Unraveling Surface Plasmon Decay in Core–Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis

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• 作者：Hao Huang ; Lei Zhang ; Zhiheng Lv ; Ran Long ; Chao Zhang ; Yue Lin ; Kecheng Wei ; Chengming Wang ; Lu Chen ; Zhi-Yuan Li ; Qun Zhang ; Yi Luo ; Yujie Xiong
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：June 1, 2016
• 年：2016
• 卷：138
• 期：21
• 页码：6822-6828
• 全文大小：451K
• 年卷期：0
• ISSN：1520-5126

文摘

Harnessing surface plasmon of metal nanostructures to promote catalytic organic synthesis holds great promise in solar-to-chemical energy conversion. High conversion efficiency relies not only on broadening the absorption spectrum but on coupling the harvested energy into chemical reactions. Such coupling undergoes hot-electron transfer and photothermal conversion during the decay of surface plasmon; however, the two plasmonic effects are unfortunately entangled, making their individual roles still under debate. Here, we report that in a model system of bimetallic Au–Pd core–shell nanostructures the two effects can be disentangled through tailoring the shell thickness at atomic-level precision. As demonstrated by our ultrafast absorption spectroscopy characterizations, the achieved tunability of the two effects in a model reaction of Pd-catalyzed organic hydrogenation offers a knob for enhancing energy coupling. In addition, the two intrinsic plasmonic modes at 400–700 and 700–1000 nm in the bar-shaped nanostructures allow for utilizing photons to a large extent in full solar spectrum. This work establishes a paradigmatic guidance toward designing plasmonic–catalytic nanomaterials for enhanced solar-to-chemical energy conversion.