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Emergence of Heptazine-Based Graphitic Carbon Nitride within Hydrogel Nanocomposites for Scarless Healing of Burn Wounds
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2020-11-23 , DOI: 10.1021/acsapm.0c01020
Aarti Singh 1 , Dakshi Kochhar 1 , Sampathkumar Jeevanandham 1 , Chirantan Kar 2 , Rohan Bhattacharya 1 , Adeeba Shakeel 1 , Monalisa Mukherjee 1
Affiliation  

Graphitic carbon nitride (gCN) has only recently experienced a renaissance in a myriad of domains despite existing as a long-established material described in the chemical literature. Notwithstanding the upturn, their conventional synthesis at extremely high temperatures yielding limiting compositions stands in the way of achieving a paradigm shift in gCN fabrication. With the ultimate goal of surpassing these hurdles, we utilize N-doped carbon nanosheets (N-CNS) as a filler in free-radical-mediated aqueous copolymerization. By dispersing N-CNS in a polymer matrix, high-performance mechanically robust composites could be developed and tailored to individual applications. As-synthesized hydrogel nanocomposite systems are used to decode the balance for emulating evolutionary accomplishments of nature’s nanocomposites like the “abalone’s nacre”. At a lower concentration (0.05%), N-CNS disperse homogeneously and interact intimately with the polymer matrix forming an “interphase” zone around individual nanofillers dramatically affecting the mobility of polymer chains to yield sheet architectures. On increasing the filler concentration (0.3%), the intercalation phenomenon gets perturbed due to an intrinsically oriented aggregation of nanofiller giving rise to a surge in entropy that leads to conspicuous buckling and tubular aggregates. At the interfacial regime, the poly(acrylic acid) domains come in closer proximity to the hydrophobic cages of N-CNS, and a nanoconfinement effect exerts high pressure manifesting acid-catalyzed condensation of melamine units to form, for the first time, quasi-two-dimensional heptazine-gCN (h-gCN) within hydrogel nanocomposites. Polymer properties are enhanced by the addition of N-CNS through complex interfacial interactions and the unique distributions of internanofiller distances. Endowed with mechanical properties that closely mimic natural skin and combined with the repurposed drug “losartan”, these hydrogel nanocomposites offer scarless healing of second-degree burns.

中文翻译:

水凝胶纳米复合材料中庚烷基石墨碳氮化物的出现,可无创地治愈烧伤。

石墨化的氮化碳(gCN)直到最近才经历了无数领域的复兴,尽管它作为化学文献中描述的悠久材料存在。尽管好转,但它们在极高温度下的常规合成产生了受限的组合物,阻碍了gCN制造中的范例转变。为了超越这些障碍,我们利用N掺杂碳纳米片(N-CNS)作为自由基介导的水性共聚中的填料。通过将N-CNS分散在聚合物基质中,可以开发高性能的机械坚固的复合材料,并针对各种应用进行定制。合成后的水凝胶纳米复合材料系统用于解码平衡,以模拟“鲍鱼的珍珠质”等自然纳米复合材料的进化成就。在较低的浓度(0.05%)下,N-CNS会均匀分散并与聚合物基质紧密相互作用,从而在各个纳米填料周围形成一个“相间”区域,从而极大地影响聚合物链的流动性,从而产生片状结构。在增加填料浓度(0.3%)时,由于纳米填料的内在取向聚集,插层现象受到干扰,从而引起熵激增,从而导致明显的屈曲和管状聚集体。在界面状态下,聚(丙烯酸)结构域更靠近N-CNS的疏水笼,纳米约束效应施加高压,这表明酸催化的三聚氰胺单元缩合首次形成了准三聚氰胺。水凝胶纳米复合材料中的二维庚嗪-gCN(h-gCN)。通过复杂的界面相互作用和NANOFILLER距离的独特分布,通过添加N-CNS可以增强聚合物的性能。这些水凝胶纳米复合材料具有与天然皮肤非常相似的机械性能,并结合了改用的药物“氯沙坦”,可无创地治愈二级烧伤。
更新日期:2020-12-11
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