Autocatalytic Nucleation and Self-Assembly of Inorganic Nanoparticles into Complex Biosimilar Networks

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Connor N. McGlothin, Kody G. Whisnant, Emine Sumeyra Turali Emre, Dickson Owuor, Jun Lu, Xiongye Xiao, Drew Vecchio, Scott Van Epps, Paul Bogdan, Nicholas Kotov
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Abstract

Self-replication of bioorganic molecules and oil microdroplets have been explored as models in prebiotic chemistry. An analogous process for inorganic nanomaterials would involve the autocatalytic nucleation of metal, semiconductor, or ceramic nanoparticles-an area that remains largely uncharted. Demonstrating such systems would be both fundamentally intriguing and practically relevant, especially if the resulting particles self-assemble into complex structures beyond the capabilities of molecules or droplets. Here, we show that autocatalytic nucleation occurs with silver nanoparticles, which subsequently self-assemble into chains through spatially restricted attachment. In dispersions containing “hedgehog” particles, these reactions produce complex colloids with hierarchical spike organization. On solid surfaces, autocatalytic nucleation of nanoparticles yields conformal networks with hierarchical organization, including nanoparticle “colonies.” We analyzed the complexity of both types of solid-stabilized particle assemblies via graph theory (GT). The complexity index of idealized spiky colloids is comparable to that of complex algal skeletons. The GT analysis of the percolating nanoparticle networks revealed their similarities to the bacterial, but not fungal, biofilms. We conclude that coupling autocatalytic nucleation with self-assembly enables the generation of complex, biosimilar particles and films. This work establishes mathematical and structural parallels between biotic and abiotic matter, integrating self-organization, autocatalytic nucleation, and theoretical description of complex systems. Utilization of quantitative descriptors of connectivity patterns opens possibility to GT-based biomimetic engineering of conductive coatings and other complex nanostructures.

Abstract Image

无机纳米颗粒在复杂生物类似物网络中的自催化成核和自组装
分子和微滴的自我复制已被探索作为益生元化学的模型。无机纳米材料的类似过程涉及纳米粒子的自催化成核,这是一个很大程度上未知的领域。演示这样的系统将从根本上吸引人,并具有实际意义,特别是如果产生的粒子能够自我组装。在这里,我们证明了自组装的自催化成核偶与银纳米粒子发生。在含有“刺猬”颗粒的分散体中,这些反应产生具有分层刺状组织的复杂胶体。在固体表面,纳米颗粒的自催化成核产生具有层次组织的保形网络,包括纳米颗粒“菌落”。我们利用图论分析了这两种固体稳定粒子组合的复杂性。理想化的尖状胶体的复杂性指数与复杂的藻类骨架的复杂性指数相当。渗透纳米颗粒网络的GT分析揭示了它们与细菌生物膜的相似性,而不是真菌生物膜。我们得出的结论是,将自催化成核与自组装耦合可以生成复杂的、生物类似的颗粒和膜。这项工作建立了生物和非生物物质之间的数学和结构相似性,整合了自组织、自催化成核和复杂系统的理论描述。利用连接模式的定量描述符为导电涂层和其他复杂纳米结构的基于gts的仿生工程提供了可能性。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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