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Perovskite-based nanocubes with simultaneously improved visible-light absorption and charge separation enabling efficient photocatalytic CO2 reduction
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2016 (English)In: Nano Energy, ISSN 2211-2855, Vol. 30, 59-68 p.Article in journal (Refereed) Published
Abstract [en]

Finding an ideal model to disclose the role upon tuning band structure and charge separation of wide-bandgap perovskite semiconductors by introducing suitable heteroatoms remains a huge challenge in photocatalysis. Herein, we propose an efficient pathway to increase the light absorption and charge separation for nitrogen and oxygen-vacancy confined in sodium tantalate nanocubes (Vo-NaTaON) and nitrogen-doped graphene quantum dots (N-GQDs) grafted Vo-NaTaON nanocubes by solution-etching-induced phase-transition and in-situ reduction strategies. First-principles calculations demonstrate that the simultaneous incorporation of nitrogen and oxygen-vacancy in sodium tantalate can effectively regulate the electronic structure of sodium tantalate. The analysis of UV–vis spectra and electron paramagnetic resonance reveal that the synergistic contribution of nitrogen and oxygen-vacancy endows the wide-bandgap perovskites tuning the band absorption region from UV (315 nm) to visible regime beyond 600 nm. As expected, an optimized Vo-NaTaON catalyst was developed, exhibiting superior broad spectrum photochemical reduction of CO2 to fuels. Moreover, N-GQDs/Vo-NaTaON heterojunctions further improve the broad spectrum CO2 photoreduction due to the synergetic catalytic effect of simultaneously improved light-absorption and charge separation. This work may open up more opportunities in the design of efficient photocatalysts for applications in solar photochemical conversion.

Place, publisher, year, edition, pages
Elsevier, 2016. Vol. 30, 59-68 p.
Keyword [en]
Band structure tuning, Charge separation, CO2 photoreduction, Nitrogen-doped graphene quantum dots, Perovskite, Absorption spectroscopy, Band structure, Calculations, Carbon dioxide, Doping (additives), Electromagnetic wave absorption, Electronic structure, Energy gap, Graphene, Heterojunctions, Light, Light absorption, Magnetic resonance, Nanocrystals, Nitrogen, Oxygen, Paramagnetic resonance, Semiconductor quantum dots, Separation, Sodium, Tuning, Wide band gap semiconductors, Charge separations, First-principles calculation, Induced phase transition, Nitrogen doped graphene, Photo-reduction, Photochemical conversion, Structure tuning, Visible light absorption, Oxygen vacancies
National Category
Chemical Sciences
URN: urn:nbn:se:kth:diva-195197DOI: 10.1016/j.nanoen.2016.09.033ScopusID: 2-s2.0-84991497913OAI: diva2:1051311

QC 20161201

Available from: 2016-12-01 Created: 2016-11-02 Last updated: 2016-12-01Bibliographically approved

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Sun, Licheng
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