Surface-supported metal cluster carbonyls. Chemisorption decomposition and reactivity of hexadecacarbonylhexarhodium supported on alumina, silica-alumina, and magnesia

Smith, Anthony K.; Hugues, F.; Théolier, A.; Basset, Jean‐Marie; Ugo, R.; Zanderighi, G.M.; Bilhou, J. L.; Graydon, W. F.

doi:10.1021/ic50201a030

Cited by 172 publications

(62 citation statements)

References 60 publications

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“…Moreover, Chen et al [31] studied the effect of SBA-15 on Rh/Mn-supported catalysts on CO hydrogenation, and found that the catalytic performance depended on the different chemical properties of SBA-15 modified by different promoters rather than the surface areas. In this work, we also infer that there are some other properties rather than the surface area of silica, such as the role of surface hydroxyl groups on silica mentioned by many researchers [32][33][34][35][36], which affect the catalytic performance of the Rh-Mn-Li/SiO 2 catalysts.…”

Section: Samplesmentioning

confidence: 68%

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Mao

Han

et al. 2013

Journal of Molecular Catalysis A: Chemical

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Section: Samplesmentioning

confidence: 68%

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Mao

Han

et al. 2013

Journal of Molecular Catalysis A: Chemical

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“…Smith et al 38 In summary, all the observations demonstrate the importance of surface hydroxyl groups or water in the chemistry of metal carbonyl clusters on metal oxide surfaces. The chemistry is analogous to that occurring in solutions, but the results are still only qualitative.…”

mentioning

confidence: 83%

Probing Metal Oxide Surface Reactivity with Adsorbate Organometallic Chemistry: Formation of Iridium Carbonyl Clusters on γ-Al₂O₃

and

Gates

1997

Langmuir

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Ir8(CO)22] 2-was formed by surface-mediated synthesis by treatment of [Ir(CO)2(acac)] supported on uncalcined γ-Al2O3 under 1 atm of CO at room temperature. The formation of [Ir8(CO)22] 2-completes the synthesis of a family of iridium carbonyl clusters, including [Ir4(CO)12], [HIr4(CO)11] -, [Ir6(CO)15] 2-, and [Ir8(CO)22] 2-, on the surface of γ-Al2O3. The surface chemistry parallels known solution chemistry of the synthesis of the family of iridium carbonyls. The products formed are controlled largely by the basicity of the solution or surface, and the analogy between the solution and surface chemistry provides a preliminary, qualitative basis for characterizing the basicity of γ-Al2O3 and other metal oxide samples. Decarbonylation of [Ir8(CO)22] 2-on γ-Al2O3 led to nearly uniform tetrahedral Ir4 clusters; it is likely that the Ir-Ir single bond linking two iridium tetrahedral moieties in the precursor [Ir8(CO)22] 2-on γ-Al2O3 was broken during the decarbonylation.

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“…In a well-done investigation (16), it was postulated that surface hydroxyls on A1 2 0 3 are effective in converting the Rh 6 (CO) 16 to a species in which the Rho in the carbonyl is oxidized to Rh ,…”

Section: Isolated Rh Sitesmentioning

confidence: 99%

Site distribution studies of Rh supported on Al2O3—An infrared study of chemisorbed CO

Cavanagh

Yates

1981

The Journal of Chemical Physics

187

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Using infrared spectroscopy, chemisorbed CO has been employed as a surface probe to observe differences in Rh site distributions on Al2O3-supported Rh. It has been found that higher loadings of Rh lead to Rh site distributions resembling those found on Rh(111) single crystals, whereas low Rh loadings produce isolated Rh sites preferentially. The isolated Rh sites yield infrared spectra characteristic of a species Rh(CO)2. Chemisorption of oxygen onto the CO-covered surface effectively eliminates crystalline Rh sites, leaving only the isolated Rh sites which maintain their bonding to CO as seen by infrared spectroscopy. Estimates of the infrared extinction coefficient for Rh(CO)2 have been made. The results are consistent with data from other laboratories which indicate that the Rh is in a Rhd+ oxidation state.

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Surface-supported metal cluster carbonyls. Chemisorption decomposition and reactivity of hexadecacarbonylhexarhodium supported on alumina, silica-alumina, and magnesia

Cited by 172 publications

References 60 publications

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Probing Metal Oxide Surface Reactivity with Adsorbate Organometallic Chemistry: Formation of Iridium Carbonyl Clusters on γ-Al₂O₃

Site distribution studies of Rh supported on Al2O3—An infrared study of chemisorbed CO

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Surface-supported metal cluster carbonyls. Chemisorption decomposition and reactivity of hexadecacarbonylhexarhodium supported on alumina, silica-alumina, and magnesia

Cited by 172 publications

References 60 publications

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Catalytic conversion of syngas into C2+ oxygenates over Rh/SiO2-based catalysts: The remarkable effect of hydroxyls on the SiO2

Probing Metal Oxide Surface Reactivity with Adsorbate Organometallic Chemistry: Formation of Iridium Carbonyl Clusters on γ-Al2O3

Site distribution studies of Rh supported on Al2O3—An infrared study of chemisorbed CO

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Product

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Probing Metal Oxide Surface Reactivity with Adsorbate Organometallic Chemistry: Formation of Iridium Carbonyl Clusters on γ-Al₂O₃