Optimal Configuration of N-Doped Carbon Defects in 2D Turbostratic Carbon Nanomesh for Advanced Oxygen Reduction Electrocatalysis

Angew Chem Int Ed Engl. 2020 Jul 13;59(29):11999-12006. doi: 10.1002/anie.202000936. Epub 2020 May 12.

Abstract

The charge redistribution strategy driven by heteroatom doping or defect engineering has been developed as an efficient method to endow inert carbon with significant oxygen reduction reaction (ORR) activity. The synergetic effect between the two approaches is thus expected to be more effective for manipulating the charge distribution of carbon materials for exceptional ORR performance. Herein we report a novel molecular design strategy to achieve a 2D porous turbostratic carbon nanomesh with abundant N-doped carbon defects (NDC). The molecular level integration of aromatic rings as the carbon source and urea units as the N source and sacrificial template into the novel precursor of polyurea (PU) promises the formation of abundant carbon edge defects and N doping sites. A special active site-a carbon edge defect doped with a graphitic valley N atom-was revealed to be responsible for the exceptional ORR performance of NDC material.

Keywords: carbon defects; molecular design; nitrogen doping; oxygen reduction reaction.