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Issue 9, 2018
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Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal

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Abstract

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 E1/2 = 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 (Jk) 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.

Graphical abstract: Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal

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Publication details

The article was received on 21 May 2018, accepted on 15 Jun 2018 and first published on 27 Jun 2018


Article type: Communication
DOI: 10.1039/C8EE01481G
Citation: Energy Environ. Sci., 2018,11, 2348-2352
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    Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal

    Y. Han, Y. Wang, R. Xu, W. Chen, L. Zheng, A. Han, Y. Zhu, J. Zhang, H. Zhang, J. Luo, C. Chen, Q. Peng, D. Wang and Y. Li, Energy Environ. Sci., 2018, 11, 2348
    DOI: 10.1039/C8EE01481G

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