Abstract
The localized surface plasmon resonance (LSPR) excitation in plasmonic nanoparticles (NPs) in the visible and near-infrared ranges is currently at the forefront of improving photocatalytic performances via plasmonic photocatalysis. One bottleneck of this field is that the NPs that often display the best optical properties in the visible and near-infrared ranges are based on expensive noble metals such as silver (Ag) and gold (Au). While earth-abundant plasmonic materials have been proposed together with catalytic metals in antenna–reactor systems, their performances remain limited by their optical properties. Importantly, the synthesis of plasmonic photocatalysts remains challenging in terms of scalability while often requiring several steps, high temperatures, and special conditions. Herein, we address these challenges by developing a one-pot, gram-scale, room-temperature synthesis of earth-abundant plasmonic photocatalysts while improving their activities beyond what has been dictated by the LSPR excitation of the plasmonic component. We describe the mechanochemical synthesis of earth-abundant plasmonic photocatalysts by using MoO3 (antenna) and Au (reactor) NPs as a proof-of-concept example and demonstrate that the dual plasmonic excitation of antenna and reactor sites enables the tuning of plasmonic photocatalytic performances toward the reductive coupling of nitrobenzene to azobenzene as a model reaction. In addition to providing a pathway to the facile and gram-scale synthesis of plasmonic photocatalysts, the results reported herein may open pathways to improved activities in plasmonic catalysis.
Highlights
Mechanochemistry is a mature field,[1] there has been a renewed interest in the development of mechanochemical approaches for the synthesis of inorganic materials, such as oxides[2−5] and metal nanoparticles (NPs).[6−12] This has been driven by attractive features of mechanochemistry relative to commonly reported batch solution phase strategies
We aim to address both challenges, i.e., to develop a one-pot, gram-scale, room-temperature synthesis of earth-abundant plasmonic photocatalysts while improving their activities beyond what has been dictated by the localized surface plasmon resonance (LSPR) excitation of the plasmonic component
Au NPs and (ii) it acts as a source of hydrogen species that can intercalate into the MoO3 structure
Summary
Mechanochemistry is a mature field,[1] there has been a renewed interest in the development of mechanochemical approaches for the synthesis of inorganic materials, such as oxides[2−5] and metal nanoparticles (NPs).[6−12] This has been driven by attractive features of mechanochemistry relative to commonly reported batch solution phase strategies. Metal NPs present unique electronic, optical, and chemical properties that can be pivotal to new imaging and therapeutical applications,[13] to allow more sustainable molecular transformations,[14] and to enable a transition to a more sustainable society and circular economy.[15]. It has been demonstrated that, in addition to outstanding optical properties, LSPR excitation can contribute to accelerate or drive several chemical reactions.[18,19] NPs supporting LSPR excitation in the visible and nearinfrared ranges (plasmonic NPs) are currently at the forefront of improving photocatalytic performances.[20−22] This field, named “plasmonic catalysis” (or “plasmonic photocatalysis”), allows for much milder conditions and alternative reaction
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