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Graphite Intercalation Compounds Derived by Green Chemistry as Oxygen Reduction Reaction Catalysts
journal contribution
posted on 2020-09-09, 16:38 authored by Jianchao Zhao, Joseph H. Dumont, Ulises Martinez, Javier Macossay, Kateryna Artyushkova, Plamen Atanassov, Gautam GuptaPrecious group metal
(PGM) catalysts such as Pt supported on carbon
supports are expensive catalysts utilized for the oxygen reduction
reaction (ORR) due to their unmatched catalytic activity and durability.
As an alternative, PGM-free ORR electrocatalysts that offer respectable
catalytic activity are being pursued. Most of the notable PGM-free
catalysts are obtained either from a bottom-up approach synthesis
utilizing nitrogen-rich polymers as building blocks, or from a top
down approach, where nitrogen and metal moieties are incorporated
to carbonaceous matrixes. The systematic understanding of the origin
of catalytic activity for either case is speculative and currently
employed synthesis techniques typically generate large amounts of
hazardous waste such as acids, oxidizing agents, and solvents. Herein,
for the first time, we investigate the catalytic activity of graphite-based
materials obtained via intercalation strategies that minimally perturb
the graphitic backbone. Our outlined approaches demonstrate initial
efforts to not only elucidate the role of each element but also significantly
reduce the use of hazardous chemicals, which remains a pressing challenge.
Graphite intercalation compounds (GIC) were obtained using fewer steps
and solvent-free processes. X-ray diffraction and Raman results confirm
the successful intercalation of FeCl3 between graphite
layers. Electrochemical data shows that the ORR performance of FeCl3-intercalated GIC displays slight improvement where the onset
potential reaches 0.77 V vs RHE in alkaline environments. However,
expansion of the graphite and solvent-free incorporation of iron and
nitrogen moieties resulted in a significant increase in ORR activity
with onset potential to 0.89 V vs RHE, a maximum half-wave of 0.72
V vs RHE, and a limiting current of about 2.5 mA cm–2. We anticipate that the use of near solvent-free processes that
result in a high yield of catalysts along with the fundamental insight
into the origin of electrochemical activity will tremendously impact
the methodologies for developing next-generation ORR catalysts.
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Keywords
Graphite Intercalation Compounds De...solvent-free processesGraphite intercalation compounds0.77 V vs RHEOxygen Reduction Reaction Catalysts...0.72 V vs RHEbottom-up approach synthesisoxygen reduction reactionnext-generation ORR catalystsFeCl 30.89 V vs RHEintercalated GIC displaysPGM-free ORR electrocatalysts
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