Heteroatom Coordinated Single-Atom Electrocatalysts on Carbon Substrate for Highly Efficient Oxygen Reduction Reaction

Xie, Yuhan

Heteroatom Coordinated Single-Atom Electrocatalysts on Carbon Substrate for Highly Efficient Oxygen Reduction Reaction

Xie, Yuhan

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Publication Type:: Thesis
Issue Date:: 2023

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Field	Value	Language
dc.contributor.author	Xie, Yuhan
dc.date.accessioned	2024-04-22T02:56:25Z
dc.date.available	2024-04-22T02:56:25Z
dc.date.issued	2023
dc.identifier.uri	http://hdl.handle.net/10453/178163
dc.description	University of Technology Sydney. Faculty of Science.	en_US.UTF-8
dc.description.abstract	The oxygen reduction reaction (ORR) is a critical cathodic reaction in fuel cells and metal-air batteries. The scarcity of platinum and its poor durability impede its Industrialization. Single-atom catalysts (SACs) are promising substitutes for 100% utilization efficiency and competitive performance. However, a challenge regarding the controllable synthesis and characterization hindered structure-property investigations. This thesis investigates a series of iron and zinc SACs electrocatalysts to determine clues for the controllable synthesis and structure-property relationships. The first project presents a facile method for synthesizing SACs by anchoring iron and zinc atoms by five types of sulfur-containing ligands. We found that different sulfur-contained ligands lead to different structures and ORR performances in both alkaline and acidic electrolytes. In the next project, we devised a bi-functional ligand-assisted synthesis approach for the second project to regulate the distance between Fe and Zn single-atom pairs. The aim is to achieve direct O-O bond cleavage. We provided comprehensive evidence that the streamlined dissociative pathway has been successfully accomplished by charge and electron transfer that is evenly distributed, effectively reducing the energy of the O-O σ bond. We elucidated the dynamic characteristics of paired heteroatoms resulting from distance-related influences, offering an understanding of the fundamental mechanisms.	en_US.UTF-8
dc.format	Thesis (PhD)
dc.language.iso	en_US	en_US.UTF-8
dc.relation	https://opus.lib.uts.edu.au/bitstream/10453/178163/1/thesis.pdf
dc.rights	info:eu-repo/semantics/embargoedAccess
dc.rights	The author owns the copyright in this thesis including all reproduction and reuse rights for the work. The work may not be altered without the permission of the copyright owner. Attribution is essential when quoting or paraphrasing from this thesis.
dc.rights	© 2023 Yuhan Xie
dc.rights	au.edu.uts.lib/cph
dc.title	Heteroatom Coordinated Single-Atom Electrocatalysts on Carbon Substrate for Highly Efficient Oxygen Reduction Reaction	en_US.UTF-8
dc.type	Thesis
utslib.copyright.status	embargoed	*
utslib.copyright.embargo	2025-04-20T00:00:00+1000

Abstract:

The oxygen reduction reaction (ORR) is a critical cathodic reaction in fuel cells and metal-air batteries. The scarcity of platinum and its poor durability impede its Industrialization. Single-atom catalysts (SACs) are promising substitutes for 100% utilization efficiency and competitive performance. However, a challenge regarding the controllable synthesis and characterization hindered structure-property investigations. This thesis investigates a series of iron and zinc SACs electrocatalysts to determine clues for the controllable synthesis and structure-property relationships. The first project presents a facile method for synthesizing SACs by anchoring iron and zinc atoms by five types of sulfur-containing ligands. We found that different sulfur-contained ligands lead to different structures and ORR performances in both alkaline and acidic electrolytes. In the next project, we devised a bi-functional ligand-assisted synthesis approach for the second project to regulate the distance between Fe and Zn single-atom pairs. The aim is to achieve direct O-O bond cleavage. We provided comprehensive evidence that the streamlined dissociative pathway has been successfully accomplished by charge and electron transfer that is evenly distributed, effectively reducing the energy of the O-O σ bond. We elucidated the dynamic characteristics of paired heteroatoms resulting from distance-related influences, offering an understanding of the fundamental mechanisms.

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http://hdl.handle.net/10453/178163