Domain structure for an amorphous iridium-oxide water-oxidation catalyst characterized by X-ray pair distribution function analysis

Jier Huang; James D. Blakemore; Diego Fazi; Oleksandr Kokhan; Nathan D. Schley; Robert H. Crabtree; Gary W. Brudvig; David M. Tiede

doi:10.1039/c3cp54878c

Domain structure for an amorphous iridium-oxide water-oxidation catalyst characterized by X-ray pair distribution function analysis

Jier Huang, James D. Blakemore, Diego Fazi, Oleksandr Kokhan, Nathan D. Schley, Robert H. Crabtree, Gary W. Brudvig, David M. Tiede

Yale University

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

25 Citations (Scopus)

Abstract

The domain structure of an amorphous, "blue layer" iridium-oxide water-oxidation catalyst film (BL) electrodeposited from the soluble precursor complex, [Cp*Ir(H₂O)₃]SO₄, was characterized by X-ray pair distribution function (PDF) analysis. The results show that the experimental PDF can be fit remarkably well using a single Ir ₅O₂₂ cluster extracted from the rutile lattice. The model includes distortions that indicate the presence of Ir(μ-O)₃Ir or distorted Ir(μ-O)₂Ir substructures, and hence deviations from a rutile structure. The five Ir atom cluster is suggested to represent the population-averaged distribution of metal-oxo clusters in the film. BL is found to be distinguished from other amorphous film water-oxidation catalysts because of the remarkably small domain size and homogeneity. As such, the blue layer catalyst provides a model for investigating ligand-determined metal-oxide cluster assembly and catalyst mechanism. This journal is

Original language	English
Pages (from-to)	1814-1819
Number of pages	6
Journal	Physical Chemistry Chemical Physics
Volume	16
Issue number	5
DOIs	https://doi.org/10.1039/c3cp54878c
Publication status	Published - Feb 7 2014

ASJC Scopus subject areas

Physics and Astronomy(all)
Physical and Theoretical Chemistry

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Domain structure for an amorphous iridium-oxide water-oxidation catalyst characterized by X-ray pair distribution function analysis. / Huang, Jier; Blakemore, James D.; Fazi, Diego; Kokhan, Oleksandr; Schley, Nathan D.; Crabtree, Robert H.; Brudvig, Gary W.; Tiede, David M.

In: Physical Chemistry Chemical Physics, Vol. 16, No. 5, 07.02.2014, p. 1814-1819.

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

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abstract = "The domain structure of an amorphous, {"}blue layer{"} iridium-oxide water-oxidation catalyst film (BL) electrodeposited from the soluble precursor complex, [Cp*Ir(H2O)3]SO4, was characterized by X-ray pair distribution function (PDF) analysis. The results show that the experimental PDF can be fit remarkably well using a single Ir 5O22 cluster extracted from the rutile lattice. The model includes distortions that indicate the presence of Ir(μ-O)3Ir or distorted Ir(μ-O)2Ir substructures, and hence deviations from a rutile structure. The five Ir atom cluster is suggested to represent the population-averaged distribution of metal-oxo clusters in the film. BL is found to be distinguished from other amorphous film water-oxidation catalysts because of the remarkably small domain size and homogeneity. As such, the blue layer catalyst provides a model for investigating ligand-determined metal-oxide cluster assembly and catalyst mechanism. This journal is",

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AU - Schley, Nathan D.

AU - Crabtree, Robert H.

AU - Brudvig, Gary W.

AU - Tiede, David M.

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