Facile and Universal Defect Engineering Toward Highly Stable Carbon‐Based Polymer Brushes with High Grafting Density

Abstract Carbon‐based polymer brushes (CBPBs) are an important class of functional polymer materials, which synergistically combine the advantageous properties of both carbons and polymers. However, the conventional fabrication procedures of CBPBs involve tedious multistep modification, including preoxidation of carbon substrates, introduction of initiating groups, and subsequent graft polymerization. In this study, a simple yet versatile defect‐engineering strategy is proposed for the efficient synthesis of high‐grafting‐density CBPBs with highly stable CC linkages via free radical polymerization. This strategy involves the introduction and removal of nitrogen heteroatoms in the carbon skeletons via a simple temperature‐Fmed heat treatment, leading to the formation of numerous carbon defects (e.g., pentagons, heptagons, and octagons) with reactive C=C bonds in the carbon substrates. The as‐proposed methodology enables the facile fabrication of CBPBs with various carbon substrates and polymers. More importantly, the highly grafted polymer chains in the resulting CBPBs are tethered with the carbon skeletons by robust CC bonds, which can endure strong acid and alkali environments. These interesting findings will shed new light on the well‐orchestrated design of CBPBs and broaden their applications in various areas with fascinating performances.