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Computational Design and Evaluation of New Materials for Energy and Environmental Applications

Bagusetty, Abhishek (2020) Computational Design and Evaluation of New Materials for Energy and Environmental Applications. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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With a constant demand for efficient energy devices, significant efforts were invested into the development of proton exchange membrane (PEM) fuel cells. Yet, water management and hydration in these PEM fuel cells are a well-known limiting factors for proton transport. The first-principles density functional theory (DFT) study helped to develop two novel 2- D materials that can potentially alleviate the need for aqueous conditions to propagate proton conduction within fuel cells. Anhydrous proton conduction can be achieved when graphane is functionalized with hydroxyl and amine groups as graphamine and graphanol, respectively. Ab-initio molecular dynamics simulations indicated that the proton transport is facile with a relatively low reaction barrier due to the presence of a self-assembling network of hydrogen bonds established over the surface of these materials. Moreover, proton self-diffusivity increases with temperature and thermodynamic stability calculations indicate that these materials are appropriate for intermediate-temperature fuel cells.

Given the environmental concerns of tritiated water (HTO), this work is an attempt to understand the fundamental nature of differential hydrogen bonding offered by the hydrogen isotopes. When two phases (liquid and vapor) of water are in equilibrium, there can be slight difference in the relative abundance of water isotopes for each phase. The treatment of nuclei under classical mechanics is not appropriate for the study of lighter atoms like hydrogen and its isotopes. By employing path-integral-based molecular simulations one can account for quantum motion of the nuclei to determine isotopic fractionation ratios for water isotopologues in phase equilibrium and cocrystallization of water isotopologues with poly- oxacyclobutane. Due to the inherent computationally intensive nature of these calculations, a combination of reduced-cost and accelerated techniques such as high-order splitting and thermostating procedures were used to achieve convergence of quantum mechanical proper- ties.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Bagusetty, Abhishekabb58@pitt.eduabb58
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairJohnson, J. Karlkarlj@pitt.edukarlj
Committee MemberJordan, Kenneth
Committee MemberMpourmpakis,
Committee MemberVelankar,
Date: 29 January 2020
Date Type: Publication
Defense Date: 18 November 2019
Approval Date: 29 January 2020
Submission Date: 15 November 2019
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Number of Pages: 119
Institution: University of Pittsburgh
Schools and Programs: Swanson School of Engineering > Computational Modeling and Simulation
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: anhydrous, proton transport, path integral molecular dynamics, equilibrium isotope fractionation ratio
Date Deposited: 29 Jan 2020 15:58
Last Modified: 29 Jan 2020 15:58


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