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Modular Self-Assembly of Protein Cage Lattices for Multistep Catalysis
ACS Nano ( IF 15.8 ) Pub Date : 2017-11-20 00:00:00 , DOI: 10.1021/acsnano.7b06049
Masaki Uchida 1 , Kimberly McCoy 1 , Masafumi Fukuto , Lin Yang , Hideyuki Yoshimura 1, 2 , Heini M. Miettinen , Ben LaFrance , Dustin P. Patterson 3 , Benjamin Schwarz 1 , Jonathan A. Karty 1 , Peter E. Prevelige 4 , Byeongdu Lee 5 , Trevor Douglas 1
Affiliation  

The assembly of individual molecules into hierarchical structures is a promising strategy for developing three-dimensional materials with properties arising from interaction between the individual building blocks. Virus capsids are elegant examples of biomolecular nanostructures, which are themselves hierarchically assembled from a limited number of protein subunits. Here, we demonstrate the bio-inspired modular construction of materials with two levels of hierarchy: the formation of catalytically active individual virus-like particles (VLPs) through directed self-assembly of capsid subunits with enzyme encapsulation, and the assembly of these VLP building blocks into three-dimensional arrays. The structure of the assembled arrays was successfully altered from an amorphous aggregate to an ordered structure, with a face-centered cubic lattice, by modifying the exterior surface of the VLP without changing its overall morphology, to modulate interparticle interactions. The assembly behavior and resultant lattice structure was a consequence of interparticle interaction between exterior surfaces of individual particles and thus independent of the enzyme cargos encapsulated within the VLPs. These superlattice materials, composed of two populations of enzyme-packaged VLP modules, retained the coupled catalytic activity in a two-step reaction for isobutanol synthesis. This study demonstrates a significant step toward the bottom-up fabrication of functional superlattice materials using a self-assembly process across multiple length scales and exhibits properties and function that arise from the interaction between individual building blocks.

中文翻译:

蛋白质笼格的模块化自组装,用于多步催化

将单个分子组装成分层结构是开发具有因单个构造块之间的相互作用而产生的特性的三维材料的有前途的策略。病毒衣壳是生物分子纳米结构的典范,它们本身是由有限数量的蛋白质亚基组成的层次结构。在这里,我们展示了具有两个层次结构的材料的生物启发性模块化结构:通过衣壳亚基的定向自组装和酶包封,形成具有催化活性的单个病毒样颗粒(VLP),以及这些VLP建筑物的组装块成三维数组。组装后的阵列结构成功地从无定形聚集体变为具有面心立方晶格的有序结构,通过修改VLP的外表面而不改变其整体形态来调节粒子间的相互作用。组装行为和所得晶格结构是单个颗粒外表面之间的颗粒间相互作用的结果,因此与封装在VLP中的酶货物无关。这些由两类酶包装的VLP模块组成的超晶格材料在异丁醇合成的两步反应中保持了偶联的催化活性。这项研究表明,采用跨多个长度尺度的自组装工艺,朝着自底向上制造功能性超晶格材料迈出了重要的一步,并且展现出了各个构件之间的相互作用所产生的特性和功能。
更新日期:2017-11-21
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