DNA-Origami-Directed Self-Assembly of Discrete Silver-Nanoparticle Architectures
DNA-Origami-Directed Self-Assembly of Discrete Silver-Nanoparticle Architectures
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DOI：
10.1002/anie.201000330
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发表时间：
2010-01-01
影响因子：
16.6
通讯作者：
Liu, Yan
中科院分区：
文献类型：
--
作者：
Pal, Suchetan;Deng, Zhengtao;Liu, Yan
自下而上的贵金属纳米粒子（NPs）的纳米级精度的组织是纳米技术的一个重要目标。[1]这些纳米粒子的DNA引导的自组装已经显示出应对这一挑战的重大进展。[2]在DNA引导下，纳米粒子被组织成离散的、[3]一维的、[4]二维的、[5]和三维的结构已经取得了巨大的进展。[6]金纳米粒子（AuNPs）的简单DNA功能化策略现在可用，使AuNPs成为随后自组装形成更高阶结构的首选（更容易）候选物。相反，介导的DNA自组装组装的组装银纳米粒子（AgNP）到高阶，明确定义的离散的纳米结构还没有得到很好的探索，主要是由于这些系统的相对不稳定性。Ag比Au更容易氧化，因此，AgNP表面上的共轭配体更不稳定，并且AgNP倾向于在具有高盐浓度的溶液中不可逆地聚集。然而，高盐浓度对于有效的DNA自组装至关重要。最近，我们和其他人开始通过将多个硫部分连接到DNA [4c]以形成稳定的AgNP-DNA缀合物来解决这个问题，该缀合物在具有高盐浓度的缓冲液中抵抗聚集。[7]在本文中，我们报道了一种自下而上的方法，通过使用与嵌合硫代磷酸化DNA（ps-po DNA）缀合的AgNP（直径20 nm）作为构建块，在三角形形状的自组装DNA折纸结构上制造离散的、有序的AgNP纳米结构。离散的单体、二聚体和三聚体AgNP结构和AgNP-AuNP杂化结构可以以高收率可靠地构建。我们证明，相邻的AgNPs之间的中心到中心的距离可以精确地从94到29 nm调谐，其中的距离分布是有限的纳米粒子的尺寸分布。DNA折纸技术[8]是一种开发良好的方法，通过使用大约200个短的DNA链将单链基因组DNA（例如M13 mp 18，7249个核苷酸长的DNA）折叠成几何定义的纳米颗粒来创建完全可寻址的DNA纳米结构。在这项研究中，我们利用DNA折纸的组织能力，开发了一种强大的策略，将难以控制的AgNP组装成定义明确的纳米颗粒。
The bottom-up organization of noble-metal nanoparticles (NPs) with nanometer-scale precision is an important goal in nanotechnology.[1] The DNA-guided self-assembly of these nanoparticles has shown significant progress to meet this challenge.[2] Enormous progress has been made in the DNA-guided organization of nanoparticles into discrete,[3] onedimensional,[4] two-dimensional,[5] and three-dimensional architectures.[6] Facile DNA-functionalization strategies for gold nanoparticles (AuNPs) are now available, making AuNPs preferred (easier) candidates for subsequent selfassembly to form higher-order structures. In contrast, the mediation by DNA self-assembly of the assembly of silver nanoparticles (AgNPs) into higher-order, well-defined discrete nanoarchitectures has not been well explored, mainly as a result of the relative instability of these systems. Ag undergoes oxidization more readily than Au; therefore, the conjugated ligands on the surface of AgNPs are more labile, and AgNPs tend to aggregate irreversibly in solutions with a high salt concentration. However, a high salt concentration is crucial for efficient DNA self-assembly. Recently, we and others started to address this problem by attaching multiple sulfur moieties to DNA [4c] to form stable AgNP–DNA conjugates that resist aggregation in buffers with a high salt concentration.[7]Herein we report a bottom-up method for the fabrication of discrete, well-ordered AgNP nanoarchitectures on selfassembled DNA origami structures of triangular shape by using AgNPs (20 nm in diameter) conjugated with chimeric phosphorothioated DNA (ps-po DNA) as building blocks. Discrete monomeric, dimeric, and trimeric AgNP structures and a AgNP–AuNP hybrid structure could be constructed reliably in high yield. We demonstrate that the center-tocenter distance between adjacent AgNPs can be precisely tuned from 94 to 29 nm, whereby the distance distribution is limited by the size distribution of the nanoparticles. DNA-origami technology [8] is a well-developed method to create fully addressable DNA nanostructures by using approximately 200 short staple DNA strands to fold a single-stranded genomic DNA (eg the DNA of M13mp18, 7249 nucleotides long) into geometrically defined nanopatterns. In this study, we exploited the organizational power of DNA origami to develop a robust strategy for the assembly of otherwise hard-to-control AgNPs into well-defined nano-