Synthesis of highly thermal conductive carbon nanotubes on cellulose nanofiber film-loaded polyethylene glycol phase change material with flame retardancy by layered double hydroxide

The nitrogen-doped carbon nanotubes (CNTs) were obtained by using methyl orange as a soft template and high temperature treatment, on which the layered double hydroxide (LDH) was grown in situ by hydrothermal method, and finally mixed with the phase change materials (PCM) by vacuum filtration to obtain a series of novel composite films with great flame retardancy and thermal conductivity. The use of cellulose nanofiber (CNF), polyvinylpyrrolidone (PVP) and polyethylene glycol (PEG) as PCM increased the film-forming properties, and the CNTs could improve the thermal conductivity of composites, while reducing the agglomeration of LDH nanolayers and improving the flame retardancy of the composite films. The results showed that the LDH grown on the nanotubes had a typical hexagonal lamellar structure, and its uniform distribution was the fundamental reason for the flame retardancy of the films which was verified by defined combustion experiments, the shortest self-extinguishing time and the least unburned area were achieved at a mass ratio of 7.14 % of LDH material. The melt and crystallization enthalpies of the thermally conductive flame-retardant films were 74.65 J/g−1 and 74.82 J/g−1, and the thermal conductivity of the material was increased to 0.04129 W/(m·K) after the use of 2.5 % thermally conductive filler. It can reduce the temperature of LED by up to 5.9 °C during the LED opening process and up to 5.2 °C during the LED closing process.