Date of Award

Spring 4-30-2025

Document Type

Honors Project

Degree Name

Bachelor of Science

Department

Chemistry

Department Chair or Program Director

Dr. K. Nicole Crowder

First Advisor

Dr. K. Nicole Crowder

Second Advisor

Dr. Kelli M. Slunt

Third Advisor

Dr. E. Davis Oldham

Fourth Advisor

Dr. Sarah E. Smith

Major or Concentration

Biochemistry

Abstract

The electrochemical reduction of carbon dioxide (CO2) offers a promising strategy for reducing excess atmospheric CO2 by converting it into valuable chemical products. This process can be catalyzed by transition metal complexes, particularly those with extended aromatic ligands such as terpyridines which coordinate with metals in a tridentate fashion. When tethered to an electrode, the terpyridine-metal catalyst complex allows for stable binding and reusability without the need for chemical separation to recover the catalyst. Self-assembled monolayers (SAMs) of (3-bromopropyl) phosphonic acid were formed on copper surfaces, enabling attachment of terpyridine ligands through a click reaction between a substituted azide and a terminal alkyne on the terpyridine. Surface assembly was optimized by varying solvents and concentrations of (3-bromopropyl) phosphonic acid, with optimal coverage observed with 1.0 mM (3-bromopropyl) phosphonic acid in acetone. Click reaction conditions were modified to form strong and irreversible triazole linkages between the SAM and the functional ligand, and the terpyridine-metal complexes were synthesized in solution. Click products and ligand synthesis in solution were characterized using 1H NMR and IR spectroscopy, and surface bound products were characterized through fixed angle specular reflectance IR. This stepwise synthesis of a stable, surface-bound catalytic system offers an approach towards efficient and reusable electrochemical CO2 reduction systems.

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