Quantitative Criteria for Solvent Selection in Liquid-Phase Exfoliation: Balancing Exfoliation and Stabilization...

Area of Science:

• Materials Science
• Chemical Engineering
• Computational Chemistry

Background:

• Liquid-phase exfoliation (LPE) is crucial for obtaining 2D materials.
• Solvent selection significantly impacts LPE efficiency by influencing interlayer interactions and material stability.
• Understanding solvent-material interactions is vital for optimizing LPE processes.

Purpose of the Study:

• To theoretically analyze and experimentally validate the optimal solvent selection for Mg(OH)₂ liquid-phase exfoliation.
• To establish a quantitative framework for predicting solvent performance in LPE.
• To elucidate the physicochemical properties governing solvent effectiveness in LPE.

Main Methods:

• First-principles calculations were employed to determine exfoliation and binding energies.
• Principal component analysis (PCA) was used to identify key solvent properties influencing LPE.
• Experimental validation was performed to confirm theoretical predictions.
• Biaxial straining theory was applied to understand solvent-material interactions.

Main Results:

• Dimethyl sulfoxide (DMSO) demonstrated the lowest exfoliation energy, indicating reduced interlayer attraction.
• N-methyl-2-pyrrolidone (NMP) exhibited the highest binding energy, suggesting superior stabilization of exfoliated layers.
• PCA revealed that solvent polarity and dipole moment govern exfoliation energy, while planarity and polarity influence binding energy.
• Experimental results confirmed DMSO's superior performance over water for Mg(OH)₂ LPE.

Conclusions:

• A quantitative framework for solvent selection in LPE of Mg(OH)₂ has been established.
• The findings provide insights into optimizing solvent choice for enhanced LPE efficiency.
• This study facilitates the rational design of LPE processes for 2D materials.