Rapidly Adaptive All-covalent Nanoparticle Surface Engineering.
Rapidly Adaptive All-covalent Nanoparticle Surface Engineering.
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快速自适应全共价纳米粒子表面工程。
DOI：
10.1002/chem.202101042
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发表时间：
2021-07-07
期刊：
影响因子：
--
通讯作者：
Kay ER
中科院分区：
文献类型：
--
作者：
Diez-Castellnou M;Suo R;Marro N;Matthew SAL;Kay ER
新兴的纳米技术要求纳米级组件的操作具有相同的可预测性和可编程性，这在分子合成方法学中被认为是理所当然的。然而，在纳米材料表面上安装适当的反应性化学功能之前需要在反应性范围、功能化密度或两者方面进行妥协。在这里，我们介绍了一种理想化的动态共价纳米粒子构建块，用于胶体纳米材料的发散和自适应合成后修饰。缩醛保护的单层稳定的金纳米颗粒通过操作简单的方案制备，并且长期储存稳定。反应性醛官能团的可调表面密度可按需显示，从而从一个纳米级合成子中获得广泛的自适应表面工程选择。分子精度，界面反应动力学和动态表面组成可以原位探测在合奏水平分析听话。 高功能化密度与快速平衡动力学相结合，使环境适应性的表面组成和快速的纳米粒子性能切换响应简单的化学效应。乙缩醛封端的表面配体稳定理想化的胶体纳米颗粒构建块。在温和的条件下，通过精确的化学计量控制，按需活化被掩蔽的醛官能团，揭示了全共价合成后表面工程的通用平台。表面上的动态共价转化导致了不同的结构和功能修饰，包括快速适应环境的纳米材料。
Emerging nanotechnologies demand the manipulation of nanoscale components with the same predictability and programmability as is taken for granted in molecular synthetic methodologies. Yet installing appropriately reactive chemical functionality on nanomaterial surfaces has previously entailed compromises in terms of reactivity scope, functionalization density, or both. Here, we introduce an idealized dynamic covalent nanoparticle building block for divergent and adaptive post‐synthesis modification of colloidal nanomaterials. Acetal‐protected monolayer‐stabilized gold nanoparticles are prepared via operationally simple protocols and are stable to long‐term storage. Tunable surface densities of reactive aldehyde functionalities are revealed on‐demand, leading to a wide range of adaptive surface engineering options from one nanoscale synthon. Analytically tractable with molecular precision, interfacial reaction kinetics and dynamic surface constitutions can be probed in situ at the ensemble level. High functionalization densities combined with rapid equilibration kinetics enable environmentally adaptive surface constitutions and rapid nanoparticle property switching in response to simple chemical effectors. Acetal‐terminated surface ligands stabilize idealized colloidal nanoparticle building blocks. On‐demand activation of the masked aldehyde functionality occurs rapidly under mild conditions with precise stoichiometric control, revealing a versatile platform for all‐covalent post‐synthesis surface engineering. On‐surface dynamic covalent transformations lead to diverse structural and functional modifications including rapidly adaptive environment‐responsive nanomaterials.
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