Precious Metal-Free Nickel Nitride Catalyst for the Oxygen Reduction Reaction

Melissa E. Kreider, Alessandro Gallo, Seoin Back, Yunzhi Liu, Samira Siahrostami, Dennis Nordlund, Robert Sinclair, Jens K. Nørskov, Laurie A. King, Thomas F. Jaramillo
Year of publication: 
ACS Applied Materials Interfaces

With promising activity and stability for the oxygen reduction reaction (ORR), transition metal nitrides are an interesting class of non-platinum group catalysts for polymer electrolyte membrane fuel cells. Here, we report an active thin-film nickel nitride catalyst synthesized through a reactive sputtering method. In rotating disk electrode testing in a 0.1 M HClO4 electrolyte, the crystalline nickel nitride film achieved high activity and selectivity to four-electron ORR. It also exhibited good stability during 10 and 40 h chronoamperometry measurements in acid and alkaline electrolyte, respectively. A combined experiment-theory approach, with detailed ex situ materials characterization and density functional theory calculations, provides insight into the structure of the catalyst and its surface during catalysis. Design strategies for activity and stability improvement through alloying and nanostructuring are discussed.

Acknowlegment: The authors gratefully acknowledge the support of the Toyota Research Institute. The US Department of Energy (DoE) Office of Basic Energy Sciences (BES) is gratefully acknowledged for primary support for SUNCAT Center for Interface Science and Catalysis. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF) and the Stanford Nanofabrication Facility (SNF), supported by the National Science Foundation under Award ECCS-1542152. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under contract no. DE-AC02-76SF00515. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under contract no. DE-AC02-05CH11231. A.G. would like to thank J. Vinson at NIST for his support with the OCEAN code. S.S. also acknowledges University of Calgary’s Canada First Research Excellence Fund Program, the Global Research Initiative in Sustainable Low Carbon Unconventional Resources.

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