Hydrothermal and solid-state transformation of ruthenium-supported Keggin-type heteropolytungstates [XW 11O 39{Ru(II)(benzene) (H 2O)}] n- (X = P (n = 5), Si (n = 6), Ge (n = 6)) to ruthenium-substituted Keggin-type heteropolytungstates

Shuhei Ogo, Mayumi Miyamoto, Yusuke Ide, Tsuneji Sano, Masahiro Sadakane

Research output: Contribution to journalArticle

28 Citations (Scopus)

Abstract

A new pathway for the preparation of mono-ruthenium (Ru)(iii)-substituted Keggin-type heteropolytungstates with an aqua ligand, [PW 11O 39Ru(iii)(H 2O)] 4- (1a), [SiW 11O 39Ru(iii)(H 2O)] 5- (1b) and [GeW 11O 39Ru(iii)(H 2O)] 5- (1c), using [Ru(ii)(benzene)Cl 2] 2 as a Ru source was described. Compounds 1a-1c were prepared by reacting [XW 11O 39] n- (X = P, Si and Ge) with [Ru(ii)(benzene)Cl 2] 2 under hydrothermal condition and were isolated as caesium salts. Ru(benzene)-supported heteropolytungstates, [PW 11O 39{Ru(ii)(benzene)(H 2O)}] 5- (2a), [SiW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2b) and [GeW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2c), were first produced in the reaction media, and then transformed to 1a, 1b and 1c, respectively, under hydrothermal conditions. Calcination of Ru(benzene)-supported heteropolytungstates, 2a, 2b and 2c, in the solid state produced mixtures of 1a, 1b and 1c with CO (carbon monoxide)-coordinated complexes, [PW 11O 39Ru(ii)(CO)] 5- (4a), [SiW 11O 39Ru(ii)(CO)] 6- (4b) and [GeW 11O 39Ru(ii)(CO)] 6- (4c), respectively. From comparison of their catalytic activities in water oxidation reaction, it was indicated that ruthenium should be incorporated in the heteropolytungstate in order to promote catalytic activity.

Original languageEnglish
Pages (from-to)9901-9907
Number of pages7
JournalDalton Transactions
Volume41
Issue number33
DOIs
Publication statusPublished - 2012 Sep 7
Externally publishedYes

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Ruthenium
Benzene
Carbon Monoxide
Catalyst activity
Cesium
Polysilicon
Calcination
Salts
Ligands
Oxidation

ASJC Scopus subject areas

  • Inorganic Chemistry

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Hydrothermal and solid-state transformation of ruthenium-supported Keggin-type heteropolytungstates [XW 11O 39{Ru(II)(benzene) (H 2O)}] n- (X = P (n = 5), Si (n = 6), Ge (n = 6)) to ruthenium-substituted Keggin-type heteropolytungstates. / Ogo, Shuhei; Miyamoto, Mayumi; Ide, Yusuke; Sano, Tsuneji; Sadakane, Masahiro.

In: Dalton Transactions, Vol. 41, No. 33, 07.09.2012, p. 9901-9907.

Research output: Contribution to journalArticle

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title = "Hydrothermal and solid-state transformation of ruthenium-supported Keggin-type heteropolytungstates [XW 11O 39{Ru(II)(benzene) (H 2O)}] n- (X = P (n = 5), Si (n = 6), Ge (n = 6)) to ruthenium-substituted Keggin-type heteropolytungstates",
abstract = "A new pathway for the preparation of mono-ruthenium (Ru)(iii)-substituted Keggin-type heteropolytungstates with an aqua ligand, [PW 11O 39Ru(iii)(H 2O)] 4- (1a), [SiW 11O 39Ru(iii)(H 2O)] 5- (1b) and [GeW 11O 39Ru(iii)(H 2O)] 5- (1c), using [Ru(ii)(benzene)Cl 2] 2 as a Ru source was described. Compounds 1a-1c were prepared by reacting [XW 11O 39] n- (X = P, Si and Ge) with [Ru(ii)(benzene)Cl 2] 2 under hydrothermal condition and were isolated as caesium salts. Ru(benzene)-supported heteropolytungstates, [PW 11O 39{Ru(ii)(benzene)(H 2O)}] 5- (2a), [SiW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2b) and [GeW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2c), were first produced in the reaction media, and then transformed to 1a, 1b and 1c, respectively, under hydrothermal conditions. Calcination of Ru(benzene)-supported heteropolytungstates, 2a, 2b and 2c, in the solid state produced mixtures of 1a, 1b and 1c with CO (carbon monoxide)-coordinated complexes, [PW 11O 39Ru(ii)(CO)] 5- (4a), [SiW 11O 39Ru(ii)(CO)] 6- (4b) and [GeW 11O 39Ru(ii)(CO)] 6- (4c), respectively. From comparison of their catalytic activities in water oxidation reaction, it was indicated that ruthenium should be incorporated in the heteropolytungstate in order to promote catalytic activity.",
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T1 - Hydrothermal and solid-state transformation of ruthenium-supported Keggin-type heteropolytungstates [XW 11O 39{Ru(II)(benzene) (H 2O)}] n- (X = P (n = 5), Si (n = 6), Ge (n = 6)) to ruthenium-substituted Keggin-type heteropolytungstates

AU - Ogo, Shuhei

AU - Miyamoto, Mayumi

AU - Ide, Yusuke

AU - Sano, Tsuneji

AU - Sadakane, Masahiro

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AB - A new pathway for the preparation of mono-ruthenium (Ru)(iii)-substituted Keggin-type heteropolytungstates with an aqua ligand, [PW 11O 39Ru(iii)(H 2O)] 4- (1a), [SiW 11O 39Ru(iii)(H 2O)] 5- (1b) and [GeW 11O 39Ru(iii)(H 2O)] 5- (1c), using [Ru(ii)(benzene)Cl 2] 2 as a Ru source was described. Compounds 1a-1c were prepared by reacting [XW 11O 39] n- (X = P, Si and Ge) with [Ru(ii)(benzene)Cl 2] 2 under hydrothermal condition and were isolated as caesium salts. Ru(benzene)-supported heteropolytungstates, [PW 11O 39{Ru(ii)(benzene)(H 2O)}] 5- (2a), [SiW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2b) and [GeW 11O 39{Ru(ii)(benzene)(H 2O)}] 6- (2c), were first produced in the reaction media, and then transformed to 1a, 1b and 1c, respectively, under hydrothermal conditions. Calcination of Ru(benzene)-supported heteropolytungstates, 2a, 2b and 2c, in the solid state produced mixtures of 1a, 1b and 1c with CO (carbon monoxide)-coordinated complexes, [PW 11O 39Ru(ii)(CO)] 5- (4a), [SiW 11O 39Ru(ii)(CO)] 6- (4b) and [GeW 11O 39Ru(ii)(CO)] 6- (4c), respectively. From comparison of their catalytic activities in water oxidation reaction, it was indicated that ruthenium should be incorporated in the heteropolytungstate in order to promote catalytic activity.

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