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石墨烯量子点在引导聚合物自组装形成奇异的 Kagome 晶格和 Janus 纳米结构中的应用

Graphene Quantum Dots in the Game of Directing Polymer Self-Assembly to Exotic Kagome Lattice and Janus Nanostructures.

作者信息

Shakeel Adeeba, Bhattacharya Rohan, Jeevanandham Sampathkumar, Kochhar Dakshi, Singh Aarti, Mehra Lalita, Ghufran Maryam, Garg Piyush, Sangam Sujata, Biswas Subhrajit, Tyagi Amit, Kalyanasundaram Dinesh, Chakrabarti Sandip, Mukherjee Monalisa

机构信息

Amity Institute of Biotechnology , Amity University , Noida 201303 , India.

Amity Institute of Click Chemistry Research and Studies , Amity University , Noida 201303 , India.

出版信息

ACS Nano. 2019 Aug 27;13(8):9397-9407. doi: 10.1021/acsnano.9b04188. Epub 2019 Aug 7.

DOI:10.1021/acsnano.9b04188
PMID:31381848
Abstract

Graphene quantum dots (GQDs) are the harbingers of a paradigm shift that revitalize self-assembly of the colloidal puzzle by adding shape and size to the material-design palette. Although self-assembly is ubiquitous in nature, the extent to which these molecular legos can be engineered reminds us that we are still apprenticing polymer carpenters. In this quest to unlock exotic nanostructures ascending from eventual anisotropy, we have utilized different concentrations of GQDs as a filler in free-radical-mediated aqueous copolymerization. Extensive polymer grafting over the geometrically confined landscape of GQDs (0.05%) bolsters crystallization instilling a loom which steers interaction of polymeric cilia into interlaced equilateral triangles with high sophistication. Such two-dimensional (2D) assemblies epitomizing the planar tiling of "Star of David" forming a molecular kagome lattice (KL) without metal templation evoke petrichor. Interestingly, a higher percentage (0.3%) of GQDs allow selective tuning of the interfacial property of copolymers breaking symmetry due to surface energy incongruity, producing exotic Janus nanomicelles (JNMs). Herein, with the help of a suite of characterizations, we delineate the mechanism behind the formation of the KL and JNMs which forms a depot of heightened drug accretion with targeted delivery of 5-fluorouracil in the colon as validated by gamma scintigraphy studies.

摘要

石墨烯量子点(GQDs)是范式转变的先驱,通过为材料设计调色板增添形状和尺寸,重振了胶体拼图的自组装。尽管自组装在自然界中无处不在,但这些分子组件能够被设计的程度提醒我们,我们仍然是聚合物领域的新手。在探索从最终的各向异性中产生奇异纳米结构的过程中,我们在自由基介导的水相共聚反应中使用了不同浓度的GQDs作为填料。在几何受限的GQDs(0.05%)表面进行广泛的聚合物接枝,增强了结晶作用,形成了一种机制,该机制将聚合物纤毛的相互作用引导成高度复杂的交错等边三角形。这种二维(2D)组装体现了“大卫之星”的平面平铺,形成了一个没有金属模板的分子 Kagome 晶格(KL),令人联想到雨后的泥土气息。有趣的是,较高百分比(0.3%)的GQDs由于表面能不一致而打破对称性,从而允许对共聚物的界面性质进行选择性调节,产生奇异的 Janus 纳米胶束(JNMs)。在此,借助一系列表征,我们描绘了KL和JNMs形成背后的机制,其形成了一个增强药物积聚的储存库,并通过γ闪烁扫描研究验证了在结肠中对5-氟尿嘧啶的靶向递送。

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