Document Type
Thesis
Degree Name
Master of Science (MSc)
Department
Chemistry
Faculty/School
Faculty of Science
First Advisor
Dr. Hind Al-Abadleh
Advisor Role
Supervisor
Second Advisor
Dr. Vladimir Kitaev
Advisor Role
Supervising committee member
Third Advisor
Dr. Yaser Abu-Lebdeh
Advisor Role
Supervising committee member
Abstract
Global climate change is a major challenge facing the world in the 21st century. This environmental crisis originated from excess amounts of atmospheric carbon dioxide (CO2) released from burning fossil fuels. One promising remediation method to decrease atmospheric CO2 levels is called carbon dioxide electrochemical reduction (CO2ER). In CO2ER, the CO2 gas undergoes chemical reduction to other hydrocarbon fuels. For CO2ER to take place, an energy source and a catalyst are needed. In this thesis, three aspects of CO2ER were investigated using attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy coupled with other surface sensitive characterization tools. First, we studied the surface chemistry of copper oxide (CuO) nanoparticles with major CO2ER intermediates, formate (HCOO-), bicarbonate (HCO3-), and acetate (CH3COO-). We quantified the adsorption and desorption mechanisms of each intermediate in-situ and in real time under CO2ER experimental conditions (Langmuir, 2022, 38(48), 14789). The second aspect of this thesis was examining the photochemical reactivity of CuO nanoparticles mixed with Ag nanoparticles in converting surface species of CO2ER intermediates to products. The last part of this thesis involved the use of a novel spectroelectrochemical (SEC) cell to directly monitor surface species during electrochemical experiments on Cu-coated electrodes. Major results from this thesis are (1) CO2ER intermediates form mostly outer-sphere complexes with CuO nanoparticles highlighting the importance of hydrogen bonding to the CO2ER mechanism, (2) No positive effect of plasmonic properties were observed by the addition of commercial polydispersed Ag nanoparticles to CuO, and (3) the use of the SEC is highly promising to bridge the gap between IR spectroscopy and electrochemistry and gain mechanistic insights into surface processes.
Recommended Citation
Hsu, Jason, "Mechanistic Studies of CO2 Electrochemical Reduction (CO2ER) on Cu and CuO Nanoparticles with In-Situ ATR-FTIR Spectroscopy" (2023). Theses and Dissertations (Comprehensive). 2549.
https://scholars.wlu.ca/etd/2549
Convocation Year
2023
Convocation Season
Spring
Included in
Environmental Chemistry Commons, Materials Chemistry Commons, Physical Chemistry Commons