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Date Permissions Signed

6-2020

Date of Award

Spring 2020

Document Type

Masters Thesis

Department or Program Affiliation

Chemistry

Degree Name

Master of Science (MS)

Department

Chemistry

First Advisor

Gilbertson, John D.

Second Advisor

Scheuermann, Margaret Louise

Third Advisor

Rider, David A. (Materials scientist)

Abstract

Carbon dioxide (CO2) and bioavailable nitrogen in the form of nitrates (NO3-) and nitrites (NO2-) are serious environmental pollutants. However, without economic incentives there is little interest in remediation of these pollutants outside of laboratory scale experiments. CO2 can be converted to carbon monoxide (CO), a valuable building block in Fischer-Tropsch sourced fuel, and NO3- and NO2- can be converted to ammonia, another important chemical building block. However, both require effective, low-cost catalysts to be financially viable options. This thesis seeks to demonstrate the conversion of CO2 to CO as well as NO3- and NO2- reduction. To accomplish this a cobalt centered redox active pyridine diimine ligand scaffold with an appended hemilabile, proton responsive pyridine ring (PyrrPDI) was synthesized. The PyrrPDI scaffold is capable of storing multiple electron equivalents, making it ideal for small molecule activation where several electrons are often required. Reduction of the complex was carried out through chemical and electrochemical means. Once reduced this complex shows activity toward both CO2 and NO2-, releasing CO and/or NO gas. When acid is introduced the complex showed electrocatalytic activity toward NO2-, with small amounts of ammonia being produced though the primary product of that reaction is currently unknown. An unexpected reaction between Samarium diiodide (SmI2) being used as a chemical reductant and nitrite lead to examination of SmI2 as a means to convert various nitrogen oxides to N2.

Type

Text

Keywords

Cobalt, Nitrosyl, Nitrite

Publisher

Western Washington University

OCLC Number

1156320701

Subject – LCSH

Ligands (Biochemistry); Nitrates; Nitrites; Carbon dioxide; Samarium--Reactivity; Cobalt--Reactivity

Format

application/pdf

Genre/Form

masters theses

Language

English

Rights

Copying of this document in whole or in part is allowable only for scholarly purposes. It is understood, however, that any copying or publication of this document for commercial purposes, or for financial gain, shall not be allowed without the author’s written permission.

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