Solution structures of highly active molecular ir water-oxidation catalysts from density functional theory combined with high-energy X-ray scattering and EXAFS spectroscopy

Ke R. Yang, Adam J. Matula, Gihan Kwon, Jiyun Hong, Stafford W. Sheehan, Julianne M. Thomsen, Gary W. Brudvig, Robert H. Crabtree, David M. Tiede, Lin X. Chen, Victor S. Batista*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

64 Scopus citations

Abstract

The solution structures of highly active Ir water-oxidation catalysts are elucidated by combining density functional theory, high-energy X-ray scattering (HEXS), and extended X-ray absorption fine structure (EXAFS) spectroscopy. We find that the catalysts are Ir dimers with mono-μ-O cores and terminal anionic ligands, generated in situ through partial oxidation of a common catalyst precursor. The proposed structures are supported by 1H and 17O NMR, EPR, resonance Raman and UV-vis spectra, electrophoresis, etc. Our findings are particularly valuable to understand the mechanism of water oxidation by highly reactive Ir catalysts. Importantly, our DFTEXAFS-HEXS methodology provides a new in situ technique for characterization of active species in catalytic systems.

Original languageEnglish (US)
Pages (from-to)5511-5514
Number of pages4
JournalJournal of the American Chemical Society
Volume138
Issue number17
DOIs
StatePublished - May 4 2016

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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