Communication: Water activation and splitting by single metal-atom anions
Abstract
We report experimental and computational results pertaining to the activation and splitting of single water molecules by single atomic platinum anions. The anion photoelectron spectra of [Pt(H2O)]−, formed under different conditions, exhibit spectral features that are due to the anion-molecule complex, Pt−(H2O), and to the reaction intermediates, HPtOH− and H2PtO−, in which one and two O–H bonds have been broken, respectively. Additionally, the observations of PtO− and H2+ in mass spectra strongly imply that water splitting via the reaction Pt− + H2O → PtO− + H2 has occurred. Extending these studies to nickel and palladium shows that they too are able to activate single water molecules, as evidenced by the formation of the reaction intermediates, HNiOH− and HPdOH−. Computations at the coupled cluster singles and doubles with perturbatively connected triples level of theory provide structures and vertical detachment energies (VDEs) for both HMOH− and H2MO− intermediates. The calculated and measured VDE values are in good agreement and thus support their identification.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Dec 10, 2018
- Source ID
- 10.1063/1.5050913
Entities
People
- Evangelos Miliordos
- Gaoxiang Liu
- Kit H Bowen
- Martin Tschurl
- Sandra M Ciborowski
- Sotiris Xantheas
- Ulrich Boesl
- Ulrich Heiz
- Xinxing Zhang
Organizations
- Air Force Office of Scientific Research
- Division of Chemistry
- Johns Hopkins University
- Nankai University
- Pacific Northwest National Laboratory
- Technical University of Munich
- United States Department of Energy
- University of Washington