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

Yunhu Han, Yanggang Wang, Ruirui Xu, Wenxing Chen, Lirong Zheng, Aijuan Han, Youqi Zhu, Jian Zhang, Huabin Zhang, Jun Luo, Chen Chen, Qing Peng, Dingsheng Wang, Yadong Li

Research output: Contribution to journalArticlepeer-review

328 Scopus citations

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.
Original languageEnglish (US)
Pages (from-to)2348-2352
Number of pages5
JournalEnergy and Environmental Science
Volume11
Issue number9
DOIs
StatePublished - Sep 1 2018
Externally publishedYes

Bibliographical note

Generated from Scopus record by KAUST IRTS on 2022-09-15

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