| 1. |
- Boscolo Bibi, Sara, 1993-, et al.
(författare)
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Multi-spectroscopic study of electrochemically-formed oxide-derived gold electrodes
- 2024
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 26:3, s. 2332-2340
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Tidskriftsartikel (refereegranskat)abstract
- Oxide-derived metals are produced by reducing an oxide precursor. These materials, including gold, have shown improved catalytic performance over many native metals. The origin of this improvement for gold is not yet understood. In this study, operando non-resonant sum frequency generation (SFG) and ex situ high-pressure X-ray photoelectron spectroscopy (HP-XPS) have been employed to investigate electrochemically-formed oxide-derived gold (OD-Au) from polycrystalline gold surfaces. A range of different oxidizing conditions were used to form OD-Au in acidic aqueous medium (H3PO4, pH = 1). Our electrochemical data after OD-Au is generated suggest that the surface is metallic gold, however SFG signal variations indicate the presence of subsurface gold oxide remnants between the metallic gold surface layer and bulk gold. The HP-XPS results suggest that this subsurface gold oxide could be in the form of Au2O3 or Au(OH)3. Furthermore, the SFG measurements show that with reducing electrochemical treatments the original gold metallic state can be restored, meaning the subsurface gold oxide is released. This work demonstrates that remnants of gold oxide persist beneath the topmost gold layer when the OD-Au is created, potentially facilitating the understanding of the improved catalytic properties of OD-Au.
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| 4. |
- El-Zohry, Ahmed M., et al.
(författare)
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Highly Emissive Biological Bilirubin Molecules : Shedding New Light on the Phototherapy Scheme
- 2021
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 125:32, s. 9213-9222
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Tidskriftsartikel (refereegranskat)abstract
- Bilirubin (BR) is the main end-product of the hemoglobin catabolism. For decades, its photophysics has been mainly discussed in terms of ultrafast deactivation of the excited state in solution, where, indeed, BR shows a very low green emission quantum yield (EQY), 0.03%, resulting from an efficient nonradiative isomerization process. Herein, we present, for the first time, unique and exceptional photophysical properties of solid-state BR, which amend by changing the type of crystal, from a closely packed alpha crystal to an amorphous loosely packed beta crystal. BR alpha crystals show a very bright red emission with an EQY of ca. 24%, whereas beta crystals present, in addition, a low green EQY of ca. 0.5%. By combining density functional theory (DFT) calculations and time-resolved emission spectroscopy, we trace back this dual emission to the presence of two types of BR molecules in the crystal: a stiff monomer, M1, distorted by particularly strong internal H-bonds and a floppy monomer, M2, having a structure close to that of BR in solution. We assign the red strong emission of BR crystals to M1 present in both the alpha and beta crystals, while the low green emission, only present in the amorphous (beta) crystal, is interpreted as M2 emission. Efficient energy-transfer processes from M2 to M1 in the closely packed a crystal are invoked to explain the absence of the green component in its emission spectrum. Interestingly, these unique photophysical properties of BR remain in polar solvents such as water. Based on these unprecedented findings, we propose a new model for the phototherapy scheme of BR inside the human body and highlight the usefulness of BR as a strong biological fluorescent probe.
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| 5. |
- El-Zohry, Ahmed M., et al.
(författare)
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Ultrafast transient infrared spectroscopy for probing trapping states in hybrid perovskite films
- 2022
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Ingår i: Communications Chemistry. - : Springer Science and Business Media LLC. - 2399-3669. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- Studying the charge dynamics of perovskite materials is a crucial step to understand the outstanding performance of these materials in various fields. Herein, we utilize transient absorption in the mid-infrared region, where solely electron signatures in the conduction bands are monitored without external contributions from other dynamical species. Within the measured range of 4000 nm to 6000 nm (2500–1666 cm−1), the recombination and the trapping processes of the excited carriers could be easily monitored. Moreover, we reveal that within this spectral region the trapping process could be distinguished from recombination process, in which the iodide-based films show more tendencies to trap the excited electrons in comparison to the bromide-based derivatives. The trapping process was assigned due to the emission released in the mid-infrared region, while the traditional band-gap recombination process did not show such process. Various parameters have been tested such as film composition, excitation dependence and the probing wavelength. This study opens new frontiers for the transient mid-infrared absorption to assign the trapping process in perovskite films both qualitatively and quantitatively, along with the potential applications of perovskite films in the mid-IR region.
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| 7. |
- Abdelhamid, Hani Nasser, et al.
(författare)
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Towards implementing hierarchical porous zeolitic imidazolate frameworks in dye-sensitized solar cells
- 2019
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Ingår i: Royal Society Open Science. - : Royal Society Publishing. - 2054-5703. ; 6:7
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Tidskriftsartikel (refereegranskat)abstract
- A one-pot method for encapsulation of dye, which can be applied for dye-sensitized solar cells (DSSCs), and synthesis of hierarchical porous zeolitic imidazolate frameworks (ZIF-8), is reported. The size of the encapsulated dye tunes the mesoporosity and surface area of ZIF-8. The mesopore size, Langmuir surface area and pore volume are 15 nm, 960-1500 m(2). g(-1) and 0.36-0.61 cm(3). g(-1), respectively. After encapsulation into ZIF-8, the dyes show longer emission lifetimes (greater than 4-8-fold) as compared to the corresponding non-encapsulated dyes, due to suppression of aggregation, and torsional motions.
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| 8. |
- Abdellah, Mohamed, et al.
(författare)
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Time-Resolved IR Spectroscopy Reveals a. Mechanism with TiO2 as a Reversible Electron Acceptor in a TiO2-Re Catalyst System for CO2 Photoreduction
- 2017
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Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 139:3, s. 1226-1232
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Tidskriftsartikel (refereegranskat)abstract
- Attaching the phosphonated molecular catalyst [(ReBr)-Br-I(bpy)-(CO)(3)](0) to the wide-bandgap semiconductor TiO2 strongly enhances the rate of visible-light-driven reduction of CO2 to CO in dimethylformamide with triethanolamine (TEOA) as sacrificial electron donor. Herein, we show by transient mid-IR spectroscopy that the mechanism of catalyst photoreduction is initiated by ultrafast electron injection into TiO2, followed by rapid (ps-ns) and sequential two-electron oxidation of TEOA that is coordinated to the Re center. The injected electrons can be stored in the conduction band of TiO2 on an ms-s time scale, and we propose that they lead to further reduction of the Re catalyst and completion of the catalytic cycle. Thus, the excited Re catalyst gives away one electron and would eventually get three electrons back. The function of an electron reservoir would represent a role for TiO2 in photocatalytic CO2 reduction that has previously not been considered. We propose that the increase in photocatalytic activity upon heterogenization of the catalyst to TiO2 is due to the slow charge recombination and the high oxidative power of the Re-II species after electron injection as compared to the excited MLCT state of the unbound Re catalyst or when immobilized on ZrO2, which results in a more efficient reaction with TEOA.
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| 9. |
- Bi, Dongqin, et al.
(författare)
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Improved Morphology Control Using a Modified Two-Step Method for Efficient Perovskite Solar Cells
- 2014
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 6:21, s. 18751-18757
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Tidskriftsartikel (refereegranskat)abstract
- A two-step wet chemical synthesis method for methylammonium lead(II) triiodide (CH3NH3PbI3) perovskite is further developed for the preparation of highly reproducible solar cells, with the following structure: fluorine-doped tin oxide (FTO)/TiO2 (compact)/TiO2 (mesoporous)/CH3NH3PbI3/spiro-OMeTAD/Ag. The morphology of the perovskite layer could be controlled by careful variation of the processing conditions. Specifically, by modifying the drying process and inclusion of a dichloromethane treatment, more uniform films could be prepared, with longer emission lifetime in the perovskite material and longer electron lifetime in solar cell devices, as well as faster electron transport and enhanced charge collection at the selective contacts. Solar cell efficiencies up to 13.5% were obtained.
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| 10. |
- Bi, Dongqin, et al.
(författare)
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Unraveling the Effect of PbI2 Concentration on Charge Recombination Kinetics in Perovskite Solar Cells
- 2015
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Ingår i: ACS Photonics. - : American Chemical Society (ACS). - 2330-4022. ; 2:5, s. 589-594
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Tidskriftsartikel (refereegranskat)abstract
- CH3NH3PbI3 perovskite solar cells have rapidly risen to the forefront of emerging photovoltaic technologies. A solution-based, two-step method was reported to enhance the reproducibility of these solar cells. In this method, first a coating of PbI2 is applied by spin-coating onto a TiO2-coated substrate, followed by a dip in a methylammonium iodide solution, leading to conversion to CH3NH3PbI3. The concentration of PbI2 in the spin-coating solution is a very important factor that affects the infiltration of the perovskite and the amount deposited. The best solar cell performance of 13.9% was obtained by devices prepared using 1.0 M of PbI2 in dimethylformamide. These devices also had the longest electron lifetime and shortest carrier transport time, yielding lowest recombination losses. Rapid quenching of the perovskite emission is found in device-like structures, suggesting reasonably good efficient carrier extraction at the TiO2 interface and quantitative extraction at the spiro-OMeTAD interface.
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