Existing proton exchange membranes have the disadvantages of low proton conductivity at high temperature, high cost, and poor barrier properties. Montmorillonite (MMT) materials have excellent thermal and chemical stability, and two-dimensional nanostructures formed by exfoliated MMT show excellent proton conductivity. Therefore, they are expected to become new proton exchange membrane materials. However, the existing exfoliation methods still lack a unified theoretical guidance. In this work, we systematically investigate the detailed swelling and exfoliation properties of MMT with different intercalation cations via extensive molecular dynamics simulations. We find that the swelling properties are determined by the hydration capacity of interlayer cations, and the exfoliation mainly occurs via a lateral sliding process between adjacent layers. The exfoliation energy barrier strongly depends on the interaction strength between interlayer cations and MMT nanosheets, swelling degree, and surface charge density. Lower interaction strength and a higher swelling degree together with larger surface charge density can result in an easy exfoliation process. Our work unveiled the detailed mechanism of the exfoliation process of MMT nanosheets and may contribute to the search for efficient MMT exfoliation methods.

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