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CuBiW 2 O 8 (CBTO), with a band gap of 1.9–2.0 eV, responds to a wide region of the electromagnetic spectrum, which makes it a good candidate for solar-driven photocatalytic energy conversion and water treatment. We have previously demonstrated a Cu-rich solid state approach that enables the synthesis of CBTO accompanied by thermodynamically stable Bi 2 WO 6 impurity. Here, we describe an improved synthesis protocol with decreased impurity and synthesis time, and the first demonstration of CBTO as a functional material using photocatalytic Cr( vi ) photoreduction as a probe reaction. Transient absorption spectroscopy (TAS) was performed to investigate the ultrafast dynamics of the charge carriers after photoexcitation. The presence of two populations of photoexcited carriers was found, including short-lived free carriers with ∼10 ps lifetime and long-lived shallowly-trapped carriers with ∼1 ns lifetime. Together with carrier mobilities measured in our previous study, the new TAS results indicate that the long-lived charges have diffusion lengths similar to the CBTO particle size and were likely responsible for the majority of the photocatalytic activity. High activity of CBTO for Cr( vi ) photoreduction (∼100% reduction of 5 mg L −1 of Cr( vi ) in 15 minutes) was demonstrated, which clearly establishes the promise of this novel oxide for visible light-driven photocatalytic applications. Radical quenching experiments indicate that both ˙OH radicals and O 2 ˙ − radicals are produced by CBTO and are involved in the photoreduction of Cr( vi ). Repeated photocatalysis tests and analysis of the surface after the reaction show that CBTO is a stable and potentially reusable catalyst. Insights gained from correlating the synthesis conditions, carrier dynamics, and reactive species suggests that CBTO prepared with the improved protocol would be a favorable choice for photocatalytic reactions such as water decontamination from organic pollutants, water splitting, and solar fuel generation using visible light.
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One-step aerosol synthesis of a double perovskite oxide (KBaTeBiO 6 ) as potential catalysts for CO 2 photoreduction
This study presents a comprehensive investigation on the aerosol synthesis of a semiconducting double perovskite oxide with a nominal composition of KBaTeBiO 6 , which is considered as a potential candidate for CO 2 photoreduction. We demonstrate the rapid synthesis of the multispecies compounds KBaTeBiO 6 with extreme high purity and controllable size through a single-step furnace aerosol reactor (FuAR) process. The formation mechanism of the perovskite in the aerosol route is investigated using thermogravimetric analysis to identify the optimal reference temperature, residence time and other operational parameters in the FuAR synthesis process to obtain the highly pure KBaTeBiO 6 nanoparticles. It is observed that particle formation in the FuAR is based on a mixture of gas-to-particle and liquid-to-particle mechanisms. The phase purity of the perovskite nanoparticles depends on the ratio of the residence time and the reaction time. The particle size is strongly affected by the precursor concentration, residence time and the furnace temperature. Finally, the photocatalytic performance of the synthesized KBaTeBiO 6 nanoparticles is investigated for CO 2 photoreduction under UV-light. The best performing sample exhibits an average CO production rate of 180 μmol g −1 h −1 in the first half hour with a quantum efficiency of 1.19%, demonstrating KBaTeBiO 6 as a promising photocatalyst for CO 2 photoreduction.
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- Award ID(s):
- 1806147
- PAR ID:
- 10253134
- Date Published:
- Journal Name:
- Nanoscale
- ISSN:
- 2040-3364
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/D1NR01505B
