Molybdenum nitrides as oxygen reduction reaction catalysts: Structural and electrochemical studies

Cao, Bingfei; Neuefeind, Joerg C.; Adzic, Radoslav R.; Khalifah, Peter G.

doi:10.1021/ic5024778

Title: Molybdenum nitrides as oxygen reduction reaction catalysts: Structural and electrochemical studies

Journal Article · Mon Feb 09 00:00:00 EST 2015 · Inorganic Chemistry

DOI:https://doi.org/10.1021/ic5024778· OSTI ID:1330514

Cao, Bingfei ^[1]; Neuefeind, Joerg C. ^[2]; Adzic, Radoslav R. ^[3]; Khalifah, Peter G. ^[1]

Stony Brook Univ., Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Monometallic (δ-MoN, Mo₅N₆, and Mo₂N) and bimetallic molybdenum nitrides (Co_0.6Mo_1.4N₂) were investigated as electrocatalysts for the oxygen reduction reaction (ORR), which is a key half-reaction in hydrogen fuel cells. Monometallic hexagonal molybdenum nitrides are found to exhibit improved activities over rock salt type molybdenum nitride (γ-Mo₂N), suggesting that improvements are due to either the higher molybdenum valence or a more favorable coordination environment in the hexagonal structures. Further enhancements in activity were found for hexagonal bimetallic cobalt molybdenum nitride (Co_0.6Mo_1.4N₂), resulting in a modest onset potential of 0.713 V versus reversible hydrogen electrode (RHE). Co_0.6Mo_1.4N₂ exhibits good stability in acidic environments, and in the potential range lower than 0.5 V versus RHE, the ORR appears to proceed via a four-electron mechanism based on the analysis of rotating disc electrode results. A redetermination of the structures of the binary molybdenum nitrides was carried out using neutron diffraction data, which is far more sensitive to nitrogen site positions than X-ray diffraction data. In conclusion, the revised monometallic hexagonal nitride structures all share many common features with the Co_0.6Mo_1.4N₂ structure, which has alternating layers of cations in octahedral and trigonal prismatic coordination, and are thus not limited to only trigonal prismatic Mo environments (as was originally postulated for δ-MoN).

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1330514

Journal Information:: Inorganic Chemistry, Vol. 54, Issue 5; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 79 works

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