期刊
ACS NANO
卷 13, 期 10, 页码 11853-11862出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b05913
关键词
Fe nanoclusters; electrocatalysts; oxygen reduction; single-atom catalyst; DFT computation
类别
资金
- National Key R&D Program of China [2017YFE0120500]
- National Natural Science Foundation of China [51502099]
- Fundamental Research Funds for the Central Universities [HUST 2018KFYYXJJ051, 2019KFYXMBZ076]
- UNL Holland Computing Center
- China Scholarship Council (CSC)
Single-atom catalysts (SACs) have emerged as one of the most promising alternatives to noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). While SACs can offer notable benefits in terms of lowering overall catalyst cost, there is still room for improvement regarding catalyst activity. To this end, we designed and successfully fabricated an ORR electro-catalyst in which atomic clusters are embedded in an atomically dispersed Fe-N-C matrix (Fe-AC@Fe-SA-N-C), as shown by comprehensive measurements using aberration-corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential of Fe-AC @Fe-SA-N-C is 0.912 V (versus reversible hydrogen electrode (RHE)), exceeding that of commercial Pt/C (0.897 V), Fe-SA-N-C (0.844 V), as well as the half-wave potentials of most reported non-platinum-group metal catalysts. The ORR activity of the designed catalyst stems from single-atom active centers but is markedly enhanced by the presence of Fe nanoclusters, as confirmed by both experimental measurements and theoretical calculations.
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