Nitrogen-Doped Graphene Oxide Electrocatalysts for the Oxygen Reduction Reaction

Dumont, Joseph H.; Martinez, Ulises; Artyushkova, Kateryna; Purdy, Geraldine M.; Dattelbaum, Andrew M.; Zelenay, Piotr; Mohite, Aditya; Atanassov, Plamen; Gupta, Gautam

doi:10.1021/acsanm.8b02235

Nitrogen-Doped Graphene Oxide Electrocatalysts for the Oxygen Reduction Reaction

Journal Article · Thu Jan 31 23:00:00 EST 2019 · ACS Applied Nano Materials

DOI:https://doi.org/10.1021/acsanm.8b02235· OSTI ID:1495149

^[1]; ^[2]; ^[3]; Purdy, Geraldine M. ^[2]; Dattelbaum, Andrew M. ^[2]; ^[2]; ^[2]; ^[3]; Gupta, Gautam ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of New Mexico, Albuquerque, NM (United States)

Platinum group metal-free (PGM-free) electrocatalysts for the oxygen reduction reaction (ORR) often exhibit a complex functionalized graphitic structure. Because of this complex structure, limited understanding exists about the design factors for the synthesis of high-performing materials. Graphene, a two-dimensional hexagonal structure of carbon, is amenable to structural and functional group modifications, making it an ideal analogue to study crucial properties of more complex graphitic materials utilized as electrocatalysts. In this paper, we report the synthesis of active nitrogen-doped graphene oxide catalysts for the ORR in which their activity and four-electron selectivity are enhanced using simple solvent and electrochemical treatments. The solvents, chosen based on Hansen’s solubility parameters, drive a substantial change in the morphology of the functionalized graphene materials by (i) forming microporous holes in the graphitic sheets that lead to edge defects and (ii) inducing 3D structure in the graphitic sheets that promotes ORR. Additionally, the cycling of these catalysts has highlighted the multiplicity of the active sites, with different durability, leading to a highly selective catalyst over time, with a minimal loss in performance. High ORR activity was demonstrated in an alkaline electrolyte with an onset potential of ~1.1 V and half-wave potential of 0.84 V vs RHE. Furthermore, long-term stability potential cycling showed minimal loss in half-wave potential (<3%) in both N₂- and O₂-saturated solutions with improved selectivity toward the four-electron reduction after 10000 cycles. Lastly, the results described in this work provide additional understanding about graphitic electrocatalysts in alkaline media that may be utilized to further enhance the performance of PGM-free ORR electrocatalysts.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1495149

Report Number(s):: LA-UR--18-20904

Journal Information:: ACS Applied Nano Materials, Journal Name: ACS Applied Nano Materials Journal Issue: 3 Vol. 2; ISSN 2574-0970

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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