Ismail, Idil, Stuttaford-Fowler, Holly, Ochan-Ashok, Curtis, Robertson, Christopher and Habershon, Scott (2019) Data for Automatic proposal of multi-step reaction mechanisms using a graph-driven search. [Dataset]

	Archive (ZIP) ch-200319-wrap-change--data.zip - Accepted Version Available under License Creative Commons Attribution 4.0. Download (8Kb)
	Plain Text README.txt - Accepted Version Available under License Creative Commons Attribution 4.0. Download (349b)

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Abstract

Proposing and testing mechanistic hypotheses stands as one of the key applications of contemporary computational chemistry. In the majority of computational mechanistic analyses, the individual elementary steps leading from reactants to products are proposed by the user, based on learnt chemical knowledge, intuition, or comparison to an existing well-characterized mechanism for a closely-related chemical reaction. However, the pre-requisite of prior chemical knowledge is a barrier to automated (or `black box') mechanistic generation and assessment, and may simultaneously preclude mechanistic proposals which lie outside the `standard' chemical reaction set. In this Article, we propose a simple random-walk algorithm that searches for the set of elementary chemical reactions which transform defined reactant structures into target products. Our approach operates exclusively in the space of molecular connectivity matrices, seeking out the set of chemically-sensible bonding changes which link connectivity matrices for input reactant and product structures. We subsequently illustrate how atomic coordinates for each elementary reaction can be generated under the action of a bond-enforcing potential, prior to further analysis by ab initio quantum chemistry. Our approach is successfully demonstrated for CO oxidation, the water-gas shift reaction, and n-hexane aromatization, all catalyzed by Pt nanoparticles.

Item Type:	Dataset
Subjects:	Q Science > QD Chemistry
Divisions:	Faculty of Science > Chemistry Faculty of Science > Centre for Scientific Computing
Type of Data:	Experimental data. Text files.
Publisher:	Department of Chemistry, University of Warwick
Official Date:	4 April 2019
Dates:	Date Event 31 January 2019 Submitted 4 April 2019 Published
Date of first compliant deposit:	25 March 2019
Publication Status:	Published
Access rights to Published version:	Restricted or Subscription Access
Copyright Holders:	University of Warwick
Description:	This zip file contains the energy data information for Figures 3, 4 and 5 for the manuscript: Automatic Proposal of Multi-Step Reaction Mechanisms Using a Graph-Driven Search, by Idil Ismail, Holly Stuttaford-Fowler, Curtis Ochan-Ashok, Christopher Robertson, and Scott Habershon. Submitted to Journal of Physical Chemistry, January 2019.
Funder:	Engineering and Physical Sciences Research Council (EPSRC)
Grant number:	EP/R020477/1
RIOXX Funder/Project Grant:	Project/Grant ID RIOXX Funder Name Funder ID EP/R020477/1 [EPSRC] Engineering and Physical Sciences Research Council http://dx.doi.org/10.13039/501100000266

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