Chen Tao, Tong Fengxia, Enderlein Jörg, Zheng Zhaoke
III. Institute of Physics - Biophysics, Georg August Universität, Friedrich-Hund-Platz 1, 37077 Göttingen, Germany.
State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, China.
Nano Lett. 2020 May 13;20(5):3326-3330. doi: 10.1021/acs.nanolett.0c00206. Epub 2020 Apr 24.
Understanding the underlying kinetic mechanism of plasmon-enhanced catalysis is important for designing optimized bimetal nanostructures. Here, we characterize product formation rate at both the single-particle and ensemble level. The single-particle measurement allows us to reveal the underlying catalytic kinetic mechanisms of a bimetal nanostructure. Combining this with ensemble observations of two different catalytic behaviors of this catalyst with and without illumination shows that energetic charge carriers induce a transition from a competitive reactant adsorption type to a noncompetitive adsorption type, which leads to the suppression of catalytic rate decay at high reactant concentration. Theoretical modeling as well as analysis of hole acceptability of scavengers on Pt and Au surfaces indicates that the Pt light absorptivity is enhanced near Au and the energetic charges may form directly from the Pt part of the Au-Pt nanostructure. The presented study deepens our understanding of plasmon-enhanced catalysis by bimetal nanostructures.
理解等离子体增强催化的潜在动力学机制对于设计优化的双金属纳米结构至关重要。在此，我们在单粒子和整体水平上表征产物形成速率。单粒子测量使我们能够揭示双金属纳米结构的潜在催化动力学机制。将此与对该催化剂在有光照和无光照情况下两种不同催化行为的整体观察相结合，表明高能电荷载流子会引发从竞争性反应物吸附类型到非竞争性吸附类型的转变，这导致在高反应物浓度下催化速率衰减受到抑制。理论建模以及对清除剂在铂和金表面的空穴接受性分析表明，铂在金附近的光吸收率增强，并且高能电荷可能直接从金 - 铂纳米结构的铂部分形成。本研究加深了我们对双金属纳米结构等离子体增强催化的理解。
