聚（丙烯酸）和羟乙基纤维素水凝胶中结构依赖性二氧化氯释放：来自实时正电子湮没寿命谱和量子化学计算的见解

Structure-dependent chlorine dioxide release from poly(acrylic acid) and hydroxyethyl cellulose hydrogels: Insights from real-time positron annihilation lifetime spectroscopy and quantum chemical calculations.

作者信息

Poursafar Pegah, Kazsoki Adrienn, Palcsó Barnabás, Süvegh Károly, Zelkó Romána

机构信息

University Pharmacy Department of Pharmacy Administration, Faculty of Pharmaceutical Sciences, Semmelweis University, Hőgyes E. Street 7-9, H-1092 Budapest, Hungary.

Eötvös Loránd University Laboratory of Nuclear Chemistry, P.O. Box 32, H-1518 Budapest, Hungary.

出版信息

Food Chem X. 2025 Jul 11;29:102782. doi: 10.1016/j.fochx.2025.102782. eCollection 2025 Jul.

DOI:10.1016/j.fochx.2025.102782

PMID:40852572

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12369423/

Abstract

Chlorine dioxide (ClO₂) is a potent disinfectant used in controlled-release systems for water treatment and antimicrobial purposes. This study investigates ClO₂ release kinetics in poly(acrylic acid) (PAA) and hydroxyethyl cellulose (HEC) hydrogels via positron annihilation lifetime spectroscopy and quantum chemical modeling. PAA hydrogels released ClO₂ 2.5 times faster than HEC, with a 68.7 % decrease in o-Ps lifetime intensity in 12 h, compared to 27.3 % for HEC. This rapid release is linked to PAA's linear, anionic structure, showing binding energies of -24.8 kJ/mol for ClO₂ and - 65.6 kJ/mol for water. HEC hydrogels showed concentration-dependent release; 4 %/w HEC retained 57.6 % more ClO₂ after 24 h than 2 %w/w HEC. Quantum calculations confirmed stronger secondary bond energies for PAA (-24.8 kJ/mol) than HEC (-19.6 kJ/mol) with ClO₂, revealing structure-dependent release mechanisms. These results highlight polymer architecture's critical role in controlled-release behavior, guiding hydrogel-based antimicrobial delivery design for food preservation and water treatment.

摘要

二氧化氯（ClO₂）是一种强效消毒剂，用于水处理和抗菌的控释系统。本研究通过正电子湮没寿命谱和量子化学建模研究了二氧化氯在聚丙烯酸（PAA）和羟乙基纤维素（HEC）水凝胶中的释放动力学。PAA水凝胶释放ClO₂的速度比HEC快2.5倍，在12小时内邻位正电子素（o-Ps）寿命强度降低了68.7%，而HEC为27.3%。这种快速释放与PAA的线性阴离子结构有关，其对ClO₂的结合能为-24.8kJ/mol，对水的结合能为-65.6kJ/mol。HEC水凝胶表现出浓度依赖性释放；24小时后，4%/w的HEC比2%w/w的HEC多保留57.6%的ClO₂。量子计算证实，PAA（-24.8kJ/mol）与ClO₂的二级键能比HEC（-19.6kJ/mol）更强，揭示了结构依赖性释放机制。这些结果突出了聚合物结构在控释行为中的关键作用，为基于水凝胶的食品保鲜和水处理抗菌递送设计提供了指导。