Dual-Shelled Multidoped Hollow Carbon Nanocages with Hierarchical Porosity for High-Performance Oxygen Reduction Reaction in Both Alkaline and Acidic Media.

Wang, Teng; Yang, Chao; Liu, Yijiang; Yang, Mei; Li, Xufeng; He, Yan; Li, Huaming; Chen, Hongbiao et al. · Nano Lett · 2020

basic_science · Level V

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Abstract

The rational design and facile synthesis of metal organic framework (MOF)-derived carbon materials with high oxygen reduction reaction (ORR) activity still remains challenging. Herein, we report on a simple yet robust route to dual-shelled Co, N, and S co-doped hollow carbon nanocages (denoted Co-N/S-DSHCN) with outstanding ORR performance. The concurrent compositional and structural engineering of the zeolitic imidazolate framework (ZIF-67), enabled by its coating with trithiocyanuric acid (TCA), yields core-shelled precursor particles which are subsequently carbonized into Co-N/S-DSHCN. Notably, Co-N/S-DSHCN-3.5 outperforms the commercial Pt/C, representing a +25 mV onset potential (<i>E</i><sub>on</sub>) and a +43 mV half-wave potential (<i>E</i><sub>1/2</sub>) in 0.1 M KOH and a comparable <i>E</i><sub>1/2</sub> to Pt/C in 0.5 M H<sub>2</sub>SO<sub>4</sub>, respectively. Such impressive ORR activities of Co-N/S-DSHCN-3.5 originate from the effective synergy of Co, N, and S co-doping (i.e., a compositional tuning) in conjunction with a unique dual-shelled hollow architecture containing hierarchical porosity (i.e., a structural tailoring).