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Efficient Near-Infrared-Activated Photocatalytic Hydrogen Evolution from Ammonia Borane with Core-Shell Upconversion-Semiconductor Hybrid Nanostructures.

ABSTRACT: In this work, the photocatalytic hydrogen evolution from ammonia borane under near-infrared laser irradiation at ambient temperature was demonstrated by using the novel core-shell upconversion-semiconductor hybrid nanostructures (NaGdF₄:Yb³⁺/Er³⁺@NaGdF₄@Cu₂O). The particles were successfully synthesized in a final concentration of 10 mg/mL. The particles were characterized via high resolution transmission electron microscopy (HRTEM), photoluminescence, energy dispersive X-ray analysis (EDAX), and powder X-ray diffraction. The near-infrared-driven photocatalytic activities of such hybrid nanoparticles are remarkably higher than that with bare upconversion nanoparticles (UCNPs) under the same irradiation. The upconverted photoluminescence of UCNPs efficiently reabsorbed by Cu₂O promotes the charge separation in the semiconducting shell, and facilitates the formation of photoinduced electrons and hydroxyl radicals generated via the reaction between H₂O and holes. Both serve as reactive species on the dissociation of the weak B-N bond in an aqueous medium, to produce hydrogen under near-infrared excitation, resulting in enhanced photocatalytic activities. The photocatalyst of NaGdF₄:Yb³⁺/Er³⁺@NaGdF₄@Cu₂O (UCNPs@Cu₂O) suffered no loss of efficacy after several cycles. This work sheds light on the rational design of near-infrared-activated photocatalysts, and can be used as a proof-of-concept for on-board hydrogen generation from ammonia borane under near-infrared illumination, with the aim of green energy suppliers.

SUBMITTER: Evangelista AJ

PROVIDER: S-EPMC8707141 | biostudies-literature |

REPOSITORIES: biostudies-literature

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