Title

A Defect-Driven Metal-free Electrocatalyst for Oxygen Reduction in Acidic Electrolyte

RIS ID

131198

Publication Details

Li, D., Jia, Y., Chang, G., Chen, J., Liu, H., Wang, J., Hu, Y., Xia, Y., Yang, D. & Yao, X. (2018). A Defect-Driven Metal-free Electrocatalyst for Oxygen Reduction in Acidic Electrolyte. Chem, 4 (10), 2345-2356.

Abstract

Newly N-S-C coordination-structured active sites, originating from the integrity of edged thiophene S, graphitic N, and pentagon defects, were reconstructed by N-modified S defects in carbon aerogel with a 3D hierarchical macro-meso-microporous structure. This metal-free material exhibited outstanding oxygen reduction reaction (ORR) activity (e.g., half-wave potentials of 0.76 V in 0.5 M H2SO4 and 0.1 M HClO4; 0.85 V in 0.1 M KOH) with good stability and high current density in both acidic and alkaline electrolytes. The experimental and computational results reveal that the pentagon S defect is essential for the ORR in acidic electrolytes because it provides a remarkable increase in reactivity. One graphitic-type N in the meta-position of the pentagon defect further significantly improves the reactivity as a result of locally precise control of the electronic structure, thus forming highly active sites for ORR in acid.

Grant Number

ARC/DP170102267

Grant Number

ARC/CE140100012

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