Computational Design of Oligopeptides as Carbon Capture Agents

Author

Amarachi G. Sylvanus, University of Tennessee, KnoxvilleFollow

Date of Award

8-2025

Degree Type

Dissertation

Degree Name

Doctor of Philosophy

Major

Chemistry

Major Professor

Konstantinos D. Vogiatzis

Committee Members

Konstantinos D. Vogiatzis, Fred Heberle, Joshua Baccile, David Keffer

Abstract

This work presents a computational framework for understanding and designing bioinspired materials for CO₂ capture. We started by calculating highly accurate reference interaction energies with electronic structure theory for amino acid-CO₂ complexes and benchmarking different density functionals for performing large-scale DFT calculations on oligopeptide-CO₂ molecular systems. Building on this, we explored all possible dipeptides, revealing that cooperative effects significantly enhance CO₂ binding, particularly in sequences containing polar residues. We then developed TriScore, a descriptor-based ranking metric, to screen 8000 tripeptides for CO₂ interaction. DFT and SAPT0 analyses confirmed that the top-ranking tripeptides exhibit stronger, electrostatically driven non-covalent interactions. Finally, we extended our investigation to amino acids in solution to evaluate their potential in solvent-based direct air capture systems. This progression from single amino acids to solution-phase systems offers a scalable strategy for designing oligopeptide-based CO₂ sorbents.

Recommended Citation

Sylvanus, Amarachi G., "Computational Design of Oligopeptides as Carbon Capture Agents. " PhD diss., University of Tennessee, 2025.
https://trace.tennessee.edu/utk_graddiss/12776