A simple surface engineering to develop the potential of carbon nitride nanosheets in high-performance polymer nanocomposites conducted by first-principles calculations

Abstract

The incompatible interface between carbon nitride (CN) nanosheets and polymer resin is a huge challenge to develop high-performance polymer/CN nanocomposites. Recently, the complicated surface functionalization methods reported severely hinder the commercial production and practical application of polymer/CN nanocomposites. Herein, conducted by the first-principles calculations, a simple surface engineering is put forward to change the surface characteristic of CN nanosheets by rapidly introducing oxygen atoms with a chemical oxidation method. Presented by the first-principles calculations, it is found that the introduction of oxygen atoms can enhance the adsorption energy between oxygen-doping carbon nitride nanosheets (OCN) and waterborne polyurethane (WPU) resin. As a result, a stronger interfacial interaction and better dispersion state are presented in WPU/OCN nanocomposites, thus laying the foundation for the properties enhancement. Further, effective suppression effects for thermal pyrolysis and fire hazards of WPU resin are demonstrated by OCN nanosheets. As presented by cone calorimeter results, the peak values of heat release rate and total heat release in WPU/OCN-2 are decreased to 806 kW/m2 and 43.3 MJ/m2, significantly less than those of pure WPU (1028 kW/m2 and 55.9 MJ/m2). Meanwhile, more char residue, lower signal intensity of pyrolysis gas, and a prolonged time for signal peak also confirm that the addition of 2.0 wt% OCN nanosheets can hinder the thermal degradation behavior of WPU resin. In addition, the introduction of oxygen atoms promotes the formation of hydrogen bond interactions between OCN nanosheets and WPU matrix, thus enhancing interfacial compatibility and overcoming the re-stack problem. As a result, break strength and elongation at break of WPU/OCN-2 are up to 621% and 24.4 MPa, respectively. The combination of first-principles calculations and surface engineering opens a new approach for designing and developing high-performance polymer nanocomposites.