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Chemical and Electrocatalytic Ammonia Oxidation by Ferrocene

preprint
submitted on 25.08.2019, 00:00 and posted on 27.08.2019, 15:44 by Mahdi Raghibi Boroujeni, Christine Greene, Jeffery A. Bertke, Timothy H. Warren
Recognizing the potential of ammonia to serve as a carbon-free fuel, we describe an electrocatalytic system for the oxidation of ammonia based on ferrocene (Cp2Fe), an inexpensive, robust catalyst utilizing Earth-abundant iron. Ferrocenium (Cp2Fe+), the 1-electron oxidized form of ferrocene, cleanly oxidizes ammonia to generate nitrogen gas (N2) and protons captured by excess ammonia as NH4+ with electrons reducing ferrocenium to ferrocene. This process occurs under electrocatalytic conditions to generate N2 with sustained current. Simple modification of ferrocene through sulfonation allows for solubility in liquid ammonia to enable electrocatalysis in highly concentrated, energy dense solutions of ammonia. Kinetic and computational analysis provides mechanistic insight into the oxidation of ammonia by ferrocenium.

Funding

US Department of Energy, Basic Energy Sciences (DE-SC001779)

History

Email Address of Submitting Author

thw@georgetown.edu

Institution

Georgetown University

Country

USA

ORCID For Submitting Author

0000-0001-9217-8890

Declaration of Conflict of Interest

No conflicts of interest declared.

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