从二维纳米片薄膜中控制释放分子嵌入剂,ACS Nano

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从二维纳米片薄膜中控制释放分子嵌入剂
ACS Nano ( IF 15.8 ) Pub Date : 2021-12-06 , DOI: 10.1021/acsnano.1c07888
Muchun Liu ₁ , Deisy C Carvalho Fernandes ₂ , Zachary S S L Saleeba ₂ , Robert H Hurt ₂

Affiliation

二维（2D）纳米片与化学溶质的溶液共沉积产生纳米片-分子异质结构。这些宏观层状杂化物的一个特征是它们能够释放插入的分子试剂以在其表面或附近环境中表达化学功能。需要系统的设计方法来控制这种分子释放，以匹配特定应用中对速率和寿命的需求。我们假设释放动力学受层状固体内的传输过程控制，这主要涉及通过层间范德华间隙形成的纳米通道的受限分子扩散。在这里，制造了各种氧化石墨烯 (GO)/分子杂化物，并经过瞬态实验来表征释放动力学、位置和机制。各种薄膜类型的Z方向扩散系数。由于纳米通道的限制和蛇形路径效应，扩散系数比游离溶液中的扩散系数低 8 个数量级，这种延迟是二维材料在有用的时间尺度上控制和延长释放的能力的基础。通过压缩起皱或起皱对异质结构薄膜进行平面内纹理化是一种有用的设计工具，可用于控制给定薄膜类型和分子插层剂的释放速率。通过对化学杀病毒剂的控制释放的案例研究证明了这种方法的潜力。

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Controlled Release of Molecular Intercalants from Two-Dimensional Nanosheet Films

Solution co-deposition of two-dimensional (2D) nanosheets with chemical solutes yields nanosheet–molecular heterostructures. A feature of these macroscopic layered hybrids is their ability to release the intercalated molecular agent to express chemical functionality on their surfaces or in their near surroundings. Systematic design methods are needed to control this molecular release to match the demand for rate and lifetime in specific applications. We hypothesize that release kinetics are controlled by transport processes within the layered solids, which primarily involve confined molecular diffusion through nanochannels formed by intersheet van der Waals gaps. Here a variety of graphene oxide (GO)/molecular hybrids are fabricated and subject to transient experiments to characterize release kinetics, locations, and mechanisms. The measured release rate profiles can be successfully described by a numerical model of internal transport processes, and the results used to extract effective Z-directional diffusion coefficients for various film types. The diffusion coefficients are found to be 8 orders of magnitude lower than those in free solution due to nanochannel confinement and serpentine path effects, and this retardation underlies the ability of 2D materials to control and extend release over useful time scales. In-plane texturing of the heterostructured films by compressive wrinkling or crumpling is shown to be a useful design tool to control the release rate for a given film type and molecular intercalant. The potential of this approach is demonstrated through case studies on the controlled release of chemical virucidal agents.

更新日期：2021-12-28

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