表面等离子体共振效应在光电催化中的应用及机理研究

Application of Surface Plasma Resonance Effect in Photoelectrocatalysis and Mechanism Study

面对日益严峻的能源和环境问题,人们对可再生能源的需求日益增强。本文通过以金为核的二元及三元纳米粒子,设计了一种表面等离子体共振(surface plasmonic resonance,SPR)增强的光电催化剂。其中,金核通过SPR效应在光照下产生光热效应及光电效应,提高了材料的催化活性。光照条件下纳米粒子表面的局域热点温度可以通过4-甲氧基异腈苯探针分子利用表面增强拉曼光谱得到。同时利用对氨基苯硫酚(PATP)探针分子证实SPR产生的光电催化效应。最重要的是,通过定量计算得到了光热效应及光电效应在SPR增强的光电催化性能各自的贡献。这些结果为表面等离子体共振协助增强的光电催化反应提供理论依据,并为新型光电催化材料提供了新的设计思路。

The need for alternative energy sources is growing stronger due to the increasing energy demand and environmental concerns.Here we designed the surface plasmon resonance(SPR)promoted solar fuel cells by tailoring a Au core Pd shell Pt mushroom structure nanoparticles to enhance the catalytic activity of the direct methanol fuel cells(DMFCs).The combination of the Pd and Pt provides a synergistic effect while the Au core provides the photothermal and photoelectrocatalytic effect by SPR under irradiation to enhance the catalytic activity of the electrooxidation of methanol.A complex synergistic effect is achieved by using all three metals in combination,and the whole is greater than the sum of its parts.The temperature on the nanoparticle surface after illumination are detected by surface-enhanced Raman scattering(SERS)with a probe molecule of 4-methoxyphenyl isocyanide.The photoelectrocatalytic effect generated from SPR is proved by SERS with a probe molecule of p-aminothiophenol(PATP).Most importantly,the quantitative calculation of the ratio of the photothermal and photoelectrocatalysis effect contributed to the catalytic activity is realized.These results provide a novel design of catalysts for the solar fuel cells based on the SPR effect.