期刊
NANO LETTERS
卷 18, 期 11, 页码 7289-7297出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b03499
关键词
Plasmonic catalysis; nanorattles; platinum; selectivity; visible light; hydrogenation
类别
资金
- FAPESP [2015/21366-9, 2015/26308-7, 2016/16738-7, 2016/17866-9, 2017/07564-8, 2015/11452-5]
- Serrapilheira Institute [Serra-1709-16900]
- CNPq [422647/2016-0]
- Coordenacao de Aperfeicoamento de Pessoal de Nivel Superior - Brazil (CAPES) [001]
- CAPES
- NASA EPSCoR Grant [NNX16A-Q97A]
- Engineering and Physical Sciences (U.K.) [EP/M010619/1, EP/P009050/1]
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme [ERC-2016-STG-EvoluTEM-715502]
- Fundacao de Amparo a Pesquisa do Estado de Sao Paulo (FAPESP) [16/16738-7, 17/07564-8] Funding Source: FAPESP
- EPSRC [EP/P009050/1, EP/M010619/1, EP/P025021/1] Funding Source: UKRI
The localized surface plasmon resonance (LSPR) excitation in plasmonic nanoparticles has been used to accelerate several catalytic transformations under visible-light irradiation. In order to fully harness the potential of plasmonic catalysis, multimetallic nanoparticles containing a plasmonic and a catalytic component, where LSPR-excited energetic charge carriers and the intrinsic catalytic active sites work synergistically, have raised increased attention. Despite several exciting studies observing rate enhancements, controlling reaction selectivity remains very challenging. Here, by employing multimetallic nanoparticles combining Au, Ag, and Pt in an Au@Ag@Pt core-shell and an Au@AgPt nanorattle architectures, we demonstrate that reaction selectivity of a sequential reaction can be controlled under visible light illumination. The control of the reaction selectivity in plasmonic catalysis was demonstrated for the hydrogenation of phenylacetylene as a model transformation. We have found that the localized interaction between the triple bond in phenylacetylene and the Pt nanoparticle surface enables selective hydrogenation of the triple bond (relative to the double bond in styrene) under visible light illumination. Atomistic calculations show that the enhanced selectivity toward the partial hydrogenation product is driven by distinct adsorption configurations and charge delocalization of the reactant and the reaction intermediate at the catalyst surface. We believe these results will contribute to the use of plasmonic catalysis to drive and control a wealth of selective molecular transformations under ecofriendly conditions and visible light illumination.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据