Journal
ACS NANO
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c06459
Keywords
Fe-N-C; single-atom catalysts; heteroatoms; fuel cells; oxygen reduction
Categories
Funding
- Advanced Photon Source
- U.S. Department of Energy (DOE) , Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- National Science Foundation Graduate Research Fellowship [DGE1255832]
- Center for Institutional Research Computing at Washington State University
- U.S. DOE, Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office
- Franceschi Microscopy & Imaging Center of Washington State University
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Fe-N-C single-atomic metal site catalysts (SACs) have attracted great interest as substitutes for Pt-based catalysts in the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. Efforts have been made to modulate the electronic structure of metal single-atomic sites to enhance the catalytic activities. This study uses chlorine to adjust the active center via a near-range coordinated interaction, improving the intrinsic ORR activity.
Fe-N-C single-atomic metal site catalysts (SACs) have garnered tremendous interest in the oxygen reduction reaction (ORR) to substitute Pt-based catalysts in proton exchange membrane fuel cells. Nowadays, efforts have been devoted to modulating the electronic structure of metal single-atomic sites for enhancing the catalytic activities of Fe- N-C SACs, like doping heteroatoms to modulate the electronic structure of the Fe-N-x active center. However, most strategies use uncontrolled long-range interactions with heteroatoms on the Fe-N-x substrate, and thus the effect may not precisely control near-range coordinated interactions. Herein, the chlorine (Cl) is used to adjust the Fe-N-x active center via a near-range coordinated interaction. The synthesized FeN4Cl SAC likely contains the FeN4Cl active sites in the carbon matrix. The additional Fe-Cl coordination improves the instrinsic ORR activity compared with normal FeNx SAC, evidenced by density functional theory calculations, the measured ORR half-wave potential (E-1/2, 0.818 V), and excellent membrane electrode assembly performance.
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