ABSTRACT Stilbenes are bioactive phytochemicals with notable health benefits, yet their extraction is hindered by hydrophobicity and reliance on toxic solvents. This study introduces a green, sustainable approach for stilbene extraction using hydrophilic natural deep eutectic solvents (NADES), with cajaninstilbene acid (CSA) from pigeon pea ( Cajanus cajan ) as the model compound. After screening, the optimal NADES and ultrasound‐assisted extraction conditions were identified, achieving a predicted CSA yield of 0.832 mg/g. The method demonstrated excellent reusability and sustainability. Spectroscopic analyses (ATR‐FTIR, 1 H NMR, 1 3 C NMR, 2D NOESY), COSMO‐RS, and molecular dynamics (MD) simulations revealed that NADES‐4 forms a hydrogen‐bonded supramolecular structure involving betaine, glycerol, and water. MD simulations further clarified the thermodynamics and synergistic non‐covalent interactions driving CSA solubilization. These findings provide mechanistic insights into NADES‐based stilbene extraction and support the development of eco‐friendly technologies for plant resource utilization.
Zhang et al. (Fri,) studied this question.