Linker-Mediated Assembly of Virus-Like Particles into Ordered Arrays via Electrostatic Control
Linker-Mediated Assembly of Virus-Like Particles into Ordered Arrays via Electrostatic Control
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DOI：
10.1021/acsabm.9b00166
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发表时间：
2019-05-20
影响因子：
4.7
通讯作者：
Jadhao, Vikram
中科院分区：
文献类型：
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作者：
Brunk, Nicholas E.;Uchida, Masaki;Jadhao, Vikram
纳米级病毒样颗粒（vlp）是由蛋白质亚基自组装而成的，为生成分层组装的功能材料（如仿生催化系统和光学超材料）提供了可能性。我们利用实验和计算方法的结合，探索了在广泛的离子条件下控制和调整高阶VLPs组装成有序阵列材料的能力。综合方法表明，P22 VLP变体，通过基因工程表现出不同的表面电荷，在PAMAM树状大分子作为相反电荷的大分子连接物存在下自组装成有序阵列。有序组装发生在与VLP表面电荷密切相关的最佳离子强度下。无论VLP的表面电荷如何，有序的VLP阵列表现出相同的远程顺序和相似的VLP结合枝状大分子结构。实验验证的模型确定了自组装过程的关键静电和动力学机制，并指导树状分子浓度的调节作为控制参数来调节VLPs的组装。集成方法为通过工程VLPs的自组装制造活性功能材料开辟了新的设计和控制策略。
Nanoscale virus-like particles (VLPs), which are self-assembled from protein subunits, offer the possibility of generating hierarchically assembled functional materials such as biomimetic catalytic systems and optical metamaterials. We explore the capacity to control and tune a higherorder assembly of VLPs into ordered array materials over a wide range of ionic conditions using a combination of experimental and computational methods. The integrated methodology demonstrates that P22 VLP variants, genetically engineered to exhibit different surface charges, self-assemble into ordered arrays in the presence of PAMAM dendrimers acting as oppositely charged, macromolecular linkers. Ordered assembly occurs at an optimal ionic strength that strongly correlates with the VLP surface charge. The ordered VLP arrays exhibit the same long-range order and a similar configuration of VLP-bound dendrimers, regardless of the VLP surface charge. The experimentally validated model identifies key electrostatic and kinetic mechanisms underlying the self-assembly process and guides the modulation of dendrimer concentration as a control parameter to tune the assembly of VLPs. The integrated approach opens new design and control strategies to fabricate active functional materials via the self-assembly of engineered VLPs.