Adjusting the length of supramolecular polymer bottlebrushes by top-down approaches.
Adjusting the length of supramolecular polymer bottlebrushes by top-down approaches.
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DOI：
10.3762/bjoc.17.175
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发表时间：
2021
影响因子：
2.7
通讯作者：
Brendel JC
中科院分区：
文献类型：
--
作者：
Klein T;Gruschwitz FV;Kuchenbrod MT;Nischang I;Hoeppener S;Brendel JC
控制一维聚合物纳米结构的长度仍然是这些结构走向应用的关键挑战。在这里，我们表明，自上而下的处理有利于直接调整的长度聚环氧乙烷（PEO）为基础的超分子聚合物瓶刷（SPBs）在水溶液中。这些圆柱形结构通过由位于纤维的疏水核心内的苯三脲（BTU）或苯三肽（BTP）基序形成的定向氢键自组装。从不同的有机溶剂到水的缓慢转变首先导致形成微米长的纤维，随后可以通过超声处理或双重不对称离心将其破碎。后者允许更好地调节所施加的剪切应力，从而能够根据时间和旋转速率接近不同尺寸的碎片。扩展的超声处理和断裂分析进一步允许估计BTU和BTP系统的拉伸强度为约16 MPa。与这些SPB的高动力学稳定性相结合，所应用的自上而下的方法代表了一种易于实现的技术，该技术朝向1D聚合物纳米结构，其具有在感兴趣的范围内可调节的长度，用于透视生物医学应用。
Controlling the length of one-dimensional (1D) polymer nanostructures remains a key challenge on the way toward the applications of these structures. Here, we demonstrate that top-down processing facilitates a straightforward adjustment of the length of polyethylene oxide (PEO)-based supramolecular polymer bottlebrushes (SPBs) in aqueous solutions. These cylindrical structures self-assemble via directional hydrogen bonds formed by benzenetrisurea (BTU) or benzenetrispeptide (BTP) motifs located within the hydrophobic core of the fiber. A slow transition from different organic solvents to water leads first to the formation of µm-long fibers, which can subsequently be fragmented by ultrasonication or dual asymmetric centrifugation. The latter allows for a better adjustment of applied shear stresses, and thus enables access to differently sized fragments depending on time and rotation rate. Extended sonication and scission analysis further allowed an estimation of tensile strengths of around 16 MPa for both the BTU and BTP systems. In combination with the high kinetic stability of these SPBs, the applied top-down methods represent an easily implementable technique toward 1D polymer nanostructures with an adjustable length in the range of interest for perspective biomedical applications.
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