Plasmon-induced selective carbon dioxide conversion on earth-abundant aluminum-cuprous oxide antenna-reactor nanoparticles

Hossein Robatjazi, Hangqi Zhao, Dayne F. Swearer, Nathaniel J. Hogan, Linan Zhou, Alessandro Alabastri, Michael J. McClain, Peter Nordlander and Naomi J. Halas ()
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Hossein Robatjazi: Rice University
Hangqi Zhao: Rice University
Dayne F. Swearer: Rice University
Nathaniel J. Hogan: Rice University
Linan Zhou: Rice University
Alessandro Alabastri: Rice University
Michael J. McClain: Rice University
Peter Nordlander: Rice University
Naomi J. Halas: Rice University

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract The rational combination of plasmonic nanoantennas with active transition metal-based catalysts, known as ‘antenna-reactor’ nanostructures, holds promise to expand the scope of chemical reactions possible with plasmonic photocatalysis. Here, we report earth-abundant embedded aluminum in cuprous oxide antenna-reactor heterostructures that operate more effectively and selectively for the reverse water-gas shift reaction under milder illumination than in conventional thermal conditions. Through rigorous comparison of the spatial temperature profile, optical absorption, and integrated electric field enhancement of the catalyst, we have been able to distinguish between competing photothermal and hot-carrier driven mechanistic pathways. The antenna-reactor geometry efficiently harnesses the plasmon resonance of aluminum to supply energetic hot-carriers and increases optical absorption in cuprous oxide for selective carbon dioxide conversion to carbon monoxide with visible light. The transition from noble metals to aluminum based antenna-reactor heterostructures in plasmonic photocatalysis provides a sustainable route to high-value chemicals and reaffirms the practical potential of plasmon-mediated chemical transformations.

Date: 2017
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DOI: 10.1038/s41467-017-00055-z

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