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Controlling energy flow in multimetallic nanostructures for plasmonic catalysis
Nature Nanotechnology ( IF 38.3 ) Pub Date : 2017-07-17 , DOI: 10.1038/nnano.2017.131
Umar Aslam , Steven Chavez , Suljo Linic

It has been shown that photoexcitation of plasmonic metal nanoparticles (Ag, Au and Cu) can induce direct photochemical reactions. However, the widespread application of this technology in catalysis has been limited by the relatively poor chemical reactivity of noble metal surfaces. Despite efforts to combine plasmonic and catalytic metals, the physical mechanisms that govern energy transfer from plasmonic metals to catalytic metals remain unclear. Here we show that hybrid core–shell nanostructures in which a core plasmonic metal harvests visible-light photons can selectively channel that energy into catalytically active centres on the nanostructure shell. To accomplish this, we developed a synthetic protocol to deposit a few monolayers of Pt onto Ag nanocubes. This model system allows us to conclusively separate the optical and catalytic functions of the hybrid nanomaterial and determine that the flow of energy is strongly biased towards the excitation of energetic charge carriers in the Pt shell. We demonstrate the utility of these nanostructures for photocatalytic chemical reactions in the preferential oxidation of CO in excess H2. Our data demonstrate that the reaction occurs exclusively on the Pt surface.



中文翻译:

控制多金属纳米结构中的能流以进行等离子体激元催化

已经表明,等离子体金属纳米颗粒(Ag,Au和Cu)的光激发可以诱导直接的光化学反应。然而,该技术在催化中的广泛应用受到贵金属表面相对较差的化学反应性的限制。尽管已努力将等离激元金属和催化金属结合起来,但控制从等离激元金属到催化金属的能量转移的物理机制仍不清楚。在这里,我们显示出混合的核-壳纳米结构,其中核心等离激元金属收集可见光光子,可以选择性地将能量引导到纳米结构壳上的催化活性中心。为实现此目的,我们开发了一种合成规程,可以在Ag纳米立方体上沉积一些单层Pt。该模型系统使我们能够最终分离杂化纳米材料的光学和催化功能,并确定能量流强烈偏向于Pt壳中高能电荷载流子的激发。我们展示了这些纳米结构在光催化化学反应中在过量H的CO优先氧化中的效用2。我们的数据表明,该反应仅在Pt表面上发生。

更新日期:2017-09-06
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