The separation and preparation of theasinensins have been hot spots in the field of tea chemistry in recent years. However, information about the mechanism of efficient adsorption of tea theasinensins by resin has been limited. In this study, the adsorption equilibrium and thermodynamics of tea theasinensins by a high-efficiency macroporous adsorption HP20 resin were evaluated. The adsorption of theasinensin A, theasinensin B, and theasinensin C on HP20 resin were spontaneous physical reaction processes. Adsorption processes were exothermic processes, and lowering the temperature was beneficial to the adsorption. The Freundlich model was more suitable to describe the adsorption of tea theasinensins. The adsorption equilibrium constant and maximum adsorption capacity of theasinensin A were significantly higher than theasinensin B and theasinensin C, which indicated that the adsorption affinity of theasinensin A was stronger than that of theasinensin B and theasinensin C. The phenolic hydroxyl groups and intramolecular hydrogen bonds of theasinensin A were more than those of theasinensin B and theasinensin C, which might be the key to the resin’s higher adsorption capacity for theasinensin A. The HP20 resin was very suitable for efficient adsorption of theasinensin A.
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