TY - JOUR
T1 - Unassisted Highly Selective Gas-Phase CO2Reduction with a Plasmonic Au/p-GaN Photocatalyst Using H2O as an Electron Donor
AU - Li, Rengui
AU - Cheng, Wen Hui
AU - Richter, Matthias H.
AU - Duchene, Joseph S.
AU - Tian, Wenming
AU - Li, Can
AU - Atwater, Harry A.
N1 - Funding Information:
This work was performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, and was primarily supported through the Office of Science of the U.S. Department of Energy (DOE) under Award No. DE SC0004993 (sample synthesis, gas-phase photocatalytic measurements, and photoelectrochemical measurements) and by the Liquid Sunlight Alliance under Award No. DE-SC0021266 (sample structural and morphological characterization and data analysis). Research was in part carried out at the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology.
Funding Information:
This work was performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, and was primarily supported through the Office of Science of the U.S. Department of Energy (DOE) under Award No. DE SC0004993 (sample synthesis, gas-phase photocatalytic measurements, and photoelectrochemical measurements), and by the Liquid Sunlight Alliance under Award No. DE-SC0021266 (sample structural and morphological characterization and data analysis). Research was in part carried out at the Molecular Materials Research Center of the Beckman Institute of the California Institute of Technology.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/5/14
Y1 - 2021/5/14
N2 - Surface plasmon resonances in metal nanostructures enable the generation of nonequilibrium hot electron-hole pairs, which has received wide interest as a means to drive chemical reactions at the nanoscale. However, harvesting hot holes in plasmonic heterostructures to drive oxidation reactions to balance the photocatalytic CO2 reduction reaction has been challenging. Further, details of the balanced redox reaction pathways for gas-phase photocatalysis have been difficult to identify. Here, we report an Au/p-GaN plasmonic heterostructure photocatalyst in which unassisted, self-sustaining, highly selective photocatalytic CO2 reduction to CO is directly balanced by water oxidation, operating under solar illumination. We find remarkable enhancements in CO yield for heterostructures that employ a metal/insulator/semiconductor configuration with an ultrathin aluminum oxide layer between composite Au/Cu nanoparticles and p-GaN. Our work underscores the potential for plasmonic heterostructure photocatalysts to perform selective and unassisted gas-phase photocatalytic CO2 reduction to convert solar energy into chemical fuels.
AB - Surface plasmon resonances in metal nanostructures enable the generation of nonequilibrium hot electron-hole pairs, which has received wide interest as a means to drive chemical reactions at the nanoscale. However, harvesting hot holes in plasmonic heterostructures to drive oxidation reactions to balance the photocatalytic CO2 reduction reaction has been challenging. Further, details of the balanced redox reaction pathways for gas-phase photocatalysis have been difficult to identify. Here, we report an Au/p-GaN plasmonic heterostructure photocatalyst in which unassisted, self-sustaining, highly selective photocatalytic CO2 reduction to CO is directly balanced by water oxidation, operating under solar illumination. We find remarkable enhancements in CO yield for heterostructures that employ a metal/insulator/semiconductor configuration with an ultrathin aluminum oxide layer between composite Au/Cu nanoparticles and p-GaN. Our work underscores the potential for plasmonic heterostructure photocatalysts to perform selective and unassisted gas-phase photocatalytic CO2 reduction to convert solar energy into chemical fuels.
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U2 - 10.1021/acsenergylett.1c00392
DO - 10.1021/acsenergylett.1c00392
M3 - Article
AN - SCOPUS:85106563706
SN - 2380-8195
VL - 6
SP - 1849
EP - 1856
JO - ACS Energy Letters
JF - ACS Energy Letters
IS - 5
ER -