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Rational Design of CO(2) Electroreduction Catalysts and Their Chemical Micro-Environments in Gas Diffusion Electrode Systems.

Record Type:	Language materials, manuscript : Monograph/item
Title/Author:	Rational Design of CO(2) Electroreduction Catalysts and Their Chemical Micro-Environments in Gas Diffusion Electrode Systems./
Author:	Wicks, Joshua.
Description:	1 online resource (163 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
Contained By:	Dissertations Abstracts International85-01B.
Subject:	Electrical engineering. -
Online resource:	click for full text (PQDT)
ISBN:	9798379766177

Rational Design of CO(2) Electroreduction Catalysts and Their Chemical Micro-Environments in Gas Diffusion Electrode Systems.
Wicks, Joshua.

Rational Design of CO(2) Electroreduction Catalysts and Their Chemical Micro-Environments in Gas Diffusion Electrode Systems. - 1 online resource (163 pages)

Source: Dissertations Abstracts International, Volume: 85-01, Section: B.

Thesis (Ph.D.)--University of Toronto (Canada), 2023.

Includes bibliographical references

A growing abundance of renewable low-carbon electricity coupled with CO2 capture and utilization are two critical components of global net-zero emissions plans. The electrochemical conversion of CO2 and CO into value-added chemicals and fuels is a promising strategy to electrify hard-to-decarbonize sectors of industry. Electrolyzers employing gas diffusion electrodes (GDEs) offer a means to elevate operational reaction rates to scalable regimes. In this thesis, I use experiment and atomistic simulations to investigate CO2 electroreduction property-performance relationships at multiple length-scales along the cross-section of a gas diffusion electrode.I begin with describing the need for industrial decarbonization, the role of CO(2) electroreduction in hard-to-decarbonize chemicals manufacturing and renewable fuels production, and fundamental background information of the reaction from theoretical and experimental perspectives. I then conduct an experimental investigation into the effect of gas diffusion layer properties on electrochemical performance, finding a 100x increase in C2H4 :CO ratio by tuning surface morphology to extend the residence time of locally-produced CO in the catalyst layer. I also experimentally explore cat-alyst:ionomer intefaces in the catalyst layer of the GDE, leading to a record ethylene partial current density of 1.3 A cm−2 . I concluded from both experimental studies that *CO coverage on the catalyst surface, as a result of CO2 and CO concentrations in the local chemical environment of catalyst sites, was an important variable influencing selective chemical production. I applied this insight - through two studies involving computational atomistic simulations - to guide catalyst material design. I studied how low *CO coverage reaction environments favor methane selectivity on CuAu catalyst materials, leading to an experimental selectivity of 56 % at a production rate of 112 mA cm−2 . Conversely, I found that high *CO coverage regimes favor pathways to acetate production in the electrochemical CO reduction reaction, leading to an experimental selectivity of 91% at a production rate of 113 mA cm−2 . I conclude with a reflection on future priorities to advance the technological readiness of CO2 electrolyzers.Broadly, the studies herein enable scientists and engineers to better understand the interplay between reaction chemistry and reactor design in gas diffusion electrode systems for CO2 and CO electroreduction.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2024

Mode of access: World Wide Web

ISBN: 9798379766177Subjects--Topical Terms:

596380
Electrical engineering.
Subjects--Index Terms:

ElectrocatalysisIndex Terms--Genre/Form:

554714
Electronic books.

Rational Design of CO(2) Electroreduction Catalysts and Their Chemical Micro-Environments in Gas Diffusion Electrode Systems.
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