Search: WFRF:(Xu Licheng)
> (2010-2014) >
Visible Light-Drive...
Visible Light-Driven Water Oxidation by a Molecular Ruthenium Catalyst in Homogeneous System
-
- Duan, Lele (author)
- KTH,Organisk kemi
-
- Xu, Yunhua (author)
- KTH,Organisk kemi
-
- Zhang, Pan (author)
- KTH,Molekylär elektronik, CMD
-
show more...
-
- Wang, Mei (author)
- KTH,Molekylär elektronik, CMD
-
- Sun, Licheng (author)
- KTH,Organisk kemi,Molekylär elektronik, CMD
-
show less...
-
(creator_code:org_t)
- 2009-12-08
- 2010
- English.
-
In: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 49:1, s. 209-215
- Related links:
-
https://urn.kb.se/re...
-
show more...
-
https://doi.org/10.1...
-
show less...
Abstract
Subject headings
Close
- Discovery of an efficient catalyst bearing low overpotential toward water oxidation is a key step for light-driven water splitting into dioxygen and dihydrogen. A mononuclear ruthenium complex, Ru(II)L(pic)(2) (1) (H2L = 2,2'-bipyridine-6,6'-dicarboxylic acids pic = 4-picoline), was found capable of oxidizing water eletrochemically at a relatively low potential and promoting light-driven water oxidation using a three-component system composed of a photosensitizer, sacrificial electron acceptor, and complex 1. The detailed electrochemical properties of 1 were studied, and the onset potentials of the electrochemically catalytic curves in pH 7.0 and pH 1.0 solutions are 1.0 and 1.5 V, respectively. The low catalytic potential of 1 under neutral conditions allows the use of [Ru(bpy)(3)](2+) and even [Ru(dmbpy)(3)](2+) as a photosensitizer for photochemical water oxidation. Two different sacrificial electron acceptors, [Co(NH3)(5)Cl]Cl-2 and Na2S2O8, were used to generate the oxidized state of ruthenium tris(2,2'-bipyridyl) photosensitizers. In addition, a two-hour photolysis of I in a pH TO phosphate buffer did not lead to obvious degradation, indicating the good photostability of our catalyst. However, under conditions of light-driven water oxidation, the catalyst deactivates quickly. In both solution and the solid state under aerobic conditions, complex 1 gradually decomposed via oxidative degradation of its ligands, and two of the decomposed products, sp(3) C-H bond oxidized Ru complexes, were identified. The capability of oxidizing the sp(3) C-H bond implies the presence of a highly oxidizing Ru species, which might also cause the final degradation of the catalyst.
Subject headings
- NATURVETENSKAP -- Kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences (hsv//eng)
Keyword
- O-O BOND
- ARTIFICIAL PHOTOSYNTHESIS
- FUNCTIONAL-MODEL
- EXCITED-STATE
- RU(II) COMPLEXES
- REDOX PROPERTIES
- PHOTOSYSTEM-II
- O-2 EVOLUTION
- OXYGEN
- LIGAND
- Chemistry
- Kemi
Publication and Content Type
- ref (subject category)
- art (subject category)
Find in a library
To the university's database