State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, People's Republic of China.
Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials and Electron Microscopy Center, Jilin University, Changchun 130012, People's Republic of China.
Anal Chem. 2023 Mar 7;95(9):4335-4343. doi: 10.1021/acs.analchem.2c04548. Epub 2023 Feb 20.
In this work, three-dimensional (3D) Ag aerogel-supported Hg single-atom catalysts (SACs) were explored as an efficient surface-enhanced Raman scattering (SERS) substrate to monitor the enhanced oxidase-like reaction. The influence of the concentrations of Hg to prepare 3D Hg/Ag aerogel networks on their SERS properties to monitor the oxidase-like reaction has been investigated, and a specific enhancement with an optimized addition of Hg has been achieved. The formation of Ag-supported Hg SACs with the optimized Hg addition was identified from a high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) image and X-ray photoelectron spectroscopy (XPS) measurement at an atomic level. This is the first discovery of Hg SACs for enzyme-like reaction applications inferred by SERS techniques. And density functional theory (DFT) was used to further reveal the oxidase-like catalytic mechanism of Hg/Ag SACs. This study provides a mild synthetic strategy to fabricate Ag aerogel-supported Hg single atoms to display promising prospects in various catalytic fields.
在这项工作中，探索了三维（3D）Ag 气凝胶负载 Hg 单原子催化剂（SAC）作为一种有效的表面增强拉曼散射（SERS）基底，以监测增强的类氧化酶反应。研究了制备 3D Hg/Ag 气凝胶网络时 Hg 浓度对其 SERS 性质监测类氧化酶反应的影响，并通过优化 Hg 的添加实现了特定的增强。通过高角度环形暗场扫描透射电子显微镜（HAADF-STEM）图像和原子水平的 X 射线光电子能谱（XPS）测量，从原子水平上确定了具有优化 Hg 添加量的 Ag 负载 Hg SAC 的形成。这是首次通过 SERS 技术发现用于类酶反应应用的 Hg SAC。并且使用密度泛函理论（DFT）进一步揭示了 Hg/Ag SAC 的类氧化酶催化机制。这项研究提供了一种温和的合成策略，用于制备 Ag 气凝胶负载的 Hg 单原子，在各种催化领域显示出广阔的应用前景。
