期刊
ENERGY & ENVIRONMENTAL SCIENCE
卷 11, 期 9, 页码 2348-2352出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ee01481g
关键词
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资金
- National Postdoctoral Program for Innovative Talents [BX201600084]
- China Ministry of Science and Technology [2016YFA, 0202801]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117]
Adjusting the electronic structure of the active center is a highly effective strategy for improving the performance of catalysts. Herein, we report an atomically dispersed catalyst (FeCl1N4/CNS), which realized for the first time a great improvement of the ORR by controlling the electronic structure of the central metal with a coordinated chlorine. The half-wave potential of FeCl1N4/CNS is E-1/2 = 0.921 V, which is the highest among the reported values for non-precious metal electrocatalysts and far exceeds that of FeN4/CN and commercial Pt/C in alkaline solution. Besides an exceptionally high kinetic current density (J(k)) of 41.11 mA cm(-2) at 0.85 V, it also has a good methanol tolerance and outstanding stability. Experiments and DFT demonstrated that the near-range interaction with chlorine and the long-range interaction with sulfur of Fe modulated the electronic structure of the active site, thus resulting in a great improvement of the ORR in alkaline media. The present findings could open new avenues for the design of superior electrocatalysts.
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