Monomicelle‐Directed Engineering of Strained Carbon Nanoribbons as Oxygen Reduction Catalyst

Abstract

AbstractTo date, precisely tailoring local active sites of well‐defined earth‐abundant metal‐free carbon‐based electrocatalysts for attractive electrocatalytic oxygen reduction reaction (ORR), remains challenging. Herein, the authors successfully introduce a strain effect on active C–C bonds adjacent to edged graphitic nitrogen (N), which raises appropriate spin‐polarization and charge density of carbon active sites and kinetically favor the facilitation of O2 adsorption and the activation of O‐containing intermediates. Thus, the constructed metal‐free carbon nanoribbons (CNRs‐C) with high‐curved edges exhibit outstanding ORR activity with half‐wave potentials of 0.78 and 0.9 V in 0.5 m H2SO4 and 0.1 m KOH, respectively, overwhelming the planar one (0.52 and 0.81 V) and the N‐doped carbon sheet (0.41 and 0.71 V). Especially in acidic media, the kinetic current density (Jk) is 18 times higher than that of the planar one and the N‐doped carbon sheet. Notably, these findings show the spin polarization of the asymmetric structure by introducing a strain effect on the C–C bonds for boosting ORR.