Quantitative Analysis of DNA-Mediated Formation of Metal Nanocrystals.
Quantitative Analysis of DNA-Mediated Formation of Metal Nanocrystals.
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DNA介导的金属纳米晶体形成的定量分析。
DOI：
10.1021/jacs.0c08604
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发表时间：
2020-11-18
影响因子：
15
通讯作者：
Lu, Yi
中科院分区：
文献类型：
--
作者：
Wang, Yiming;Counihan, Michael J.;Lin, Jeffrey Wayjer;Rodriguez-Lopez, Joaquin;Yang, Hong;Lu, Yi
具有所需结构的金属纳米晶体的预测合成依赖于对晶体形成过程的精确控制。使用封端配体是影响金属离子还原和纳米晶体形成的有效方法。然而，使用传统的封端配体很难实现预测合成纳米结构。 DNA作为一类有前景的生物分子加帽配体，已被用于在各种金属纳米晶体中产生序列特异性形态。然而，由于缺乏定量实验证据，对 DNA 介导的纳米晶体形成的机制了解仍然难以捉摸。在此，我们定量分析了 DNA 对 Ag+ 还原的精确控制以及所得 Au-Ag 核壳纳米晶体的结构。我们推导出 DNA 和 Ag+ 之间的平衡结合常数、序列特异性 Ag+ 还原途径的动力学速率常数，以及 DNA 钝化后纳米晶体上保留的活性表面位点的百分比。这三个协同因素在热力学和动力学上影响成核和生长过程，从而促进了用不同DNA序列合成的Au-Ag纳米晶体的形态演化。这项研究证明了使用功能性 DNA 序列作为多功能且可调节的封端配体系统来预测金属纳米结构合成的潜力。
The predictive synthesis of metal nanocrystals with desired structures relies on the precise control of the crystal formation process. Using a capping ligand is an effective method to affect the reduction of metal ions and the formation of nanocrystals. However, predictively synthesizing nanostructures has been difficult to achieve using conventional capping ligands. DNA, as a class of the promising biomolecular capping ligands, has been used to generate sequence-specific morphologies in various metal nanocrystals. However, mechanistic insight into the DNA-mediated nanocrystal formation remains elusive due to the lack of quantitative experimental evidence. Herein, we quantitatively analyzed the precise control of DNA over Ag+ reduction and the structures of resulting Au–Ag core–shell nanocrystals. We derived the equilibrium binding constants between DNA and Ag+, the kinetic rate constants of sequence-specific Ag+ reduction pathways, and the percentage of active surface sites remaining on the nanocrystals after DNA passivation. These three synergistic factors influence the nucleation and growth process both thermodynamically and kinetically, which contributed to the morphological evolution of Au–Ag nanocrystals synthesized with different DNA sequences. This study demonstrates the potential of using functional DNA sequences as a versatile and tunable capping ligand system for the predictable synthesis of metal nanostructures.
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影响因子：
15
作者：
Langille, Mark R.;Personick, Michelle L.;Mirkin, Chad A.
通讯作者：
Mirkin, Chad A.
影响因子：
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作者：
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通讯作者：
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作者：
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通讯作者：
Davey, WP
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作者：
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通讯作者：
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通讯作者：
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