Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands

Abstract Simulation of conformationally complicated molecules requires multiple levels of theory to obtain accurate thermodynamics, requiring significant researcher time to implement. We automate this workflow using all open-source code (XTBDFT) and apply it toward a practical challenge: diphosphino...

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Autores principales:	Sibo Lin, Jenna C. Fromer, Yagnaseni Ghosh, Brian Hanna, Mohamed Elanany, Wei Xu
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2021
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/3b4cfa2444624778aa878c3f7ad70593
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spelling	oai:doaj.org-article:3b4cfa2444624778aa878c3f7ad705932021-12-02T11:35:52ZComputer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands10.1038/s41598-021-82816-x2045-2322https://doaj.org/article/3b4cfa2444624778aa878c3f7ad705932021-02-01T00:00:00Zhttps://doi.org/10.1038/s41598-021-82816-xhttps://doaj.org/toc/2045-2322Abstract Simulation of conformationally complicated molecules requires multiple levels of theory to obtain accurate thermodynamics, requiring significant researcher time to implement. We automate this workflow using all open-source code (XTBDFT) and apply it toward a practical challenge: diphosphinoamine (PNP) ligands used for ethylene tetramerization catalysis may isomerize (with deleterious effects) to iminobisphosphines (PPNs), and a computational method to evaluate PNP ligand candidates would save significant experimental effort. We use XTBDFT to calculate the thermodynamic stability of a wide range of conformationally complex PNP ligands against isomeriation to PPN (ΔGPPN), and establish a strong correlation between ΔGPPN and catalyst performance. Finally, we apply our method to screen novel PNP candidates, saving significant time by ruling out candidates with non-trivial synthetic routes and poor expected catalytic performance.Sibo LinJenna C. FromerYagnaseni GhoshBrian HannaMohamed ElananyWei XuNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-10 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Sibo Lin Jenna C. Fromer Yagnaseni Ghosh Brian Hanna Mohamed Elanany Wei Xu Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
description	Abstract Simulation of conformationally complicated molecules requires multiple levels of theory to obtain accurate thermodynamics, requiring significant researcher time to implement. We automate this workflow using all open-source code (XTBDFT) and apply it toward a practical challenge: diphosphinoamine (PNP) ligands used for ethylene tetramerization catalysis may isomerize (with deleterious effects) to iminobisphosphines (PPNs), and a computational method to evaluate PNP ligand candidates would save significant experimental effort. We use XTBDFT to calculate the thermodynamic stability of a wide range of conformationally complex PNP ligands against isomeriation to PPN (ΔGPPN), and establish a strong correlation between ΔGPPN and catalyst performance. Finally, we apply our method to screen novel PNP candidates, saving significant time by ruling out candidates with non-trivial synthetic routes and poor expected catalytic performance.
format	article
author	Sibo Lin Jenna C. Fromer Yagnaseni Ghosh Brian Hanna Mohamed Elanany Wei Xu
author_facet	Sibo Lin Jenna C. Fromer Yagnaseni Ghosh Brian Hanna Mohamed Elanany Wei Xu
author_sort	Sibo Lin
title	Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
title_short	Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
title_full	Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
title_fullStr	Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
title_full_unstemmed	Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
title_sort	computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands
publisher	Nature Portfolio
publishDate	2021
url	https://doaj.org/article/3b4cfa2444624778aa878c3f7ad70593
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Computer-assisted catalyst development via automated modelling of conformationally complex molecules: application to diphosphinoamine ligands

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