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Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization
Shen, GC; Liu, AM; Ichikawa, M
刊名INORGANIC CHEMISTRY
1998-10-19
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
关键词[WOS]METAL-CARBONYLS ; COBALT CLUSTERS ; SOLID-STATE ; ZEOLITES ; REACTIVITY ; COMPLEXES ; HYDROGEN ; SURFACE ; H4RU4(CO)12 ; RU3(CO)12
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.
语种英语
WOS记录号WOS:000076613700018
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文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/138185
专题中国科学院大连化学物理研究所
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
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GB/T 7714
Shen, GC,Liu, AM,Ichikawa, M. Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization[J]. INORGANIC CHEMISTRY,1998,37(21):5497-5506.
APA Shen, GC,Liu, AM,&Ichikawa, M.(1998).Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization.INORGANIC CHEMISTRY,37(21),5497-5506.
MLA Shen, GC,et al."Ruthenium carbonyl clusters in faujasite cages: Synthesis and characterization".INORGANIC CHEMISTRY 37.21(1998):5497-5506.
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