期刊
SMALL
卷 16, 期 6, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201906057
关键词
catalytic sites; Fe-N-C catalysts; hierarchically carbon skeletons; oxygen reduction; evolution reactions; X-ray absorption fine structure (XAFS)
类别
资金
- National Key R&D Program of China [2016YFB010030X, 2016YFB0700600]
- National Natural Science Foundation of China [51772117, 51732005, 11905081]
- Center for Computational Science and Engineering of Southern University of Science and Technology
Highly active and durable bifunctional oxygen electrocatalysts are of pivotal importance for clean and renewable energy conversion devices, but the lack of earth-abundant electrocatalysts to improve the intrinsic sluggish kinetic process of oxygen reduction/evolution reactions (ORR/OER) is still a challenge. Fe-N-C catalysts with abundant natural merits are considered as promising alternatives to noble-based catalysts, yet further improvements are urgently needed because of their poor stability and unclear catalytic mechanism. Here, an atomic-level Fe-N-C electrocatalyst coupled with low crystalline Fe3C-Fe nanocomposite in 3D carbon matrix (Fe-SAs/Fe3C-Fe@NC) is fabricated by a facile and scalable method. Versus atomically FeNx species and crystallized Fe3C-Fe nanoparticles, Fe-SAs/Fe3C-Fe@NC catalyst, abundant in vertical branched carbon nanotubes decorated on intertwined carbon nanofibers, exhibits high electrocatalytic activities and excellent stabilities both in ORR (E-1/2, 0.927 V) and OER (E-J=10, 1.57 V). This performance benefits from the strong synergistic effects of multicomponents and the unique structural advantages. In-depth X-ray absorption fine structure analysis and density functional theory calculation further demonstrate that more extra charges derived from modified Fe clusters decisively promote the ORR/OER performance for atomically FeN4 configurations by enhanced oxygen adsorption energy. These insightful findings inspire new perspectives for the rational design and synthesis of economical-practical bifunctional oxygen electrocatalysts.
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