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

Nanoscale
Ba-Son NguyenHsisheng Teng

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 yie...Continue Reading

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Citations

Mar 19, 2019·Chemical Society Reviews·Chao HuYa-Ping Sun
Nov 30, 2021·Journal of the American Chemical Society·Bikash JanaDirk M Guldi

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Methods Mentioned

BETA
electron resonance
transmission electron microscopy
X-ray

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