Abstract
Replacing scarce and expensive platinum (Pt) with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) has largely been impeded by the low activity of M-N-C. Herein, we implemented chemical vapor deposition (CVD) to synthesize Fe-N-C. The iron was deposited to N-C substrate at 750 ℃, has a record Fe-N4 site density of 2×1020 sites·gram-1. A combination of characterizations shows that the Fe-N4 sites formed via CVD are located exclusively on the outer-surface, with 100% site utilization. This catalyst delivers an unprecedented current density of 33 mA·cm-2 at 0.90 V i R-free (iR-corrected) in an H2-O2 PEMFC at 1.0 bar and 80 ℃. Acknowledgements This work was supported by the US Department of Energy under award number DE-EE0008416 and DE-EE0008075. The authors acknowledge the support from the U.S. Department of Energy, Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office (DOE-EERE-HFTO) through the Electrocatalysis consortium (ElectroCat) and the DOE program and technology managers, Dimitrios Papageorgopoulos, David Peterson, and Nancy Garland. The ex situ XAS experiments at the Zn K-edge were performed at the Advanced Photon Source (APS), a DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The operation of MRCAT at the APS is supported by the Department of Energy and the MRCAT member institutions. The rest of the XAS data were collected at the beamlines 6-BM, 7-BM and 8-ID (ISS) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. AC-STEM was conducted at the Center for Nanophase Materials Sciences located at Oak Ridge National Laboratory, which is a DOE Office of Science User Facility.
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