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Full text release has been delayed at the author's request until May 10, 2026

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Investigating the Nature of Active Sites in Heteroatom-doped Carbon Nanostructure Catalysts for the Oxygen Reduction Reaction

Gustin, Vance A
http://rave.ohiolink.edu/etdc/view?acc_num=osu1618579983890107

Abstract Details

2021, Doctor of Philosophy, Ohio State University, Chemical Engineering.
The oxygen reduction (ORR) and evolution reactions (OER) are of utmost importance to emerging renewable energy technologies. Proton exchange membrane (PEM) fuel cells utilize the ORR to convert hydrogen and oxygen into water and electrical power. These devices have shown promise as the primary power source in vehicular applications. Another emerging technology, unitized regenerative fuel cells, make use of both the ORR and OER to convert excess renewable energy into hydrogen and oxygen through electrolysis, which may be stored indefinitely. When energy demand increases past renewable energy production levels, the hydrogen and oxygen may be converted back into electricity through a fuel cell. One of the challenges facing the development of these technologies is the slow kinetics of the ORR and OER which requires large quantities of precious metal catalysts to achieve functional current densities. The scarcity and high cost of these precious metals, namely platinum and iridium, has resulted in an inspired effort to identify highly active and low cost alternative ORR and OER catalysts. This research work investigates the origin of ORR and OER activity of nitrogen-doped and nitrogen-boron co-doped carbon nanostructures (CNx and CNxBy respectively). The first project demonstrated the use of the bicarbonate ion as a poisoning probe for CNx catalysts and combined density functional theory (DFT) modeling with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) to study the impact of bicarbonate poisoning on the ability of surface nitrogen sites to adsorb oxygen. The second project developed a method for co-doping boron and nitrogen into carbon nanostructures and demonstrated the improved ORR iii activity that resulted from their synergistic interactions. Synthesis methods for CNxBy catalysts were optimized to selectively introduce various boron moieties and then studied using NAP-XPS to elucidate their impact on the adsorption of oxygen on the catalyst surface. Understanding the nature and origin of ORR activity in these heteroatom-doped materials will aid in efforts to rationally design highly active ORR and OER catalysts capable of replacing current state-of-the-art precious metal catalysts.
Umit Ozkan, PhD, PE (Advisor)
Aravind Asthagiri, PhD (Committee Member)
Anne Co, PhD (Committee Member)
105 p.
Chemical Engineering
Oxygen reduction reaction, Proton-exchange membrane fuel cells, near-ambient pressure X-ray photoelectron spectroscopy, electrocatalyst

Recommended Citations

Citations

  • Gustin, V. A. (2021). Investigating the Nature of Active Sites in Heteroatom-doped Carbon Nanostructure Catalysts for the Oxygen Reduction Reaction [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1618579983890107

    APA Style (7th edition)

  • Gustin, Vance. Investigating the Nature of Active Sites in Heteroatom-doped Carbon Nanostructure Catalysts for the Oxygen Reduction Reaction. 2021. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1618579983890107.

    MLA Style (8th edition)

  • Gustin, Vance. "Investigating the Nature of Active Sites in Heteroatom-doped Carbon Nanostructure Catalysts for the Oxygen Reduction Reaction." Doctoral dissertation, Ohio State University, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=osu1618579983890107

    Chicago Manual of Style (17th edition)

osu1618579983890107
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This open access ETD is published by The Ohio State University and OhioLINK.