Chem. J. Chinese Universities ›› 2020, Vol. 41 ›› Issue (12): 2788.doi: 10.7503/cjcu20200512

• Physical Chemistry • Previous Articles     Next Articles

Preparation of Platinum-modified Uniform Gold Nanopillar Electrodes and Photoelectrocatalytic Oxidation of Methanol

SUN Weixin, LIU Jia, WANG Jiazheng, ZHANG Yimiao, JIN Lei, ZHOU Jianzhang, YANG Fangzu(), WU Deyin(), TIAN Zhongqun   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces,Department of Chemistry,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China
  • Received:2020-07-31 Online:2020-12-10 Published:2020-12-09
  • Contact: WU Deyin E-mail:fzyang@xmu.edu.cn;dywu@xmu.edu.cn
  • Supported by:
    ? Supported by the National Natural Science Foundation of China(21533006)

Abstract:

Surface plasmons(SPs) excitation in nanostructured noble metals has been shown to effectively accelerate and drive photochemical reactions. Methanol, as an important alcohol fuel, has the characteristics of high energy density, wide source, low price and convenient storage. It can be used as a raw material in direct methanol fuel cell(DMFC). At present, studies have shown that surface plasmon resonance(SPR) can effectively enhance the oxidation efficiency of methanol. However, most of the current composite catalysts are core-shell structure nanoparticles, and their stability and repeatability have become a problem to be overcome, especially the thickness of the catalytic metal on the surface of the core-shell structure is not uniform and difficult to control, which has caused many uncertainties in the study of plasmon-catalyzed methanol oxidation. Therefore, this paper uses thermal lithography and ultraviolet lithography to prepare a hole array on photoresist coated glass electrode substrate with a period of 450 nm. Gold nanopillars were uniformly grown in the electrode holes with a constant current electrodeposition technique in gold sodium sulfite solution until the holes were completely filled, and a gold nanopillar array structure with a height of about 180 nm and a diameter of about 200 nm was obtained. Combined with gas phase deposition technology, a nano-Au/Pt electrode with ordered structure, uniform hot spots and large-scale production was obtained. With finite element method(FEM) analysis, the visible light absorption peaks of Au/Pt electrodes with different thicknesses and their correspon-ding electric field modes were simulated, which, combined with experimental results, proved that the electrodes have three plasmon excitation modes, including SPR at the bottom of the column and the gold film, the surface plasmon polariton(SPP) coupling on the gold film which blue-shifted when the thickness of Pt increa- ses, and the SPR coupling on the top of the nanopillar. Finally, the electrocatalytic performance of this electrode on methanol oxidation reaction under illuminations was studied, and proved that 2 nm Au/Pt has the best oxidation effect. In the 30 mA constant current oxidation of methanol experiment, light can prolong the lifetime of the electrode about 6 times, and the SPR effects help electrode surface to have a self-cleaning effect.

Key words: Nanoimprint, Electrodeposition, Surface plasmon resonance, Methanol, Photoelectric catalysis

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