;  COMPLEXES ;  HYDROGEN ;  LIGAND
语种: 英语
WOS记录号: WOS:000073580000029
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/138177
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, Dept Chem, Lash Miller Chem Labs, 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. Comprehensive structural and spectroscopic study of intrazeolite anchoring of ruthenium carbonyl clusters[J]. JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS,1998,94(9):1353-1362.
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