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

Research output: Contribution to journalArticle

37 Citations (Scopus)

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
Pages (from-to)5511-5514
Number of pages4
JournalJournal of the American Chemical Society
Volume138
Issue number17
DOIs
Publication statusPublished - May 4 2016

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Fingerprint Dive into the research topics of 'Solution structures of highly active molecular ir water-oxidation catalysts from density functional theory combined with high-energy X-ray scattering and EXAFS spectroscopy'. Together they form a unique fingerprint.

  • Cite this