Photocatalytic conversion of solar energy to fuels, such as hydrogen, is attracting enormous interest, driven by the promise of addressing both energy supply and storage. Colloidal semiconductor nanocrystals have been at the forefront of these efforts owing to their favourable and tunable optical and electronic properties as well as advances in their synthesis. The efficiency of the photocatalysts is often limited by the slow transfer and subsequent reactions of the photoexcited holes and the ensuing high charge recombination rates. Here we propose that employing a hydroxyl anion/radical redox couple to efficiently relay the hole from the semiconductor to the scavenger leads to a marked increase in the H2 generation rate without using expensive noble metal co-catalysts. The apparent quantum yield and the formation rate under 447 nm laser illumination exceeded 53% and 63 mmol g(-1) h(-1), respectively. The fast hole transfer confers long-term photostability on the system and opens new pathways to improve the oxidation side of full water splitting.
Nitrogen-doped carbon
dots synthesized from citric acid as a carbon
precursor have recently been considered to contain fluorescent derivatives
of citrazinic acid, which contribute to their emission in the blue
spectral range. To study the impact of such molecular fluorescent
species on the optical properties of carbon dots, we synthesized three
samples employing citric acid and three different nitrogen sources:
ethylenediamine, hexamethylenetetramine, and triethanolamine. On the
basis of the analysis of the nitrogen content and its coordination
by X-ray photoelectron spectroscopy, FTIR spectra, and systematically
comparing absorption, steady-state emission, and photoluminescence
decays of each kind of carbon dot, we derive the influence of the
molecular precursors and gain further understanding of the complex
structure of carbon dots highlighting the strong impact of molecular
fluorescence in the samples produced with ethylenediamine and hexamethylenetetramine.
Laser mediated remote release of encapsulated fluorescently labeled polymers from nanoengineered polyelectrolyte multilayer capsules containing gold sulfide core/gold shell nanoparticles in their walls is observed in real time on a single capsule level. We have developed a method for measuring the temperature increase and have quantitatively investigated the influence of absorption, size, and surface density of metal nanoparticles using an analytical model. Experimental measurements and numerical simulations agree with the model. The treatment presented in this work is of general nature, and it is applicable to any system where nanoparticles are used as absorbing centers. Potential biomedical applications are highlighted.
Emission color controlled, high quantum yield CH3NH3PbBr3 perovskite quantum dots are obtained by changing the temperature of a bad solvent during synthesis. The products for temperatures between 0 and 60 °C have good spectral purity with narrow emission line widths of 28–36 nm, high absolute emission quantum yields of 74% to 93%, and short radiative lifetimes of 13–27 ns.
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