Unraveling Surface Plasmon Decay in Core-Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis
Unraveling Surface Plasmon Decay in Core-Shell Nanostructures toward Broadband Light-Driven Catalytic Organic Synthesis
复制标题
揭示核壳纳米结构中的表面等离子体衰变以实现宽带光驱动催化有机合成
DOI：
10.1021/jacs.6b02532
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发表时间：
2016-06-01
影响因子：
15
通讯作者：
Xiong, Yujie
中科院分区：
文献类型：
--
作者：
Huang, Hao;Zhang, Lei;Xiong, Yujie
利用表面等离子体（金属）纳米结构来促进催化有机合成在太阳能到化学能的转换方面具有广阔的前景：高转换效率不仅依赖于拓宽吸收光谱，而且依赖于将收集的能量耦合到化学反应中。这种耦合在表面等离激元衰变过程中经历热电子转移和光热转换；然而，不幸的是，这两种等离激元效应是纠缠的——它们各自的作用仍在争论中，在这里，我们报告说，在双金属金-钯核壳纳米结构的模型系统中，这两种效应可以通过定制壳厚度来解开。 a（“原子级精度。正如我们的超快吸收光谱表征所证明的那样，“Pd催化有机氢化的三极管反应中两种效应的可调谐性为增强能量耦合提供了一个旋钮。此外，条形纳米结构中400--/00和cI700-100（）nm处的两种固有等离子体模式允许 表彰其在全太阳光谱中很大程度上利用“光子”。这项工作为设计等离子体催化纳米材料以增强太阳能到化学能的转换提供了范例指导。
Harnessing surface plasmon- of metal) nanostructuresto ptomote 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 entangleckmaking-Aeir inditdual roles still under debate, Here, we report that in a,model system of bituetallic Au-Pd core shell nanostructures the two effects- can be.disentangled through tailoring the,shell thickness a("atomictevel precision. As demonsttated by our ultrafast absorption spectroscoPy. characterizations, the achieved tunability of the two effects in a triode' reaction of "Pd-catalyzed organic hydrogenation offers a knob for enhancing energy Coupling. In addition, the two intrinsic plasmonic modes at 400--/00 ancI700-100() nm in the bar-shaped nanostructures allow for utilizing "photons td-a-large extent in full Solar spectrum. This work establishes a paradigmatic guidance toward designihg plasmonic-catalytic nanomaterials for enhanced solar-to-chemical energy conversion.