Abstract
Conversion of solar energy into liquid fuel often relies on multielectron redox processes that include highly reactive intermediates, with back reaction routes that hinder the overall efficiency of the process. Here, we reveal that these undesirable reaction pathways can be minimized, rendering the photocatalytic reactions more efficient, when charge carriers are harvested from a multiexcitonic state of a semiconductor photocatalyst. A plasmonic antenna, comprising Au nanoprisms, was employed to accomplish feasible levels of multiple carrier excitations in semiconductor nanocrystal-based photocatalytic systems (CdSe@CdS core-shell quantum dots and CdSe@CdS seeded nanorods). The antenna's near-field amplifies the otherwise inherently weak biexciton generation in the semiconductor. The two-electron photoreduction of Pt and Pd metal precursors served as model reactions. In the presence of the plasmonic antenna, these photocatalyzed two-electron reactions exhibited enhanced yields and kinetics. This work uniquely relies on a nonlinear enhancement that has potential for large amplification of photocatalytic activity in the presence of a plasmonic near-field.
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