Developing an approach for first-principles catalyst design: Application to carbon-capture catalysis

Heather J. Kulik, Sergio E. Wong, Sarah E. Baker, Carlos A. Valdez, Joe H. Satcher, Roger D. Aines, Felice C Lightstone

Research output: Contribution to journalArticlepeer-review

11 Scopus citations


An approach to catalyst design is presented in which local potential energy surface models are first built to elucidate design principles and then used to identify larger scaffold motifs that match the target geometries. Carbon sequestration via hydration is used as the model reaction, and three- and four-coordinate sp 2 or sp 3 nitrogen-ligand motifs are considered for ZnII metals. The comparison of binding, activation and product release energies over a large range of interaction distances and angles suggests that four-coordinate short ZnII - Nsp 3 bond distances favor a rapid turnover for CO2 hydration. This design strategy is then confirmed by computationally characterizing the reactivity of a known mimic over a range of metal-nitrogen bond lengths. A search of existing catalysts in a chemical database reveals structures that match the target geometry from model calculations, and subsequent calculations have identified these structures as potentially effective for CO2 hydration and sequestration.

Original languageEnglish (US)
Pages (from-to)123-131
Number of pages9
JournalActa Crystallographica Section C: Structural Chemistry
Issue number2
StatePublished - 2014
Externally publishedYes


  • carbonic anhydrase mimics
  • catalyst design
  • computational materials discovery
  • density functional theory
  • potential energy surfaces
  • reaction coordinates
  • zinc

ASJC Scopus subject areas

  • Inorganic Chemistry
  • Physical and Theoretical Chemistry
  • Materials Chemistry
  • Condensed Matter Physics
  • Medicine(all)


Dive into the research topics of 'Developing an approach for first-principles catalyst design: Application to carbon-capture catalysis'. Together they form a unique fingerprint.

Cite this