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|Title:||Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal||Authors:||Han, Yunhu
|Keywords:||Engineering::Chemical engineering||Issue Date:||2018||Source:||Han, Y., Wang, Y., Xu, R., Chen, W., Zheng, L., Han, A., ... Li, Y. (2018). Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal. Energy & Environmental Science, 11(9), 2348--2352. doi:10.1039/C8EE01481G||Journal:||Energy & Environmental Science||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.||URI:||https://hdl.handle.net/10356/144573||ISSN:||1754-5692||DOI:||10.1039/C8EE01481G||Rights:||© 2018 The Royal Society of Chemistry. All rights reserved.||Fulltext Permission:||none||Fulltext Availability:||No Fulltext|
|Appears in Collections:||SCBE Journal Articles|
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