Nitride or Oxynitride? Elucidating the Composition–Activity Relationships in Molybdenum Nitride Electrocatalysts for the Oxygen Reduction Reaction

Kreider, Melissa E.; Stevens, Michaela Burke; Liu, Yunhzi; Patel, Anjli M.; Statt, Michael J.; Gibbons, Brenna M.; Gallo, Alessandro; Ben-Naim, Micha; Mehta, Apurva; Davis, Ryan C.; Ievlev, Anton V.; Nørskov, Jens K.; Sinclair, Robert; King, Laurie A.; Jaramillo, Thomas F.

doi:10.1021/acs.chemmater.9b05212

Title: Nitride or Oxynitride? Elucidating the Composition–Activity Relationships in Molybdenum Nitride Electrocatalysts for the Oxygen Reduction Reaction

Journal Article · Wed Mar 25 00:00:00 EDT 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.9b05212· OSTI ID:1633718

^[1];

^[2];

^[1]; Statt, Michael J. ^[1]; Gibbons, Brenna M. ^[1];

^[1]; Ben-Naim, Micha ^[1];

^[3]; Davis, Ryan C. ^[3];

^[4]; Nørskov, Jens K. ^[5]; Sinclair, Robert ^[2];

^[6];

^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
Stanford Univ., CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Technical Univ. of Denmark, Lyngby (Denmark)
Manchester Metropolitan Univ. (United Kingdom)

Molybdenum nitride (Mo–N) catalysts have shown promising activity and stability for the oxygen reduction reaction (ORR) in acid. However, the effect of oxygen (O) incorporation (from synthesis, catalysis, or exposure to air) on their activity remains elusive. Here, we use reactive sputtering to synthesize three compositions of thin-film catalysts and use extensive materials characterization to investigate the depth-dependent structure and incorporated O. We show that the as-deposited Mo–N films are highly oxidized both at the surface (>30% O) and in the bulk (3–21% O) and that the ORR performance is strongly correlated with the bulk structure and composition. Activity for 4e– ORR is highest for compositions with the highest N/O and N/Mo ratio. Furthermore, H₂O₂ production for the films with moderate O content is comparable to or higher than the most H₂O₂-selective nonprecious metal catalysts in acidic electrolyte, on a moles per mass or surface area of catalyst basis. Density functional theory provides insight into the energetics of O incorporation and vacancy formation, and we hypothesize that activity trends with O/N ratios can be traced to the varying crystallite phases and their interactions with ORR adsorbates. This work demonstrates the prevalence and significance of O in metal nitride electrocatalysts and motivates further investigation into the role of O in other nonprecious metal materials.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1633718

Journal Information:: Chemistry of Materials, Vol. 32, Issue 7; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 37 works

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