Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208, United States.
J Phys Chem Lett. 2020 Nov 5;11(21):9321-9328. doi: 10.1021/acs.jpclett.0c02640. Epub 2020 Oct 22.
Enzyme-mimicking inorganic nanoparticles, also known as nanozymes, have emerged as a rapidly expanding family of artificial enzymes that exhibit superior structural robustness and catalytic durability when serving as the surrogates of natural enzymes for widespread applications. However, the performance optimization of inorganic nanozymes has been pursued in a largely empirical fashion due to lack of generic design principles guiding the rational tuning of the nanozyme activities. Here we choose Au surface-roughened nanoparticles as a model plasmonic nanozyme that combines peroxidase-mimicking behaviors with tunable plasmonic characteristics to demonstrate the feasibility of fine-tuning nanozyme activities through plasmonic excitations using visible and near-infrared light sources. Taking full advantage of the unique plasmonic tunability offered by Au surface-roughened nanoparticles, we were able to unravel the detailed relationship between plasmonic excitations and nanozyme activities that underpins the hot electron-mediated working mechanism of peroxidase-mimicking plasmonic nanozymes.
酶模拟无机纳米粒子，也称为纳米酶，是一类新兴的人工酶，它们具有优越的结构稳定性和催化耐久性，可以作为天然酶的替代品，在广泛的应用中发挥作用。然而，由于缺乏通用的设计原则来指导纳米酶活性的合理调节，因此主要通过经验方法来优化无机纳米酶的性能。在这里，我们选择 Au 表面粗糙化纳米粒子作为模型等离子体纳米酶，它结合了过氧化物酶模拟行为和可调谐的等离子体特性，以证明通过使用可见和近红外光源的等离子体激发来精细调节纳米酶活性的可行性。充分利用 Au 表面粗糙化纳米粒子提供的独特等离子体可调性，我们能够揭示等离子体激发与纳米酶活性之间的详细关系，这是过氧化物酶模拟等离子体纳米酶的热电子介导工作机制的基础。
