Abstract
Gold–palladium (Au–Pd) bimetallic nanostructures with engineered plasmon-enhanced activity sustainably drive energy-intensive chemical reactions at low temperatures with solar simulated light. A series of alloy and core–shell Au–Pd nanoparticles (NPs) were prepared to synergistically couple plasmonic (Au) and catalytic (Pd) metals to tailor their optical and catalytic properties. Metal-based catalysts supporting a localized surface plasmon resonance (SPR) can enhance energy-intensive chemical reactions via augmented carrier generation/separation and photothermal conversion. Titania-supported Au–Pd bimetallic (i) alloys and (ii) core–shell NPs initiated the ethanol (EtOH) oxidation reaction under solar-simulated irradiation, with emphasis toward driving carbon–carbon (C–C) bond cleavage at low temperatures. Plasmon-assisted complete oxidation of EtOH to CO2, as well as intermediary acetaldehyde, was examined by monitoring the yield of gaseous products from suspended particle photocatalysis. Photocatalytic, electrochemical, and photoelectrochemical (PEC) results are correlated with Au–Pd composition and homogeneity to maintain SPR-induced charge separation and mitigate the carbon monoxide poisoning effects on Pd. Photogenerated holes drive the photo-oxidation of EtOH primarily on the Au-Pd bimetallic nanocatalysts and photothermal effects improve intermediate desorption from the catalyst surface, providing a method to selectively cleave C–C bonds.
Highlights
Published: 25 February 2021Efficient chemical transformations of readily available resources via light-energy conversion enables the generation of energy-dense fuels and electrical power [1,2,3]
Directed harvesting of solar energy can be facilitated by photocatalytic processes augmented by plasmon-mediated chemistry [3,4,5,6,7,8]
Gold–palladium bimetallic alloy nanoparticles (Au1−x Pdx NPs) were prepared with the compositions Au, Au0.9 Pd0.1, Au0.75 Pd0.25, Au0.5 Pd0.5, Au0.25 Pd0.75, Au0.1 Pd0.9, and plasmonic (Au) and catalytic (Pd) using a protocol reported in Reference [5]
Summary
Published: 25 February 2021Efficient chemical transformations of readily available resources (solar energy, water, waste products, etc.) via light-energy conversion enables the generation of energy-dense fuels and electrical power [1,2,3]. Plasmonic nanostructures (Au, Ag) exhibit localized surface plasmon resonance (SPR), the coherent oscillation of conduction electrons coupled to strong local electric fields. Ohmic relaxation of “hot” electrons (100 fs to 1 ps) results in local thermal dissipation (100 ps to 10 ns) that can aid in activating adsorbed reactants and accelerating surface kinetics [3,9,10]. Emerging multifunctional photocatalysts incorporate both plasmonic and catalytic active materials for chemical conversion [3,5,6,7,8,9,10,11,12,13,14,15,16]
Sign-in/Register to view highlights & summary Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a call
