Daengmankhong Jinjutha, Pinthong Thanyaporn, Promkrainit Sudarat, Yooyod Maytinee, Mahasaranon Sararat, Punyodom Winita, Ross Sukunya, Jongjitwimol Jirapas, Tighe Brian J, Derry Matthew J, Topham Paul D, Ross Gareth M
Biopolymer Group, Department of Chemistry, Faculty of Science, Naresuan University, Phitsanulok 65000, Thailand.
Center of Excellence in Biomaterials, Faculty of Science, Naresuan University, Phitsanulok 65000, Thailand.
Polymers (Basel). 2024 Sep 5;16(17):2522. doi: 10.3390/polym16172522.
This study investigates hydrogels based on 2-Acrylamido-2-methyl-1-propanesulfonic acid sodium salt (AMPS) copolymers, incorporating N-hydroxyethyl acrylamide (HEA) and 3-sulfopropyl acrylate potassium salt (SPA). The addition of HEA and SPA is designed to fine-tune the hydrogels' water absorption and mechanical properties, ultimately enhancing their characteristics and expanding their potential for biomedical applications. A copolymer of AMPS, 2-carboxyethyl acrylate (CEA) combined with methacrylic acid (MAA) as poly(AMPS-stat-CEA-stat-MAA, PACM), was preliminarily synthesized. CEA and MAA were modified with allyl glycidyl ether (AGE) through ring-opening, yielding macromers with pendant allyl groups (PACM-AGE). Copolymers poly(AMPS-stat-HEA-stat-CEA-stat-MAA) (PAHCM) and poly(AMPS-stat-SPA-stat-CEA-stat-MAA) (PASCM) were also synthesized and modified with AGE to produce PAHCM-AGE and PASCM-AGE macromers. These copolymers and macromers were characterized by H NMR, FT-IR, and GPC, confirming successful synthesis and functionalization. The macromers were then photocrosslinked into hydrogels and evaluated for swelling, water content, and mechanical properties. The results revealed that the PASCM-AGE hydrogels exhibited superior swelling ratios and water retention, achieving equilibrium water content (~92%) within 30 min. While the mechanical properties of HEA and SPA containing hydrogels show significant differences compared to PACM-AGE hydrogel (tensile strength 2.5 MPa, elongation 47%), HEA containing PAHCM-AGE has a higher tensile strength (5.8 MPa) but lower elongation (19%). In contrast, SPA in the PASCM-AGE hydrogels led to both higher tensile strength (3.7 MPa) and greater elongation (92%), allowing for a broader range of hydrogel properties. An initial study on drug delivery behavior was conducted using PACM-AGE hydrogels loaded with photosensitizers, showing effective absorption, release, and antibacterial activity under light exposure. These AMPS-based macromers with HEA and SPA modifications demonstrate enhanced properties, making them promising for wound management and drug delivery applications.
本研究调查了基于2-丙烯酰胺基-2-甲基-1-丙磺酸钠盐（AMPS）共聚物的水凝胶，其中包含N-羟乙基丙烯酰胺（HEA）和丙烯酸钾3-磺丙酯（SPA）。添加HEA和SPA旨在微调水凝胶的吸水性和机械性能，最终改善其特性并扩大其在生物医学应用中的潜力。初步合成了AMPS、丙烯酸2-羧乙酯（CEA）与甲基丙烯酸（MAA）的共聚物聚（AMPS-无规-CEA-无规-MAA，PACM）。通过开环用烯丙基缩水甘油醚（AGE）对CEA和MAA进行改性，得到带有烯丙基侧基的大分子单体（PACM-AGE）。还合成了共聚物聚（AMPS-无规-HEA-无规-CEA-无规-MAA）（PAHCM）和聚（AMPS-无规-SPA-无规-CEA-无规-MAA）（PASCM），并用AGE进行改性以制备PAHCM-AGE和PASCM-AGE大分子单体。通过核磁共振氢谱（¹H NMR）、傅里叶变换红外光谱（FT-IR）和凝胶渗透色谱（GPC）对这些共聚物和大分子单体进行了表征，证实了合成和功能化的成功。然后将大分子单体光交联成水凝胶，并对其溶胀、含水量和机械性能进行评估。结果表明，PASCM-AGE水凝胶表现出优异的溶胀率和保水性，在30分钟内达到平衡含水量（约92%）。虽然含HEA和SPA的水凝胶的机械性能与PACM-AGE水凝胶相比有显著差异（拉伸强度2.5MPa，伸长率47%），但含HEA的PAHCM-AGE具有较高的拉伸强度（5.8MPa）但较低的伸长率（19%）。相比之下，PASCM-AGE水凝胶中的SPA导致更高的拉伸强度（3.7MPa）和更大的伸长率（92%），从而使水凝胶具有更广泛的性能范围。使用负载光敏剂的PACM-AGE水凝胶进行了药物递送行为的初步研究，结果表明在光照下具有有效的吸收、释放和抗菌活性。这些经HEA和SPA改性的基于AMPS的大分子单体表现出增强的性能，使其在伤口处理和药物递送应用方面具有广阔前景。
