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Free-standing nanoporous gold for direct plasmon enhanced electrooxidation of alcohol molecules

机译:用于直接等离子体的独立纳米多孔金增强了酒精分子的电氧化

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Localized surface plasmon resonance (LSPR) excitation enhanced chemical and electrochemical reactions represent a promising pathway for solar-to-chemical energy conversion. However, plasmonic catalysts usually suffer from low collection efficiency of hot charge carries generated by LSPR excitation due to short lifetime of hot carriers and fast electron-hole recombination. Schottky barriers between plasmonic catalysts and semiconducting supports have been utilized to prevent the electron-hole recombination. However, the interfacial barriers also hinder low-energy hot charge collection and thus affect solar-to-chemical energy conversion efficiency. Here we report that bicontinuous nanoporous gold as a Schottky barriers-free direct plasmonic catalyst can significantly enhance electro-oxidation of alcohol molecules. A high energetic hole yield of 0.486% is achieved, which is 4 times higher than that of discrete plasmonic AuAg nanoparticles. The direct plasmonic catalyst offers the highest methanol oxidation current density of 531 mu A cm(-2) among all known Au catalysts. This work provides compelling evidence that higher hot carrier collection efficiency can be achieved from direct plasmonic electrocatalysis without the assistance of Schottky junctions and has important implications in developing high efficiency plasmonic catalysts for photo-enhanced electrochemical reactions.
机译:局部表面等离子体共振(LSPR)激发增强的化学和电化学反应代表了太阳能 - 化学能量转换的有望途径。然而,由于热载体的短寿命和快速电子 - 空穴重组,因此等离子体催化剂通常由于LSPR激发产生的热电荷的低收集效率。已经利用了等离子体催化剂和半导体支撑件之间的肖特基屏障来防止电子孔重组。然而,界面屏障也阻碍了低能量热电荷收集,从而影响了太阳能化学能量转换效率。在这里,我们报告说,作为无肖特基障碍的直接等离子体催化剂可以显着增强醇分子的电氧化的双孔纳米多孔金。实现了0.486%的高能量孔产率,这是比离散等离子体Auag纳米颗粒高的4倍。直接等离子体催化剂在所有已知的Au催化剂中提供531μm(-2)的最高甲醇氧化电流密度。这项工作提供了令人信服的证据,即在没有肖特基结的情况下,可以从直接等离子体电催化效率实现更高的热载流子收集效率,并且在开发用于光增强电化学反应的高效率等离子体催化剂方面具有重要意义。

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