原子精确纳米银簇基三维框架材料的设计合成及其基于SERS信号的环境示踪

基于结构美学及其在发光、传感等领域的潜在应用，晶态纳米银簇日益引起广泛关注；深入探索新颖结构及其具有实用价值的功能特性，无疑是该领域纵深发展的核心热点。本项目设计合成系列原子精确的纳米银簇基多孔框架化合物(3DAgNF)，利用合适的还原手段得到具有规则排列的银原子掺杂纳米隙，从而赋予材料表面增强拉曼散射(SERS)活性。探索系列3DAgNF化合物的最佳合成策略，总结3DAgNF结构及还原条件对纳米隙数量和有序性的影响规律，揭示3DAgNF结构与SERS信号增强的构效关系。利用3DAgNF还原材料中银原子团对光、热、氧化还原等环境的敏感性，实现其基于SERS的环境示踪功能；并将具有不同敏感性的3DAgNF材料合理组合，制备出多因素SERS示踪标签。本项目首次提出基于SERS信号的环境示踪理念，拓展了三维纳米银簇基材料的应用空间，为示踪技术应用于存储、防伪、药品食品监控等提供全新的技术途径。

Based on structural aesthetics and its potential applications in the fields of luminescence and sensor, crystalline silver(I) nanoclusters have attracted much attention. The in-depth exploration of novel structures and their functions of practical value is undoubtedly the core of the further development in this field. In this project, a series of silver(I) nanocluster based porous framework compounds (3DAgNF) with atom-precise were designed and synthesized. The Ag(0) atoms doped nano-gaps with regular arrangement were obtained by appropriate reduction methods, thus giving the surface enhanced Raman scattering (SERS) activity of the materials. The optimal synthetic strategy of a series of 3DAgNF compounds were explored. The effects of 3DAgNF structure and reduction conditions on the number and ordering of nano-gaps were summarized, and the structure-activity relationship between 3DAgNF structure and SERS signal enhancement was revealed. Using the sensitivity of reductive 3DAgNF materials to light, heat, redox and other environments, the environmental tracer function based on SERS was realized, and the multi-factor SERS tracer labels were prepared by reasonable combination of reductive 3DAgNF materials with different sensitivities. In this project, the concept of environmental tracer based on SERS signal is put forward for the first time, which expands the application of three-dimensional silver nanocluster based materials, and provides a new technical approach for the application of tracer technology in storage, anti-counterfeiting, drug and food monitoring and so on.