title: Developing an approach for first-principles catalyst design: application to carbon-capture catalysis.
abstract: 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)-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.
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Heather J
authors: HJ
authors: Kulik
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Sergio E
authors: SE
authors: Wong
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Sarah E
authors: SE
authors: Baker
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Carlos A
authors: CA
authors: Valdez
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Joe H
authors: JH
authors: Satcher
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Roger D
authors: RD
authors: Aines
authors: Bioscience and Biotechnology Division, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA.
authors: Felice C
authors: FC
authors: Lightstone
mesh_terms: D002244:Carbon / Q000737:chemistry*; D002384:Catalysis; D018360:Crystallography, X-Ray; D008024:Ligands; D008958:Models, Molecular; D015394:Molecular Structure; D009942:Organometallic Compounds / Q000737:chemistry*; D011789:Quantum Theory; D015032:Zinc / Q000737:chemistry*
chemical_list: D008024:Ligands; D009942:Organometallic Compounds; D002244:Carbon; D015032:Zinc
keywords: CO2 capture; carbonic anhydrase mimics; catalyst design; computational materials discovery; density functional theory; potential energy surfaces; reaction coordinates; zinc