Multimetallic Metasurfaces for Enhanced Electrocatalytic Oxidations in Direct Alcohol Fuel Cells
Multimetallic Metasurfaces for Enhanced Electrocatalytic Oxidations in Direct Alcohol Fuel Cells
复制标题
直接醇类燃料电池中用于增强电催化氧化的多金属超表面
DOI：
10.1002/lpor.202200137
复制
发表时间：
2022-04
影响因子：
11
通讯作者：
Rambabu Yalavarthi;O. Yesilyurt;Olivier Henrotte;Š. Kment;V. Shalaev;A. Boltasseva;A. Naldoni
中科院分区：
文献类型：
--
作者：
Rambabu Yalavarthi;O. Yesilyurt;Olivier Henrotte;Š. Kment;V. Shalaev;A. Boltasseva;A. Naldoni
等离子体超颖表面通过使用谐振单元或纳米天线的周期性排列来实现对光的前所未有的操纵。在这里，由自立式Ni/Au-Pt纳米结构膜制成的多金属超颖表面显示出显著增强直接醇燃料电池中采用的电催化氧化反应。Ni/Au超颖表面支持光子和等离子体模式，这些模式用于电磁热点内Pt电催化剂的位点选择性沉积，其中它们的反应性可以大大增加。增强的电催化活性的甲醇氧化反应（莫尔）主要归因于电子效应，由于激发的热电荷载流子和等离子体激元近场，支持电磁模拟和动力学同位素实验。波长依赖的光电化学研究表明，Ni/Au-Pt超颖表面在宽光谱范围内增强了莫尔比，并有利于不同的光诱导反应机制，这取决于所选择的能量窗口。
Plasmonic metasurfaces enable unprecedented manipulation of light by using periodic arrangement of resonant unit cells or nanoantennas. Here, multimetallic metasurfaces made of self‐standing Ni/Au‐Pt nanostructured films are shown to significantly enhance an electrocatalytic oxidation reaction employed in direct alcohol fuel cells. The Ni/Au metasurfaces support photonic and plasmonic modes, which are leveraged for the site‐selective deposition of Pt electrocatalysts within the electromagnetic hot spots, where their reactivity can be strongly increased. The enhanced electrocatalytic activity for the methanol oxidation reaction (MOR) is primarily attributed to electronic effects due to the excitation of hot charge carriers and plasmonic near fields, as supported by electromagnetic simulations and kinetic isotopic experiments. Wavelength‐dependent photoelectrochemical investigations suggest that Ni/Au‐Pt metasurfaces enhances MOR over a broad spectral range and favors different light‐induced reaction mechanisms depending on the selected energy window.