Several concepts for platinum-based catalysts for the oxygen reduction reaction (ORR) are presented that exceed the US Department of Energy targets for Pt-related ORR mass activity. Most concepts achieve their high ORR activity by increasing the Pt specific activity at the expense of a lower electrochemically active surface area (ECSA). In the potential region controlled by kinetics, such a lower ECSA is counterbalanced by the high specific activity. At higher overpotentials, however, which are often applied in real systems, a low ECSA leads to limitations in the reaction rate not by kinetics, but by mass transport. Here we report on self-supported platinum–cobalt oxide networks that combine a high specific activity with a high ECSA. The high ECSA is achieved by a platinum–cobalt oxide bone nanostructure that exhibits unprecedentedly high mass activity for self-supported ORR catalysts. This concept promises a stable fuel-cell operation at high temperature, high current density and low humidification.
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The X-ray total scattering analysis and modelling were done in PDFgetX3 and PDFgui. The fitting parameters can be found in the Supplementary Information. The XAS data were analysed by using the IFEFFIT software. DFT calculations were performed with Gpaw and ASE, which are open source codes. The structure and script can be found on the website of the Department of Chemistry, University of Copenhagen.
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This work was supported by the Danish DFF through grant no. 4184-00332, the Villum Center for the Science of Sustainable Fuels and Chemicals (grant no. 9455) and the Danish National Research Foundation Center for High-Entropy Alloys Catalysis (CHEAC). M.A. acknowledges funding from the Swiss National Science Foundation (SNSF) via project no. 200021_184742. G.W.S. and V.B. acknowledge support from BMBF for funding the validation (VIP+) project 3DnanoMe (FKZ 03VP06451). The authors acknowledge the collaboration with L. T. Kuhn and S. B. Simonsen concerning TEM measurements, A. Mingers for ICP-MS measurements, G. Cibin, S. Belin and M. Nachtegal for technical support at the Quick EXAFS beam line, B18, Diamond Light Source (DLS), the ROCK beam line (proposal ID 20180795) of Synchrotron SOLEIL and the Super XAS beamline, X10DA, of the Swiss light source (SLS) of the Paul Scherrer Institute, respectively. The work at the ROCK beamline was supported by a public grant overseen by the French National Research Agency (ANR) as part of the ‘Investissements d’Avenir’ programme (reference ANR10-EQPX45). A.D. and M.O. received funding from the DFG (FOR2213, TP9) and the Federal Ministry of Education and Research (BMBF, ECatPEMFC, FKZ 03SF0539). K.M.Ø.J. and M.J. are grateful to the Villum Foundation for financial support through a Villum Young Investigator grant (VKR00015416). We furthermore thank DANSCATT (supported by the Danish Agency for Science and Higher Education) for support. This research used resources at the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract no. DE-AC02-06CH11357.
The authors declare no competing interests.
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Sievers, G.W., Jensen, A.W., Quinson, J. et al. Self-supported Pt–CoO networks combining high specific activity with high surface area for oxygen reduction. Nat. Mater. 20, 208–213 (2021). https://doi.org/10.1038/s41563-020-0775-8