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Synthesis and characterization of open and sandwich-type polyoxometalates reveals visible-light-driven water oxidation via POM-photosensitizer complexesElectronic supplementary information (ESI) available: Synthetic and computational methods, FT-IR/Raman/UV-vis spectra, thermogravimetric studies, cyclic voltammetry measurements, ESI-MS and light-induced water-oxidation studies. See DOI: 10.1039/c2gc16646a
The trivacant triruthenium-substituted polyoxometalate α-K 6 Na[{Ru 3 O 3 (H 2 O)Cl 2 }(SiW 9 O 34 )]·17H 2 O (1) and two sandwich-type Co- and Ni-containing silicotungstates K 11 Na 1 [M 4 (H 2 O) 2 (SiW 9 O 34 ) 2 ]· n H 2 O (M = Co 2+ , Ni 2+ ) (2, 3) based on the same Keggin-type building block...
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| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Online Access: | Get full text |
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| Summary: | The trivacant triruthenium-substituted polyoxometalate α-K
6
Na[{Ru
3
O
3
(H
2
O)Cl
2
}(SiW
9
O
34
)]·17H
2
O
(1)
and two sandwich-type Co- and Ni-containing silicotungstates K
11
Na
1
[M
4
(H
2
O)
2
(SiW
9
O
34
)
2
]·
n
H
2
O (M = Co
2+
, Ni
2+
)
(2, 3)
based on the same Keggin-type building block were obtained through variation of a solution-based protocol. All compounds were investigated with respect to their performance as visible-light-driven water oxidation catalysts (WOCs). Analytical characterizations and photocatalytic reactivity of
(1)
are correlated with results of B97D/Def2-TZVP computation. The WOC activity of
(1)
and
(2)
was found to arise from their immobilization into a recyclable POM-photosensitizer complex (POM-PS). These POM-PS complexes are formed in the initial phase of the reaction, and they prevent POM decomposition into colloidal oxide catalysts.
The challenging question of catalytic species involved in visible-light-driven water oxidation is investigated for two new polyoxometalate-based catalysts. |
|---|---|
| ISSN: | 1463-9262 1463-9270 |
| DOI: | 10.1039/c2gc16646a |