Institute of Macromolecular Compounds of the Russian Academy of Sciences, Bolshoi VO 31, 199004 St. Petersburg, Russia.
Institute of Experimental Medicine, Akademika Pavlova 12, 197376 St. Petersburg, Russia.
Int J Mol Sci. 2022 Dec 22;24(1):166. doi: 10.3390/ijms24010166.
The growth of microbial multidrug resistance is a problem in modern clinical medicine. Chemical modification of active pharmaceutical ingredients is an attractive strategy to improve their biopharmaceutical properties by increasing bioavailability and reducing drug toxicity. Conjugation of antimicrobial drugs with natural polysaccharides provides high efficiency of these systems due to targeted delivery, controlled drug release and reduced toxicity. This paper reports a two-step synthesis of colistin conjugates (CT) with succinyl chitosan (SucCS); first, we modified chitosan with succinyl anhydride to introduce a carboxyl function into the polymer molecule, which was then used for chemical grafting with amino groups of the peptide antibiotic CT using carbodiimide chemistry. The resulting polymeric delivery systems had a degree of substitution (DS) by CT of 3-8%, with conjugation efficiencies ranging from 54 to 100% and CT contents ranging from 130-318 μg/mg. The size of the obtained particles was 100-200 nm, and the ζ-potential varied from -22 to -28 mV. In vitro release studies at pH 7.4 demonstrated ultra-slow hydrolysis of amide bonds, with a CT release of 0.1-0.5% after 12 h; at pH 5.2, the hydrolysis rate slightly increased; however, it remained extremely low (1.5% of CT was released after 12 h). The antimicrobial activity of the conjugates depended on the DS. At DS 8%, the minimum inhibitory concentration (MIC) of the conjugate was equal to the MIC of native CT (1 µg/mL); at DS of 3 and 5%, the MIC increased 8-fold. In addition, the developed systems reduced CT nephrotoxicity by 20-60%; they also demonstrated the ability to reduce bacterial lipopolysaccharide-induced inflammation in vitro. Thus, these promising CT-SucCS conjugates are prospective for developing safe and effective nanoantibiotics.
微生物多重耐药性的增长是现代临床医学中的一个问题。通过增加生物利用度和降低药物毒性来改善药物的生物制药特性是一种有吸引力的策略,对活性药物成分进行化学修饰。将抗菌药物与天然多糖偶联可以提供这些系统的高效性,因为它们具有靶向递送、控制药物释放和降低毒性的作用。本文报道了两步法合成多粘菌素(CT)与琥珀酰壳聚糖(SucCS)的偶联物;首先,我们用琥珀酸酐修饰壳聚糖,在聚合物分子中引入羧基功能,然后用碳二亚胺化学法将其与肽抗生素 CT 的氨基进行化学接枝。得到的聚合物递药系统的 CT 取代度(DS)为 3-8%,偶联效率为 54-100%,CT 含量为 130-318μg/mg。所得颗粒的粒径为 100-200nm,ζ-电位在-22 至-28mV 之间。在 pH 7.4 下进行的体外释放研究表明酰胺键的水解非常缓慢,12 小时后 CT 的释放率为 0.1-0.5%;在 pH 5.2 时,水解速率略有增加;然而,仍然非常低(12 小时后释放 1.5%的 CT)。偶联物的抗菌活性取决于 DS。在 DS 为 8%时,偶联物的最低抑菌浓度(MIC)与天然 CT 的 MIC 相等(1μg/mL);在 DS 为 3%和 5%时,MIC 增加了 8 倍。此外,开发的系统降低了 CT 的肾毒性 20-60%;它们还表现出降低体外细菌脂多糖诱导的炎症的能力。因此,这些有前途的 CT-SucCS 偶联物有望开发出安全有效的纳米抗生素。