Zheng Xianying, Chen Feng, Zhang Jixi, Cai Kaiyong
Key Laboratory of Biorheological Science and Technology, Ministry of Education, College of Bioengineering, Chongqing University, No. 174 Shazheng Road, Chongqing 400044, China.
J Mater Chem B. 2016 Apr 14;4(14):2435-2443. doi: 10.1039/c5tb02784e. Epub 2016 Mar 21.
Mussel-inspired polydopamine (PDA), with its advanced bio-adhesive properties, has shown great potential in drug delivery based on host-guest interaction. However, it is difficult to synthesize PDA NPs of high surface area using the traditional polymerization of dopamine monomers in an alkaline solution. Taking advantage of the interaction between PDA and silicic acid inspired by biosilicification, PDA was rendered with high surface area in 70 nm-sized hybrid porous particles by a silica assisted one-pot preparation. PDA building blocks were successfully incorporated into the silica framework by controlled addition of dopamine (1.25-5 mol% with respect to the silica source) in a typical synthesis of mesoporous silica nanoparticles (MSNs). It is revealed that the cooperative molecular interaction between silicic acid and catechol groups of PDA results in a retardation of the silica condensation during the particle formation process. Moreover, the replacement of dopamine with polyphenols such as epigallocatechin gallate (EGCG) or tannic acid (TA) resulted in complete phase separation of the polymer and silica at the same molar ratio, suggesting the important role of amines in PDA towards stable hybridization in the particles. The application potential of the PDA-MSN hybrid nanocarriers is demonstrated by an unprecedentedly high drug (DOX) loading capacity of 1000 mg g, a sustained drug release, as well as enhanced killing efficiency of cancer cells at low dosage. These findings are expected to inspire strategies and pave a way for utilizing PDA for constructing organic-inorganic composite nanocarriers.
受贻贝启发的聚多巴胺(PDA)具有优异的生物粘附特性,在基于主客体相互作用的药物递送方面展现出巨大潜力。然而,利用多巴胺单体在碱性溶液中的传统聚合方法难以合成具有高比表面积的PDA纳米颗粒。借鉴生物矿化中PDA与硅酸之间的相互作用,通过二氧化硅辅助的一锅法制备,使PDA在70纳米尺寸的混合多孔颗粒中具有高比表面积。在介孔二氧化硅纳米颗粒(MSN)的典型合成中,通过控制多巴胺(相对于硅源为1.25 - 5摩尔%)的添加量,成功将PDA构建单元掺入二氧化硅骨架中。研究表明,硅酸与PDA的儿茶酚基团之间的协同分子相互作用导致颗粒形成过程中二氧化硅缩合反应的延迟。此外,用表没食子儿茶素没食子酸酯(EGCG)或单宁酸(TA)等多酚取代多巴胺,在相同摩尔比下会导致聚合物与二氧化硅完全相分离,这表明PDA中的胺基对于颗粒中稳定杂化起着重要作用。PDA - MSN混合纳米载体的应用潜力体现在其前所未有的1000毫克/克高载药量、持续的药物释放以及低剂量下增强的癌细胞杀伤效率。这些发现有望启发相关策略,并为利用PDA构建有机 - 无机复合纳米载体铺平道路。