Plasmonic Au nanoclusters dispersed in nitrogen-doped graphene as a robust photocatalyst for light-to-hydrogen conversion

Supported plasmonic Au nanoclusters (NCs) consisting of a few tens of atoms can potentially offer great advantages for the light-driven hydrogen evolution reaction (HER). Here, we report on the synthesis of well-dispersed and stable plasmonic Au NCs of 0.5-1.0 nm size on nitrogen-doped high surface...

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Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2021-10, Vol.9 (4), p.2281-22819
Main Authors: Van Dao, Dung, Cipriano, Luis A, Di Liberto, Giovanni, Nguyen, Thuy T. D, Ki, Sang-Woo, Son, Hoki, Kim, Gyu-Cheol, Lee, Kang Hyun, Yang, Jin-Kyu, Yu, Yeon-Tae, Pacchioni, Gianfranco, Lee, In-Hwan
Format: Article
Language:English
Subjects:
Argon
Catalytic converters
Conversion
Dispersion
Electromagnetic absorption
Freeze drying
Gold
Graphene
Hot electrons
Hydrogen
Hydrogen evolution reactions
Nanoclusters
Nanocomposites
Nanoparticles
Nitrogen
Photocatalysts
Plasmonics
Surface plasmon resonance
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Summary:Supported plasmonic Au nanoclusters (NCs) consisting of a few tens of atoms can potentially offer great advantages for the light-driven hydrogen evolution reaction (HER). Here, we report on the synthesis of well-dispersed and stable plasmonic Au NCs of 0.5-1.0 nm size on nitrogen-doped high surface area graphene (N-Gr) via freeze-drying and pyrolyzing in argon. The Au NCs/N-Gr photocatalyst exhibits under visible-light an impressive HER achievement (3.16 μmol mg cat −1 h −1 ) compared to Au single atoms/N-Gr (2.06 μmol mg cat −1 h −1 ) and Au nanoparticles (20 nm size)/N-Gr (0.92 μmol mg cat −1 h −1 ), with a maximum apparent quantum yield of 14.30%. These performances are synergistically attributed to two effects: (a) the strong surface plasmon resonance stimulated by light absorption and transferred near the surface of Au NCs, where the N-Gr conductive support can prolong the plasmon-produced hot electrons and direct the light-to-hydrogen conversion; (b) a high catalytic efficiency of Au NCs/N-Gr nanocomposites. Au nanoclusters (2.18 wt%) consisting of a few tens of atoms supported nitrogen-doped graphene deliver an impressive hydrogen evolution reaction rate of 3.16 μmol mg cat −1 h −1 under visible-light irradiation and a high maximum quantum yield of 14.3%.
ISSN:2050-7488
2050-7496
DOI:10.1039/d1ta05445g