Deposition of an oxomanganese water oxidation catalyst on TiO2 nanoparticles: computational modeling, assembly and characterization

被引：59
作者：
Li, Gonghu [1 ]
Sproviero, Eduardo M. [1 ]
Snoeberger, Robert C., III [1 ]
Iguchi, Nobuhito [1 ]
Blakemore, James D. [1 ]
Crabtree, Robert H. [1 ]
Brudvig, Gary W. [1 ]
Batista, Victor S. [1 ]
机构：
[1] Yale Univ, Dept Chem, New Haven, CT 06520 USA
来源：
ENERGY & ENVIRONMENTAL SCIENCE | 2009年 / 2卷 / 02期
基金：
美国国家科学基金会;
关键词：
OXYGEN-EVOLVING CENTER; MOLECULAR-DYNAMICS SIMULATIONS; PHOTOSYSTEM-II; O-2-EVOLVING COMPLEX; TITANIUM-DIOXIDE; MN(II)-TERPYRIDINE COMPLEXES; DIMANGANESE COMPLEX; HYDROGEN GENERATION; MANGANESE CLUSTER; FUNCTIONAL-MODEL;
D O I：
10.1039/b818708h
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Inexpensive water oxidation catalysts are needed to develop photocatalytic solar cells that mimic photosynthesis and produce fuel from sunlight and water. This paper reports the successful attachment of a dinuclear di-mu-oxo manganese water oxidation catalyst [H2O(terpy)Mn-III(mu-O)(2) Mn-IV(terpy)H2O](NO3)(3) (1, terpy = 2,2':6'2 ''-terpyridine) onto TiO2 nanoparticles (NPs) via direct adsorption, or in situ synthesis. The resulting surface complexes are characterized by EPR and UV-visible spectroscopy, electrochemical measurements and computational modeling. We conclude that the mixed-valence (III, IV) state of 1 attaches to near-amorphous TiO2 NPs by substituting one of its water ligands by the TiO2 NP, as suggested by low-temperature (7 K) EPR data. In contrast, the analogous attachment onto well-crystallized TiO2 NPs leads to dimerization of 1 forming Mn(IV) tetramers on the TiO2 surface as suggested by EPR spectroscopy and electrochemical studies.
引用
收藏
页码：230 / 238
页数：9
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