Poly(vinyl alcohol)-Assisted Exfoliation and Grafting Modification of Boron Nitride Nanosheets with a High Aspect Ratio via a Continuous Production Method for Energy Storage and Thermal Management

Hexagonal boron nitride nanosheets (BNNS) integrating many extraordinary properties are usually combined with polymers to fabricate multifunctional dielectric materials for energy storage and thermal management. Unfortunately, the existing technologies for producing BNNS generally have the disadvantages of inefficiency and low product quality, which significantly hinder the wide application of high-value nanocomposites. Herein, a novel poly(vinyl alcohol) (PVA)-assisted pan-milling method based on the innovative solid-state shear milling (S³ M) technology is reported for the production of high-quality BNNS. The uniform three-dimensional (3D) shear force field generated by pan milling not only ensured the high aspect ratio of BNNS (the average lateral size of ∼954 nm and the average thickness of ∼3.7 nm) but also induced the mechanochemical reaction between PVA and BNNS to achieve in situ grafting modification on the BNNS surface. The simultaneous high-quality exfoliation and surface modification of BNNS positively contributed to the mechanical, dielectric, and thermal conduction properties of BNNS/PVA nanocomposites. At the BNNS content of 10 wt %, the BNNS/PVA composite film exhibited excellent robustness (Young's modulus of 5305 MPa and the tensile strength of 83 MPa), with a satisfactory breakdown strength (<i>E</i>_b of 134.7 MV/m) and dielectric constant (∼5 at 1000 Hz). In addition, the substantial improvement of thermal conductivity (from 0.88 to 5.59 W·m^-1·K^-1) guaranteed the stability of the dielectric properties of the nanocomposites at high temperatures. This pan-milling method characterized by green and efficiency is highly scalable to other two-dimensional (2D) layered materials, providing a practical strategy for the industrial fabrication of nanocomposites in elevated-temperature energy storage.