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Toward an Inverse Approach for the Design of Small-Molecule Fixating Catalysts

Published online by Cambridge University Press:  14 January 2013

Thomas Weymuth  and
Markus Reiher
Thomas Weymuth
Affiliation:
ETH Zurich, Laboratory for Physical Chemistry, Wolfgang-Pauli-Strasse 10, 8093 Zurich, Switzerland
Markus Reiher*
Affiliation:
ETH Zurich, Laboratory for Physical Chemistry, Wolfgang-Pauli-Strasse 10, 8093 Zurich, Switzerland
*
*email: markus.reiher@phys.chem.ethz.ch
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Abstract

Within an inverse design approach applied to a nitrogen-fixation catalyst we discuss options for calculating “jacket” potentials that fulfill a purpose-oriented target requirement. As a target requirement we choose the vanishing geometric gradients on all atoms of a subsystem consisting of a metal center binding the small molecule to be activated - in our case dinitrogen. The additional potential can be represented within a full quantum model or by a sequence of approximations of which a field of electrostatic point charges is the simplest. In order to analyze the feasibility of this approach, we dissect a known dinitrogen-fixating complex and analyze its ligand environment expressed by the “jacket” potential. It is discussed how this ligand-bypotential replacement can be generalized for future applications that eventually allow us to find a competitive synthetic nitrogen-fixation transition metal complex. It can be expected that such a ligand-by-potential replacement approach will be applicable to any type of host-guest chemical process.

Keywords

chemical reactionelectronic structuresimulation
Type
Articles
Information
MRS Online Proceedings Library (OPL) , Volume 1524: Symposium RR – Advanced Multiscale Materials Simulation—Toward Inverse Materials Computation , 2013 , mrsf12-1524-rr06-01
Copyright
Copyright © Materials Research Society 2013

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