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

Gonghu Li; Eduardo M. Sproviero; Robert C. Snoeberger; Nobuhito Iguchi; James D. Blakemore; Robert H. Crabtree; Gary W. Brudvig; Victor S. Batista

doi:10.1039/b818708h

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

Gonghu Li, Eduardo M. Sproviero, Robert C. Snoeberger, Nobuhito Iguchi, James D. Blakemore, Robert H. Crabtree, Gary W. Brudvig, Victor S. Batista

Yale University

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

65 Citations (Scopus)

Abstract

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 - oxo manganese water oxidation catalyst [H₂O(terpy)Mnⁱⁱⁱ(-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.

Original language	English
Pages (from-to)	230-238
Number of pages	9
Journal	Energy and Environmental Science
Volume	2
Issue number	2
DOIs	https://doi.org/10.1039/b818708h
Publication status	Published - Aug 31 2009

ASJC Scopus subject areas

Environmental Chemistry
Renewable Energy, Sustainability and the Environment
Nuclear Energy and Engineering
Pollution

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Deposition of an oxomanganese water oxidation catalyst on TiO₂ nanoparticles : Computational modeling, assembly and characterization. / Li, Gonghu; Sproviero, Eduardo M.; Snoeberger, Robert C.; Iguchi, Nobuhito; Blakemore, James D.; Crabtree, Robert H.; Brudvig, Gary W.; Batista, Victor S.

In: Energy and Environmental Science, Vol. 2, No. 2, 31.08.2009, p. 230-238.

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

Li, Gonghu ; Sproviero, Eduardo M. ; Snoeberger, Robert C. ; Iguchi, Nobuhito ; Blakemore, James D. ; Crabtree, Robert H. ; Brudvig, Gary W. ; Batista, Victor S. / Deposition of an oxomanganese water oxidation catalyst on TiO₂ nanoparticles : Computational modeling, assembly and characterization. In: Energy and Environmental Science. 2009 ; Vol. 2, No. 2. pp. 230-238.

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abstract = "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 - oxo manganese water oxidation catalyst [H2O(terpy)Mniii(-O)2 Mniv(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.",

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N2 - 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 - oxo manganese water oxidation catalyst [H2O(terpy)Mniii(-O)2 Mniv(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.

AB - 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 - oxo manganese water oxidation catalyst [H2O(terpy)Mniii(-O)2 Mniv(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.

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