Premium
Developing an approach for first‐principles catalyst design: application to carbon‐capture catalysis
Author(s) -
Kulik Heather J.,
Wong Sergio E.,
Baker Sarah E.,
Valdez Carlos A.,
Satcher Joe H.,
Aines Roger D.,
Lightstone Felice C.
Publication year - 2014
Publication title -
acta crystallographica section c
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.304
H-Index - 17
ISSN - 2053-2296
DOI - 10.1107/s2053229613027666
Subject(s) - catalysis , reactivity (psychology) , carbon fibers , ligand (biochemistry) , chemistry , metal , chemical physics , nitrogen , materials science , range (aeronautics) , nanotechnology , computational chemistry , organic chemistry , composite material , medicine , biochemistry , alternative medicine , receptor , pathology , composite number
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 Zn II metals. The comparison of binding, activation and product release energies over a large range of interaction distances and angles suggests that four‐coordinate short Zn II —N sp 3 bond distances favor a rapid turnover for CO 2 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 CO 2 hydration and sequestration.