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Issue 22, 2018
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Electronic structure manipulation of graphene dots for effective hydrogen evolution from photocatalytic water decomposition

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Abstract

This paper presents a heteroatom doping strategy to manipulate the structure of graphene-based photocatalysts for effective hydrogen production from aqueous solution. Oxygenation of graphene creates a bandgap to produce semiconducting graphene oxide, nitrogen doping extends the resonant π-conjugation to prolong the charge lifetime, and sulfur doping breaks the electron neutrality to facilitate charge transfer. Accordingly, ammonia-treated sulfur–nitrogen-co-doped graphene oxide dots (A-SNGODs) are synthesized by annealing graphene oxide sheets in sulfur-ammonia, oxidizing the sheets into dots, and then hydrothermally treating the dots in ammonia. The A-SNGODs exhibit a high nitrogen content in terms of quaternary and amide groups that are formed through sulfur-mediated reactions. The peripheral amide facilitates orbital conjugations to enhance the photocatalytic activity, whereas the quaternary nitrogen patches vacancy defects to improve stability. The simultaneous presence of electron-withdrawing S and electron-donating N atoms in the A-SNGODs facilitates charge separation and results in reactive electrons. When suspended in an aqueous triethanolamine solution, Pt-deposited A-SNGODs demonstrate a hydrogen-evolution quantum yield of 29% under monochromatic 420 nm irradiation. The A-SNGODs exhibit little activity decay under 6-day visible-light irradiation. This study demonstrates the excellence of the heteroatom-doping strategy in producing stable and active graphene-based materials for photoenergy conversion.

Graphical abstract: Electronic structure manipulation of graphene dots for effective hydrogen evolution from photocatalytic water decomposition

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Publication details

The article was received on 24 Mar 2018, accepted on 04 May 2018 and first published on 05 May 2018


Article type: Paper
DOI: 10.1039/C8NR02441C
Citation: Nanoscale, 2018,10, 10721-10730
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    Electronic structure manipulation of graphene dots for effective hydrogen evolution from photocatalytic water decomposition

    B. Nguyen, Y. Xiao, C. Shih, V. Nguyen, W. Chou and H. Teng, Nanoscale, 2018, 10, 10721
    DOI: 10.1039/C8NR02441C

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