Lu, Yiyang
(2024)
STUDIES OF ENANTIOSPECIFIC INTERACTION BETWEEN CHIRAL MOLECULES AND MAGNETIZED SURFACES.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
Abstract
The chiral induced spin selectivity (CISS) effect describes the spin-dependent transport of electrons through chiral molecules, in which the preferred spin orientation is determined by the handedness of the molecule and the direction of motion. The CISS effect has attracted considerable research interest due to its important implications across a wide range of scientific fields, including enantiomeric resolution, spin controlled chemical reactions, biorecognition, among others. In this dissertation, fundamental studies on the enantiospecific spin exchange interaction between chiral molecules and magnetized ferromagnetic substrates are investigated and leveraged for enantioseparation, enantiorecognition and enantiospecific polymerization studies. In the first study, the enantiospecific adsorption of cysteine on a ferromagnetic electrode was shown to arise from a kinetically controlled process and not from a thermodynamic stabilization. In the second study, the enantiospecific adsorption of cysteine on a ferromagnetic electrode at different pHs was investigated. Here, the kinetics for enantiospecific adsorption were found to depend strongly on the charge state and geometry of the adsorbate. In the third study, the effects of spin on the enantioselective binding of amino acids with N-acetyl-cysteine coated ferromagnetic electrodes was probed. These studies revealed that the intermolecular interactions between the amino acids and the chiral ferromagnetic surface depend on the electron spin. In the fourth study, Two enantioselective electrochemical reactions that have used polarized electron spins as a chiral reagent are described; enantioselective electroreduction to resolve an enantiomer from a racemic mixture and an oxidative electropolymerization to generate a chiral polymer from achiral monomers. These studies provide a more fundamental understanding of the CISS effect, identify the key contributions necessary for using the CISS effect in enantioseparations, and shed new light on enantiorecognition.
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Details
| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
|
| Date: |
9 January 2024 |
| Date Type: |
Publication |
| Defense Date: |
26 October 2023 |
| Approval Date: |
9 January 2024 |
| Submission Date: |
7 August 2023 |
| Access Restriction: |
No restriction; Release the ETD for access worldwide immediately. |
| Number of Pages: |
195 |
| Institution: |
University of Pittsburgh |
| Schools and Programs: |
Dietrich School of Arts and Sciences > Chemistry |
| Degree: |
PhD - Doctor of Philosophy |
| Thesis Type: |
Doctoral Dissertation |
| Refereed: |
Yes |
| Uncontrolled Keywords: |
CISS, enantiospecific adsorption, biorecognition, spin exchange interaction, EQCM, |
| Date Deposited: |
09 Jan 2024 19:50 |
| Last Modified: |
09 Jan 2024 19:50 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/45284 |
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