Surface Organometallic Chemistry: Chemisorption and Thermodecomposition of Ru3(Co)12 on Partially Hydroxylated Magnesia and Related Oxides

Lindora D'Ornelas; Albert Theolier; Agnès Choplin; Jean Marie Basset

doi:10.1021/ic00280a034

Surface Organometallic Chemistry: Chemisorption and Thermodecomposition of Ru₃(Co)₁₂ on Partially Hydroxylated Magnesia and Related Oxides

Lindora D'Ornelas, Albert Theolier, Agnès Choplin^*, Jean Marie Basset

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

The reaction between Ru₃(CO)₁₂ and the surface of fully or partially hydroxylated magnesia leads to the anionic cluster [HRu₃(CO)₁₁]^-(Mg²⁺)_1/2 ([HRu₃(CO)₁₁]^- = [1]^-). The presence of [1]^- at the surface has been deduced from in situ IR and mass balance experiments; finally [1]^- has been extracted from the surface by [PPN]Cl. Formation of [1]^- from Ru₃(CO)₁₂ occurs also on the surface of zinc and lanthanum oxides. During programmed thermal decomposition of [1]^- on magnesia under vacuum or controlled atmosphere, various species have been evidenced depending on temperature and hydroxylation degree of the support: mononuclear Ru^II(CO)_n(OMg<)₂ and metallic particles of ruthenium (10-15 Å) covered with undissociated carbon monoxide. Simultaneously, three types of reactions involving the cluster carbonyl ligands occur: water gas shift reaction (which transforms those ligands into CO₂ and H₂), CO dismutation to CO₂ and surface carbon, and methanation. The water gas shift reaction is tentatively attributed to the anionic cluster while the latter two are attributed to the metal particles.

Original language	English (US)
Pages (from-to)	1261-1265
Number of pages	5
Journal	Inorganic chemistry
Volume	27
Issue number	7
DOIs	https://doi.org/10.1021/ic00280a034
State	Published - 1988
Externally published	Yes

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Inorganic Chemistry

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@article{25e9efb6e28b44ff9e8070de0824839d,

title = "Surface Organometallic Chemistry: Chemisorption and Thermodecomposition of Ru3(Co)12 on Partially Hydroxylated Magnesia and Related Oxides",

abstract = "The reaction between Ru3(CO)12 and the surface of fully or partially hydroxylated magnesia leads to the anionic cluster [HRu3(CO)11]-(Mg2+)1/2 ([HRu3(CO)11]- = [1]-). The presence of [1]- at the surface has been deduced from in situ IR and mass balance experiments; finally [1]- has been extracted from the surface by [PPN]Cl. Formation of [1]- from Ru3(CO)12 occurs also on the surface of zinc and lanthanum oxides. During programmed thermal decomposition of [1]- on magnesia under vacuum or controlled atmosphere, various species have been evidenced depending on temperature and hydroxylation degree of the support: mononuclear RuII(CO)n(OMg<)2 and metallic particles of ruthenium (10-15 {\AA}) covered with undissociated carbon monoxide. Simultaneously, three types of reactions involving the cluster carbonyl ligands occur: water gas shift reaction (which transforms those ligands into CO2 and H2), CO dismutation to CO2 and surface carbon, and methanation. The water gas shift reaction is tentatively attributed to the anionic cluster while the latter two are attributed to the metal particles.",

author = "Lindora D'Ornelas and Albert Theolier and Agn{\`e}s Choplin and Basset, {Jean Marie}",

year = "1988",

doi = "10.1021/ic00280a034",

language = "English (US)",

volume = "27",

pages = "1261--1265",

journal = "Inorganic chemistry",

issn = "0020-1669",

publisher = "American Chemical Society",

number = "7",

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T1 - Surface Organometallic Chemistry

T2 - Chemisorption and Thermodecomposition of Ru3(Co)12 on Partially Hydroxylated Magnesia and Related Oxides

AU - D'Ornelas, Lindora

AU - Theolier, Albert

AU - Choplin, Agnès

AU - Basset, Jean Marie

PY - 1988

Y1 - 1988

N2 - The reaction between Ru3(CO)12 and the surface of fully or partially hydroxylated magnesia leads to the anionic cluster [HRu3(CO)11]-(Mg2+)1/2 ([HRu3(CO)11]- = [1]-). The presence of [1]- at the surface has been deduced from in situ IR and mass balance experiments; finally [1]- has been extracted from the surface by [PPN]Cl. Formation of [1]- from Ru3(CO)12 occurs also on the surface of zinc and lanthanum oxides. During programmed thermal decomposition of [1]- on magnesia under vacuum or controlled atmosphere, various species have been evidenced depending on temperature and hydroxylation degree of the support: mononuclear RuII(CO)n(OMg<)2 and metallic particles of ruthenium (10-15 Å) covered with undissociated carbon monoxide. Simultaneously, three types of reactions involving the cluster carbonyl ligands occur: water gas shift reaction (which transforms those ligands into CO2 and H2), CO dismutation to CO2 and surface carbon, and methanation. The water gas shift reaction is tentatively attributed to the anionic cluster while the latter two are attributed to the metal particles.

AB - The reaction between Ru3(CO)12 and the surface of fully or partially hydroxylated magnesia leads to the anionic cluster [HRu3(CO)11]-(Mg2+)1/2 ([HRu3(CO)11]- = [1]-). The presence of [1]- at the surface has been deduced from in situ IR and mass balance experiments; finally [1]- has been extracted from the surface by [PPN]Cl. Formation of [1]- from Ru3(CO)12 occurs also on the surface of zinc and lanthanum oxides. During programmed thermal decomposition of [1]- on magnesia under vacuum or controlled atmosphere, various species have been evidenced depending on temperature and hydroxylation degree of the support: mononuclear RuII(CO)n(OMg<)2 and metallic particles of ruthenium (10-15 Å) covered with undissociated carbon monoxide. Simultaneously, three types of reactions involving the cluster carbonyl ligands occur: water gas shift reaction (which transforms those ligands into CO2 and H2), CO dismutation to CO2 and surface carbon, and methanation. The water gas shift reaction is tentatively attributed to the anionic cluster while the latter two are attributed to the metal particles.

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U2 - 10.1021/ic00280a034

DO - 10.1021/ic00280a034

M3 - Article

AN - SCOPUS:0000723127

SN - 0020-1669

VL - 27

SP - 1261

EP - 1265

JO - Inorganic chemistry

JF - Inorganic chemistry

IS - 7

ER -

Surface Organometallic Chemistry: Chemisorption and Thermodecomposition of Ru₃(Co)₁₂ on Partially Hydroxylated Magnesia and Related Oxides

Abstract

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