Vibrational Exfoliation of 2D Materials

ABSTRACT Liquid phase exfoliation has emerged as a key approach for the formulation and application of solution‐processed 2D materials. Contemporary methods, such as shear mixing and sonication, are sensitive to solid loadings and mixture rheology, limiting their production capacity. Here, we explore the vibration of dispersions at accelerations up to 100 as a method to address these challenges. We find that this vibrational exfoliation approach produces few‐layer graphene nanosheets through a unique material transformation pathway. Precursor particles impact vessel boundaries leading to edge folding, particle fracture, and sheet peeling. Using high‐fidelity computational models, we reveal the hydrodynamics behind this vibration process, and identify the conditions where mechanical forces in the dispersion exceed the interlayer binding energy and produce few‐layer nanosheets. We show that vibration exfoliation can be applied to dispersions containing extremely high solid loadings of up to 1000 mg mL ⁻¹ with no discernible drop in yield. This performance insensitivity to a broad range of mixture rheologies substantially increases production rates and can support diverse formulations of functional inks. We examine the application of this method to other layered materials such as h‐BN, MoS ₂ , and WS ₂ , and establish opportunities for future optimization.