Hierarchically Porous Carbons with Highly Curved Surfaces for Hosting Single Metal FeN4 Sites as Outstanding Oxygen Reduction Catalysts
Year: 2023
Type: article
Abstract: Iron–nitrogen–carbon (FeNC) materials have emerged as a promising alternative to platinum‐group metals for catalyzing the oxygen reduction reaction (ORR) in proton‐exchange‐membrane fuel cells. However, their low intrinsic activity and stability are major impediments. Herein, an FeN–C electrocatalyst with dense FeN4 sites on hierarchically porous carbons with highly curved surfaces (denoted as FeN4‐hcC) is reported. The FeN4‐hcC catalyst displays exceptional ORR activity in acidic media, with a high half‐wave potential of 0.85 V (versus reversible hydrogen electrode) in 0.5 m H2SO4. When integrated into a membrane electrode assembly, the corresponding cathode displays a high maximum peak power density of 0.592 W cm−2 and demonstrates operating durability over 30 000 cycles under harsh H2/air conditions, outperforming previously reported Fe–NC electrocatalysts. These experimental and theoretical studies suggest that the curved carbon support fine‐tunes the local coordination environment, lowers the energies of the Fe d‐band centers, and inhibits the adsorption of oxygenated species, which can enhance the ORR activity and stability. This work provides new insight into the carbon nanostructure–activity correlation for ORR catalysis. It also offers a new approach to designing advanced single‐metal‐site catalysts for energy‐conversion applications.
Source: Advanced Materials
Institutions: Center for Advancing Electronics Dresden, Technische Universität Dresden, Wuhan University of Technology, State Key Laboratory of Silicate Materials for Architecture, Purdue University West Lafayette, Indiana University – Purdue University Indianapolis, Chinese Academy of Sciences, Technical Institute of Physics and Chemistry, Max Planck Institute of Microstructure Physics, Technische Universität Darmstadt, University at Buffalo, State University of New York
Language: English
Field: Energy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $5,250
Awards: G1088600580, G1293550238, G1394529870, G1744937833, SFB 1415: Chemie der synthetischen zweidimensionalen Materialien, G2666324051, G290470551, HYDROGEN AND FUEL CELL R&D FUNDING OPPORTUNITY ANNOUNCEMENT, StRedO - Untersuchungen zum Degradationsverhalten von Eisen-Stickstoff-basierten Katalysatoren (Fe-N-C) für die Sauerstoffreduktion in der Polymer-Elektrolyt-Membran-Brennstoffzelle, G3421442083, G42699959, G434337789, G4344090363, G4540130896, G4616041893, G4672599647, G4745233088, G5003154033, Graphene Flagship Core Project 3, DURABLE MN-BASED PGM-FREE CATALYSTS FOR POLYMER ELECTROLYTE MEMBRANE FUEL CELLS, ADVANCED PGM-FREE CATHODE ENGINEERING FOR HIGH POWER DENSITY AND DURABILITY, SFB 1487: Eisen, neu gedacht!
OpenAlex ID: W4367834279