| 1. |
- Bianca, Gabriele, et al.
(författare)
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Liquid-Phase Exfoliated GeSe Nanoflakes for Photoelectrochemical-Type Photodetectors and Photoelectrochemical Water Splitting
- 2020
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Ingår i: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 12:43, s. 48598-48613
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Tidskriftsartikel (refereegranskat)abstract
- Photoelectrochemical (PEC) systems represent powerful tools to convert electromagnetic radiation into chemical fuels and electricity. In this context, two-dimensional (2D) materials are attracting enormous interest as potential advanced photo(electro)catalysts and, recently, 2D group-IVA metal monochalcogenides have been theoretically predicted to be water splitting photocatalysts. In this work, we use density functional theory calculations to theoretically investigate the photocatalytic activity of single-/few-layer GeSe nanoflakes for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in pH conditions ranging from 0 to 14. Our simulations show that GeSe nanoflakes with different thickness can be mixed in the form of nanoporous films to act as nanoscale tandem systems, in which the flakes, depending on their thickness, can operate as HER- and/or OER photocatalysts. On the basis of theoretical predictions, we report the first experimental characterization of the photo(electro)catalytic activity of single-/few-layer GeSe flakes in different aqueous media, ranging from acidic to alkaline solutions: 0.5 M H2SO4 (pH 0.3), 1 M KCl (pH 6.5), and 1 M KOH (pH 14). The films of the GeSe nanoflakes are fabricated by spray coating GeSe nanoflakes dispersion in 2-propanol obtained through liquid-phase exfoliation of synthesized orthorhombic (Pnma) GeSe bulk crystals. The PEC properties of the GeSe nanoflakes are used to design PEC-type photodetectors, reaching a responsivity of up to 0.32 AW(-1) (external quantum efficiency of 86.3%) under 455 nm excitation wavelength in acidic electrolyte. The obtained performances are superior to those of several self-powered and low-voltage solution-processed photodetectors, approaching that of self-powered commercial UV-Vis photodetectors. The obtained results inspire the use of 2D GeSe in proof-of-concept water photoelectrolysis cells.
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| 2. |
- Najafi, Leyla, et al.
(författare)
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Topochemical Transformation of Two-Dimensional VSe2 into Metallic Nonlayered VO2 for Water Splitting Reactions in Acidic and Alkaline Media
- 2022
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 16:1, s. 351-367
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Tidskriftsartikel (refereegranskat)abstract
- The engineering of the structural and morphological properties of nanomaterials is a fundamental aspect to attain desired performance in energy storage/conversion systems and multifunctional composites. We report the synthesis of room temperature-stable metallic rutile VO2 (VO2 (R)) nanosheets by topochemically transforming liquid-phase exfoliated VSe2 in a reductive Ar-H2 atmosphere. The asproduced VO2 (R) represents an example of two-dimensional (2D) nonlayered materials, whose bulk counterparts do not have a layered structure composed by layers held together by van der Waals force or electrostatic forces between charged layers and counterbalancing ions amid them. By pretreating the VSe2 nanosheets by O-2 plasma, the resulting 2D VO2 (R) nanosheets exhibit a porous morphology that increases the material specific surface area while introducing defective sites. The assynthesized porous (holey)-VO2 (R) nanosheets are investigated as metallic catalysts for the water splitting reactions in both acidic and alkaline media, reaching a maximum mass activity of 972.3 A g(-1) at -0.300 V vs RHE for the hydrogen evolution reaction (HER) in 0.5 M H2SO4 (faradaic efficiency = 100%, overpotential for the HER at 10 mA cm(-2) = 0.184 V) and a mass activity (calculated for a non 100% faradaic efficiency) of 745.9 A g(-1) at +1.580 V vs RHE for the oxygen evolution reaction (OER) in 1 M KOH (overpotential for the OER at 10 mA cm(-2) = 0.209 V). By demonstrating proof-of-concept electrolyzers, our results show the possibility to synthesize special material phases through topochemical conversion of 2D materials for advanced energy-related applications.
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