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Computational Benchmarking and Evaluation of Transition Metal Complexes toward Materials Discovery

Wheat, Ryan M (2021) Computational Benchmarking and Evaluation of Transition Metal Complexes toward Materials Discovery. Master's Thesis, University of Pittsburgh. (Unpublished)

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The synergy between computational modeling and materials analysis remains an unsolved problem, yet there is great potential for accelerating materials discovery. This work reframes the cumbersome nature of experimental intuition (trial and error) by shedding light on the utility of quantitative data as a promising alternative. With respect to Metal-Organic Frameworks, stability considerations are essential to the targeting of materials that not only possess high turnover efficiency but are also resistant to degradation. Core computational methods in this work include UFF, GFNFF, GFN2, and B97-3c for their extended utility to evaluating transition metal systems. From a molecular geometry perspective, GFN2 and B97-3c closely matched experimental bond distances for a selected series of 32 transition metal complexes (TMCs) labeled TMC32. In terms of electronic energy, bond dissociation was targeted as a means of predicting synthetic tractability and expected stability. From a separate set of 30 TMCs labeled TM30, B97-3c single-point calculations with UFF optimized geometries provided the highest accuracy. A subset of the tmQM dataset, focused solely on complexes with Ni-Cl bonds, supported the argument that GFN2 is infeasible for calculating electronic effects in its current state. These studies elevate B97-3c as an efficient method that can accelerate efforts to quantify stability in TMCs, with future work focused on correlating this data to improve MOF modeling capabilities towards materials discovery.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Wheat, Ryan Mrmw83@pitt.edurmw83
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairHutchison, Geoffrey
Committee ChairJordan, Kenneth
Committee MemberLiu,
Committee MemberWilmer, Christopher
Date: 3 May 2021
Date Type: Publication
Defense Date: 30 March 2021
Approval Date: 3 May 2021
Submission Date: 7 April 2021
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Number of Pages: 29
Institution: University of Pittsburgh
Schools and Programs: Dietrich School of Arts and Sciences > Chemistry
Degree: MS - Master of Science
Thesis Type: Master's Thesis
Refereed: Yes
Uncontrolled Keywords: MOF, DFT, GFN, Enthalpy, Bond, Metal, Organic
Date Deposited: 03 May 2021 15:37
Last Modified: 03 May 2021 15:37

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  • Computational Benchmarking and Evaluation of Transition Metal Complexes toward Materials Discovery. (deposited 03 May 2021 15:37) [Currently Displayed]


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