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Computational Materials Exploration for Capturing Carbon from the Atmosphere

Boone, Paul (2022) Computational Materials Exploration for Capturing Carbon from the Atmosphere. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Over 1 trillion tons of CO2 have been emitted into the atmosphere since we passed the concentration threshold for what is widely considered to be livable: 350 ppm CO2. While numerous negative emissions technologies have been proposed addressing this, in this dissertation I will be focusing solely on extracting CO2 from the atmosphere, or direct air capture (DAC). In contrast to capturing carbon from a point source, such as the exhaust stream of a fossil fuel power plant, research on DAC technologies has been much less explored and it is unknown what materials and process conditions will be optimal at the scale required. Porous materials, such as MOFs, are potential candidate materials for DAC, but because of the high number of porous materials and possible processes, it is impossible to test all combinations experimentally. To the best of my knowledge, there have been no significant computational screenings of materials or processes specific to DAC and I think that large efficiency gains can be made by comprehensively simulating various material classes under various proposed process conditions. The total number of material / process combinations is still daunting in size so I will also be focusing on how we can screen materials and processes faster and more accurately.
This work presents three methodology papers that facilitate and accelerate the evaluation of materials for DAC and one applied materials screening. In aggregate, this work includes (1) a correction to the instantaneous heat flux measurement as calculated by LAMMPS, (2) a strategy to automate the exploration of structure-property relationships for new physisorption applications, (3) a new Python package that implements a molecular find and replace operation on periodic structures, and (4) a computational screening of two MOFs, each with 30 functional group variations, for their ability to be part of a core-shell MOF in a defined DAC process. This work can be built on in the future to address more materials and processes, and, hopefully, will assist the greater academic community in finding better materials and processes for DAC so that it can be feasibly deployed at the necessary scale.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Boone, Paulnarcissus.pong@gmail.compab1350000-0001-8122-0926
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairWilmer, Christopher
Committee MemberMcKone,
Committee MemberMpourmpakis,
Committee MemberSteckel,
Date: 24 June 2022
Defense Date: 6 July 2022
Approval Date: 6 September 2022
Submission Date: 21 July 2022
Access Restriction: No restriction; Release the ETD for access worldwide immediately.
Number of Pages: 163
Institution: University of Pittsburgh
Schools and Programs: Swanson School of Engineering > Chemical and Petroleum Engineering
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: CO2, DAC, carbon capture, porous materials
Date Deposited: 06 Sep 2022 16:26
Last Modified: 06 Sep 2022 16:26


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