DNA步行器调控的纳米粒子超晶格  

DNA Walker-Programmed Nanoparticle Superlattice

作　　者：郭宜君 魏冰 周翔[1] 姚东宝 梁好均[1,2] Yijun Guo;Bing Wei;Xiang Zhou;Dongbao Yao;Haojun Liang(CAS Key Laboratory of Soft Matter Chemistry,Collaborative Innovation Center of Chemistry for Energy Materials,Department of Polymer Science and Engineering,University of Science and Technology of China,Hefei 230026,China;Hefei National Laboratory for Physical Sciences at the Microscale,Hefei 230026,China)

机构地区：[1]中国科学院软物质化学重点实验室,能源材料化学协同创新中心,中国科学技术大学高分子科学与工程系,合肥230026 [2]合肥微尺度物质科学国家实验室,合肥230026

出　　处：《化学学报》2021年第2期192-199,共8页Acta Chimica Sinica

基　　金：国家自然科学基金(Nos.21991132,52003264);中央高校基本业务费(No.WK20602000026)资助。

摘　　要：作为一种精巧的DNA纳米机器,DNA步行器因其优异的可设计性及可编程性在众多研究领域中展示出强大的应用价值.本工作通过将基于催化发夹组装的双足DNA步行器与DNA功能化的金纳米粒子(即球形核酸)组装相结合,开发了一种具有时间依赖性的DNA步行器驱动球形核酸恒温有序组装的策略.以单组分球形核酸组装体系为例, DNA步行器通过发夹催化组装反应驱动在球形核酸表面上随机行走并逐渐产生带有活性粘性末端的DNA杂交结构,促使球形核酸表面粘性末端间的"键合"速率与其组装速率在时间尺度上保持同步,从而得到面心立方(FCC)晶型的超晶格结构.基于类似原理,作者还构建了一种DNA步行器驱动的双组分球形核酸组装体系并以此得到氯化铯(CsCl)晶型的超晶格结构.As a kind of sophisticated dynamic DNA nanomachine, DNA walker has shown powerful application ability in many aspects due to its excellent structural designability and programmability. Taking advantage of stochastic DNA tracks on surface and adaptable DNA outputs of the well-known catalytic hairpin assembly(CHA) circuits, the DNA walkers that move along DNA-coated three-dimensional particle surfaces have attracted much interests. On the other hand, in the field of DNA-mediated nanoparticle assembly, self-assembly of nanoparticles is a thermodynamically driven nonequilibrium process, which is easily trapped at intermediate local free-energy minima, resulting in a disordered structure. Therefore, effective strategies to evade each local free-energy minimum are highly desired. In addition to the traditional annealing strategy, the time-dependent strategy relied on toehold-mediated strand-displacement DNA circuit recently reported by our group has been proven an alternative solution, where interactions between nanoparticles can be tuned in a time-dependent manner for programming dynamic pathway to achieve a free-energy minimum. Through integrating a CHA-based bipedal DNA walker with a DNA-functionalized gold nanoparticle(i.e., spherical nucleic acid;SNA) assembly, a time-dependent strategy for assembly of SNAs programmed by DNA walker at constant temperature was developed in this work. In our strategy, the active sticky ends used for assembly of SNAs can be gradually generated on nanoparticle surface after the walking of the bipedal DNA walker driven by the CHA reaction to induce the synchronization of assembly and bonding between SNAs, thereby obtaining ordered nanoparticle superlattice structure. Take a one-component SNA assembly system for example, the dynamic walking process of the bipedal DNA walker on the surface of SNA was proved to be stable with good walking ability and persistence at first. Then, the SNA assembly kinetics results showed that the bipedal walker concentrations and DNA linker ratios could grea

关 键 词：动态DNA纳米机器 双足DNA步行器 金纳米粒子 球形核酸组装 超晶格结构 

分 类 号：TB383.1[一般工业技术—材料科学与工程] Q523[生物学—生物化学]