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Ternary PtNiCu self-assembled nanocubes for plasmon-enhanced electrocatalytic hydrogen evolution and methanol oxidation reaction in visible light
摘要： The strong interaction among metal components results in the change of the electronic structure (e.g. d-band energy level) of noble metal-based alloy structures which enables the increase of catalytic activity. In this paper, self-assembled ternary PtNiCu and binary PtCu alloy nanocubes are synthesized by a one-pot high-temperature chemical reduction method. The growth mechanism of the alloy is investigated. The alloy is applied to visible light-assisted electrocatalytic hydrogen production and methanol oxidation. The ternary PtNiCu alloy exhibits superior catalytic performance (a minimum over potential of 15 mV at a current density of 10 mA cm-2, a Tafel slope of 24.1 mV/dec, and more excellent mass specific activity under visible light irradiation about 3.3 A mgPt -1), because of its regular morphology, more surface active sites, and more intense interaction between metal elements. Especially the localized surface plasmon resonance effect of Cu largely increases the electron density (photoelectric effect) on Pt under illumination, thereby further improves the photo-assisted hydrogen production and methanol catalytic oxidation performance. The results will promote efficient and accurate electrocatalysis process, paving new way for a brighter further in rational design of ternary plasmonic electrocatalysts and photoelectrocatalysis field.
关键词： Methanol oxidation reaction,Photoelectrocatalysis,Hydrogen evolution reaction,Ternary PtNiCu alloy
更新于2025-09-23 15:21:01
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Polyaniline supported g-C3N4 quantum dots surpass benchmark Pt/C: Development of morphologically engineered g-C3N4 catalysts towards a??metal-freea?? methanol electro-oxidation
摘要： In spite of being one of the most promising energy conversion devices, the state of the art in the efficient application of direct methanol fuel cell is far from being optimal mostly because of its heavy reliance on expensive Pt anode that suffers from easy CO poisoning. Here, in this work for the first time in literature, we have explored the catalytic efficacy and improved mass activity of morphologically engineered metal-free graphitic carbon nitride towards methanol oxidation. The 2D nano-sheets, 1D nano-rods, and 0D quantum dots of graphitic carbon nitride are successfully prepared from bulk by a thermo-chemical etching process. The materials are thoroughly characterized with the help of X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, field emission scanning electron microscopy, transmission electron microscopy, luminescence study and are studied for methanol oxidation reaction in basic condition with the help of cyclic voltammetry. Among the three different dimensional g-C3N4 materials, the quantum dots show higher methanol oxidation activity due to its abundant edges in nano morphology and maximum atomic percentages of active site of pyridinic N. The 0D g-C3N4 when supported on conducting polyaniline, not only shows higher electrocatalytic methanol oxidation activity than the commercial Pt/C but also demonstrates excellent CO tolerance to be a suitable and applicable metal-free anode catalyst in direct methanol fuel cell applications. The electrostatic interaction between 0D g-C3N4 and conducting polyaniline (PANI) fibres may have improved the electrical conductivity and methanol adsorption of CNQD-PANI electrocatalyst and also played a role in oxidizing the adsorbed CO to upsurge the CO tolerance.
关键词： Nano-rods,Metal-free electrocatalysis,Methanol oxidation reaction,Quantum dots,g-C3N4,Nano-sheets
更新于2025-09-19 17:13:59
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Free-standing nanoporous gold for direct plasmon enhanced electro-oxidation of alcohol molecules
摘要： 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 μA 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.
关键词： localized surface plasmon resonance,methanol oxidation reaction,nanoporous gold,electrocatalysis,Schottky barriers-free
更新于2025-09-11 14:15:04