DNA-Functionalized Silver Nanoparticles in an Alcoholic Solvent for Environment-Dictated Multimodal Actuation
DNA-Functionalized Silver Nanoparticles in an Alcoholic Solvent for Environment-Dictated Multimodal Actuation
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DOI：
10.1021/acsanm.2c01493
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发表时间：
2022-07
影响因子：
5.9
通讯作者：
Linying Kong;Luyang Wang;Yali Shi;Lin Peng;Xingguo Liang;Guoqing Wang;Hideyuki Mitomo;T. Takarada;K. Ijiro;M. Maeda
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文献类型：
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作者：
Linying Kong;Luyang Wang;Yali Shi;Lin Peng;Xingguo Liang;Guoqing Wang;Hideyuki Mitomo;T. Takarada;K. Ijiro;M. Maeda
等离子体纳米致动器具有对不受控制环境的适应性，类似于生命系统，在以人为中心的机器人应用中具有重要意义，包括纳米机械、传感器和药物输送。实现这一挑战需要等离子体纳米粒子的智能配体功能化，以便在各种刺激下精细控制其排列。本研究表明，以聚丙烯酸（PAA）为钝化配体的双链dna官能化银纳米粒子（dsDNA- agnps）可以存储通过热、光或ph刺激释放的弹性能量。加热或光激发钝化末端堆叠诱导的dsDNA- agnps组件会导致dsDNA的末端打开和熵排斥以克服吸引力，重新抑制单个dsDNA- agnps。此外，pH变化导致PAA中羧基的电荷结合/解离，为dsDNA-AgNPs的受控驱动建立了一个静电力开关。为了适应环境驱动，我们提供了dsDNA- agnps根据温度或光照的变化来调节驱动的能力，基于醇调制的dsDNA末端碱基配对。这项研究代表了迈向完全环境可激活、自我维持的智能纳米系统的重要一步。
Plasmonic nanoactuators with adaptability to uncontrolled environments resemble living systems and have implications in human-centered robotic applications, including nanomachinery, sensors, and drug delivery. Realization of the challenge has necessitated smart-ligand functionalization of plasmonic nanoparticles for the fine control of their arrangement under varied stimuli. Here we show that double-stranded DNA-functionalized silver nanoparticles (dsDNA-AgNPs) bearing poly(acrylic acid) (PAA) as the passivating ligand can store elastic energy releasable through a stimulus of heat, light, or pH. Heating or light excitation to blunt end-stacking-induced assemblies of dsDNA-AgNPs causes terminal opening of the dsDNA and entropic repulsion to overcome the attraction force, repristinating individual dsDNA-AgNPs. Furthermore, a pH change results in charge association/dissociation of the carboxyl groups in PAA, setting up an electrostatic force switch for the controlled actuation of dsDNA-AgNPs. Toward adaptable environmental actuation, we furnish dsDNA-AgNPs with the ability to adjust the actuation in response to changing temperature or light irradiation, based on alcohol-modulated terminal base pairing of the dsDNA. The study represents an important step toward fully environment-activatable, self-sustained intelligent nanosystems.