Date Approved
5-23-2024
Embargo Period
5-23-2025
Document Type
Dissertation
Degree Name
Doctor of Philosophy (Ph.D.) in Materials Science and Engineering
Department
Physics and Astronomy
College
College of Science & Mathematics
Funder
Sekisui Chemical Co., Ltd
Advisor
Samuel Lofland, Ph.D.
Committee Member 1
Jeffrey Hettinger, Ph.D.
Committee Member 2
Lei Yu, Ph.D.
Committee Member 3
Dongmei Dong, Ph.D.
Keywords
Combinatorial; Electrocatalyst; Noble Metals; Scanning Electrochemical System; Thin Film Materials
Subject(s)
Electrocatalysis; Metal catalysts
Disciplines
Materials Science and Engineering | Physics
Abstract
Electrocatalysts demonstrate significant promise for sustainable processes like carbon capture and generating recycled carbon fuels which are needed to achieve net zero carbon emissions. However, the commercialization of these processes is limited by several factors, one of which is the high cost of catalysts. The discovery and development of cheaper alternatives has been difficult due to constraints in experimental methodologies, scalability limitations, and a lack of understanding of reaction mechanisms. Within this dissertation is the development of a novel scanning electrochemical system and its implementation for high-throughput data generation from combinatorially sputtered material libraries. Combinatorial Pd-Au alloys were investigated for the electrosynthesis of DMC from the oxidation of methanol and CO. With DFT and bilayer experiments it is shown that the alloy formation is a crucial component of catalytic activity modulation for the synthesis of DMC at the Pd-Au interface. Combinatorial material libraries of Pt-Pd-Au-Ir alloys were investigated for OER with the scanning electrochemical system and 0.1 M H2SO4. Machine learning models and differential Tafel plot analysis was implemented to identify relationships between the chemical composition and the overpotential. It is shown that only 30 % Ir is needed to maintain performance, which significantly reduces the cost of the catalyst.
Recommended Citation
Page, Natalie Leong, "COMBINATORIAL STUDIES OF NOBLE METAL CATALYSTS FOR CARBON UTILIZATION" (2024). Theses and Dissertations. 3225.
https://rdw.rowan.edu/etd/3225
