Methionine-based cationic polypeptide/polypeptide block copolymer with triple-stimuli responsiveness: DNA polyplexation and phototriggered release†,Polymer Chemistry

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Methionine-based cationic polypeptide/polypeptide block copolymer with triple-stimuli responsiveness: DNA polyplexation and phototriggered release†
Polymer Chemistry ( IF 4.1 ) Pub Date : 2018-02-26 00:00:00 , DOI: 10.1039/c8py00178b
Somdeb Jana _{1,

2,

3,

4} , Yajnaseni Biswas _{1,

2,

3,

4} , Tarun K. Mandal _{1,

2,

3,

4}

Affiliation

This study demonstrates the synthesis of positively charged 2-nitrobenzyl functionalized polymethionine (P[MetNB][Br]) and its block copolymer of pseudopeptidic poly(2-ethyl-2-oxazoline) (PEtOx-b-P[MetNB][Br]) by firstly employing ring-opening polymerization (ROP), followed by post-functionalization through nucleophilic substitution. The as-prepared cationic P[MetNB][Br] and PEtOx-b-P[MetNB][Br] are readily soluble in water, exhibiting responsiveness towards multiple stimuli such as ions, temperature and light. The aqueous solutions of both of the cationic polypeptides become cloudy in the presence of anions like I⁻, ClO₄⁻ and SCN⁻ due to the formation of insoluble anionically cross-linked colloidal aggregates of cationic polypeptides. These cloudy solutions of the polypeptide and polypeptide block copolymer both show reversible upper critical solution temperature (UCST)-type phase transitions due to the dissolution of the aggregates upon heating. The parameters, polypeptide concentrations and the nature of the anion and its concentration affect the cloud points in aqueous solutions. Upon irradiation with UV light (λ = 350 nm), the pendent nitrobenzyl sulfonium moiety of both of the cationic polypeptides undergoes photocleavage to a neutral polypeptide/polypeptide block copolymer. This study further demonstrates the binding of a cationic polypeptide/polypeptide block copolymer with calf thymus DNA (ctDNA) through electrostatic complexation and its phototriggered release as monitored by fluorescence spectroscopy and gel electrophoresis.

中文翻译：

具有三刺激响应性的基于蛋氨酸的阳离子多肽/多肽嵌段共聚物：DNA多聚化和光触发释放†

这项研究表明带正电荷的2-硝基苄基官能化聚蛋氨酸（P [MetNB] [Br]）及其假肽聚（2-乙基-2-恶唑啉）（PEtOx- b -P [MetNB] [Br]的嵌段共聚物）的合成），首先使用开环聚合（ROP），然后通过亲核取代进行后官能化。所制备的阳离子P [MetNB] [Br]和PEtOx- b -P [MetNB] [Br]易溶于水，对多种刺激（例如离子，温度和光）表现出响应性。两个阳离子多肽的水溶液成为阴离子的存在等我浑浊^-，CLO ₄^-和SCN ^-由于阳离子多肽的不溶性阴离子交联的胶态聚集体的形成。多肽和多肽嵌段共聚物的这些浑浊溶液由于加热时聚集体的溶解而均显示出可逆的上临界溶液温度（UCST）型相变。参数，多肽浓度以及阴离子的性质及其浓度会影响水溶液中的浊点。紫外线照射后（λ＝ 350nm），两个阳离子多肽的侧基硝基苄基sulf部分经历光裂解成中性多肽/多肽嵌段共聚物。这项研究进一步证明了阳离子多肽/多肽嵌段共聚物与小牛胸腺DNA（ctDNA）的结合通过静电络合及其光触发释放，如荧光光谱和凝胶电泳所监测。

更新日期：2018-02-26

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