利用金属纳米晶体等离激元效应实现光驱动有机反应
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摘要
鉴于化石能源的过度开采和逐渐枯竭,太阳能的高效利用已日益引起业界的广泛关注。传统的利用太阳能是基于半导体的光电转换。除此之外,通过催化反应实现太阳能向化学能的转化是一个具有巨大潜力的路径,有望可以替代现有的传统热催化方法。我们设计并一步合成了尺寸为50纳米且具有内凹型结构的金属钯纳米晶体。通过结构对称性的降低和颗粒尺寸的增大使其能够在可见光宽谱范围内吸光,吸光后的光热效应足以为有机加氢反应提供热源。基于表面等离激元特性,该纳米结构的尖端棱角处具有局部高温,同时棱角处恰恰也是加氢反应的高活性位点,实现了太阳能利用和催化活性在空间分布上的合二为一。基于该设计,这内凹型结构金属钯纳米结构可以在室温光谱辐照下达到热反应70摄氏度下的催化转化效率。这一工作揭示了金属纳米光催化剂在光辐照下对催化反应体系带来的内在影响,也为高效催化剂的设计具有推动作用。~([1,2])
The efficient transformation of solar energy in multiple pathways has received wide interest due to the increasing energy concerns. In addition to photo-electric transformation, another potential pathway is light-driven catalytic reactions in chemistry. Based on plasmon excitation, catalytic reactions are accelerated through both plasmonic catalysis and photothermal conversion. We report here that the light in UV-to-visible range can be harvested for hydrogenation reaction using the one-pot synthesized Pd plasmonic nanostructures. Under the illumination of UV and visible light, hydrogenation reaction can be driven to different extent by altering light intensity at room temperature. This unique feature suggests that plasmonic nanostructures could be useful in many heterogeneous catalytic reactions by harvesting solar energy instead of heating. The results presented here contribute to the fundamental understanding on light-driven catalytic reactions in chemistry and provide insight for further catalysts design.
引文
[1]Long,R.,Z.Rao,K.Mao,Y.Li,C.Zhang,Q.Liu,C.Wang,Z.Y.Li,X.Wu,Y.Xiong;Angew.Chem.Int.Ed.Engl.2014,54,2425.
    [2]Long,R.,Y.Li,L.Song,Y.Xiong;Small 2015,11,3873.

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