Hot-Carrier Organic Synthesis via the Near-Perfect Absorption of Light
Qi Xiao, Timothy U Connell, Jasper J Cadusch, Ann Roberts, Anthony SR Chesman, Daniel E Gomez
ACS CATALYSIS | AMER CHEMICAL SOC | Published : 2018
Photocatalysis enables the synthesis of valuable organic compounds by exploiting photons as a chemical reagent. Although light absorption is an intrinsic step, existing approaches rely on poorly absorbing catalysts that require high illumination intensities to afford enhanced efficiencies. Here, we demonstrate that a plasmonic metamaterial capable of near-perfect light absorption (94%) readily catalyzes a model organic reaction with a 29-fold enhancement in conversion relative to controls. The oxidation of benzylamine proceeds via a reactive iminium intermediate with high selectivity at ambient temperature and pressure, using only low-intensity visible irradiation. Control experiments demons..View full abstract
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Awarded by ARC
This work was performed in part at the Melbourne Centre for Nanofabrication (MCN) in the Victorian Node of the Australian National Fabrication Facility (ANFF). The authors would like to thank Milena Czyz for her feedback regarding the photocatalytic mechanism. QX. acknowledges CSIRO for an OCE Fellowship. We acknowledge the ARC for support through a Discovery Project (No. DP160100983) and a Future Fellowship (No. FT140100514).