First-principles study of materials for solar thermochemical gas splitting

Heine Hansen*, Bryce Meredig, Christopher M Wolverton

*Corresponding author for this work

Research output: Contribution to journalConference articlepeer-review


Metal oxide materials may be used in two-step solar thermochemical water-splitting cycles to renewably produce hydrogen. Here, we use first-principles density functional calculations to investigate promising oxide materials for use in these cycles. We present a general analysis of the equilibrium thermodynamics of a two-step metal oxide water splitting cycle, and survey a large number (more than 100) binary oxide redox couples. CeO2 is promising, but the reoxidation at low temperature is kinetically limited due to slow surface processes, however, very little is known about the mechanism. We use DFT to identify stable surface structures containing surface or subsurface oxygen vacancies, H2O or H. We calculate barriers for diffusion of oxygen vacancies, and barriers for dissociation of water and the desorption of hydrogen. Our results show that the surface coverage of adsorbed H may play a key role in the kinetics of water splitting on ceria surfaces.

Original languageEnglish (US)
JournalACS National Meeting Book of Abstracts
StatePublished - Aug 25 2011
Event241st ACS National Meeting and Exposition - Anaheim, CA, United States
Duration: Mar 27 2011Mar 31 2011

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)


Dive into the research topics of 'First-principles study of materials for solar thermochemical gas splitting'. Together they form a unique fingerprint.

Cite this