| 31. |
- Ding, Xin, et al.
(författare)
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Assembling Supramolecular Dye-Sensitized Photoelectrochemical Cells for Water Splitting
- 2015
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Ingår i: ChemSusChem. - : Wiley-VCH Verlagsgesellschaft. - 1864-5631 .- 1864-564X. ; 8:23, s. 3992-3995
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Tidskriftsartikel (refereegranskat)abstract
- The method used to assemble dye-sensitized photoelectrochemical (DS-PEC) devices plays a vital role in determining its photoactivity and stability. We report a simple and effective method to assemble supramolecular DS-PECs introducing PMMA as support material and a catalyst modified with long carbon chains as photoanodes. The long carbon chains in combination with PMMA allow to better immobilize the catalyst. DS-PECs obtained by this simple method have display excellent photoactivities and stabilities. A photocurrent density of 1.1mAcm(-2) and a maximum IPCE of 9.5% have been obtained with a 0.2V vs NHE external bias.
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| 32. |
- Doubaji, Siham, et al.
(författare)
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Passivation Layer and Cathodic Redox Reactions in Sodium-Ion Batteries Probed by HAXPES
- 2016
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Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 9:1, s. 97-108
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Tidskriftsartikel (refereegranskat)abstract
- The cathode material P2-NaxCo2/3Mn2/9Ni1/9O2, which could be used in Na-ion batteries, was investigated through synchrotron-based hard X-ray photoelectron spectroscopy (HAXPES). Nondestructive analysis was made through the electrode/electrolyte interface of the first electrochemical cycle to ensure access to information not only on the active material, but also on the passivation layer formed at the electrode surface and referred to as the solid permeable interface (SPI). This investigation clearly shows the role of the SPI and the complexity of the redox reactions. Cobalt, nickel, and manganese are all electrochemically active upon cycling between 4.5 and 2.0V; all are in the 4+ state at the end of charging. Reduction to Co3+, Ni3+, and Mn3+ occurs upon discharging and, at low potential, there is partial reversible reduction to Co2+ and Ni2+. A thin layer of Na2CO3 and NaF covers the pristine electrode and reversible dissolution/reformation of these compounds is observed during the first cycle. The salt degradation products in the SPI show a dependence on potential. Phosphates mainly form at the end of the charging cycle (4.5V), whereas fluorophosphates are produced at the end of discharging (2.0V).
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| 33. |
- Etman, Ahmed S., et al.
(författare)
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Flexible Freestanding MoO3-x-Carbon Nanotubes-Nanocellulose Paper Electrodes for Charge-Storage Applications
- 2019
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Ingår i: ChemSusChem. - : John Wiley & Sons. - 1864-5631 .- 1864-564X. ; 12:23, s. 5157-5163
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Tidskriftsartikel (refereegranskat)abstract
- Herein, a one‐step synthesis protocol was developed for synthesizing freestanding/flexible paper electrodes composed of nanostructured molybdenum oxide (MoO3−x) embedded in a carbon nanotube (CNT) and Cladophora cellulose (CC) matrix. The preparation method involved sonication of the precursors, nanostructured MoO3−x, CNTs, and CC with weight ratios of 7:2:1, in a water/ethanol mixture, followed by vacuum filtration. The electrodes were straightforward to handle and possessed a thickness of approximately 12 μm and a mass loading of MoO3−x–CNTs of approximately 0.9 mg cm−2. The elemental mapping showed that the nanostructured MoO3−x was uniformly embedded inside the CNTs–CC matrix. The MoO3−x–CNTs–CC paper electrodes featured a capacity of 30 C g−1, normalized to the mass of MoO3−x–CNTs, at a current density of 78 A g−1 (corresponding to a rate of approximately 210 C based on the MoO3 content, assuming a theoretical capacity of 1339 C g−1), and exhibited a capacity retention of 91 % over 30 000 cycles. This study paves the way for the manufacturing of flexible/freestanding nanostructured MoO3−x‐based electrodes for use in charge‐storage devices at high charge/discharge rates.
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| 34. |
- Fan, Ke, et al.
(författare)
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Immobilization of a Molecular Ruthenium Catalyst on Hematite Nanorod Arrays for Water Oxidation with Stable Photocurrent
- 2015
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 8:19, s. 3242-3247
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Tidskriftsartikel (refereegranskat)abstract
- Photoelectrochemical (PEC) cells for light-driven water splitting are prepared using hematite nanorod arrays on conductive glass as the photoanode. These devices improve the photocurrent of the hematite-based photoanode for water splitting, owing to fewer surface traps and decreased electron recombination resulting from the one-dimensional structure. By employing a molecular ruthenium co-catalyst, which contains a strong 2,6-pyridine-dicarboxylic acid anchoring group at the hematite photoanode, the photocurrent of the PEC cell is enhanced with high stability for over 10000s in a 1M KOH solution. This approach can pave a route for combining one-dimensional nanomaterials and molecular catalysts to split water with high efficiency and stability.
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| 35. |
- Fan, Lizhou, et al.
(författare)
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Molecular Functionalization of NiO Nanocatalyst for Enhanced Water Oxidation by Electronic Structure Engineering
- 2020
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 13:22, s. 5901-5909
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Tidskriftsartikel (refereegranskat)abstract
- Tuning the local environment of nanomaterial-based catalysts has emerged as an effective approach to optimize their oxygen evolution reaction (OER) performance, yet the controlled electronic modulation around surface active sites remains a great challenge. Herein, directed electronic modulation of NiO nanoparticles was achieved by simple surface molecular modification with small organic molecules. By adjusting the electronic properties of modifying molecules, the local electronic structure was rationally tailored and a close electronic structure-activity relationship was discovered: the increasing electron-withdrawing modification readily decreased the electron density around surface Ni sites, accelerating the reaction kinetics and improving OER activity, and vice versa. Detailed investigation by operando Raman spectroelectrochemistry revealed that the electron-withdrawing modification facilitates the charge-transfer kinetics, stimulates the catalyst reconstruction, and promotes abundant high-valent gamma-NiOOH reactive species generation. The NiO-C(6)F(5)catalyst, with the optimized electronic environment, exhibited superior performance towards water oxidation. This work provides a well-designed and effective approach for heterogeneous catalyst fabrication under the molecular level.
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| 36. |
- Farré, Yoann, et al.
(författare)
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A Comparative Investigation of the Role of the Anchoring Group on Perylene Monoimide Dyes in NiO-Based Dye-Sensitized Solar Cells
- 2020
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 13:7, s. 1844-1855
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Tidskriftsartikel (refereegranskat)abstract
- The anchoring group of a sensitizer may strongly affect the overall properties and stability of the resulting dye-sensitized solar cells (DSSCs) and dye-sensitized photoelectrosynthetic solar cells (DSPECs). The properties of seven perylene monoimide (PMI) dyes have been comprehensively studied for their immobilization on nanocrystalline NiO film. The PMI dyes differ only by the nature of the anchoring group, which are: carboxylic acid (PMI-CO2H), phosphonic acid (PMI-PO3H2), acetyl acetone (PMI-acac), pyridine (PMI-Py), aniline (PMI-NH2), hydroxyquinoline (PMI-HQ), and dipicolinic acid (PMI-DPA). The dyes are investigated by cyclic voltammetry and spectroelectrochemistry and modeled by TD-DFT quantum chemical calculations. The mode of binding of these anchoring groups is investigated by infrared spectroscopy and the stability of the binding to NiO surface is studied by desorption experiments in acidic and basic media. The phosphonic acid group is found to offer the strongest binding to the NiO surface in terms of stability and dye loading. Finally, a photophysical study by ultrafast transient absorption spectroscopy shows that all dyes inject a hole in NiO with rate constants on a subpicosecond timescale and display similar charge recombination kinetics. The photovoltaic properties of the dyes show that PMI-HQ and PMI-acac give the highest photovoltaic performances, owing to a lower degree of aggregation on the surface.
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| 37. |
- Ferdowsi, Parnian, et al.
(författare)
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Molecular Design of Efficient Organic D-A-pi-A Dye Featuring Triphenylamine as Donor Fragment for Application in Dye-Sensitized Solar Cells
- 2018
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Ingår i: ChemSusChem. - : WILEY-V C H VERLAG GMBH. - 1864-5631 .- 1864-564X. ; 11:2, s. 494-502
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Tidskriftsartikel (refereegranskat)abstract
- A metal-free organic sensitizer, suitable for the application in dye-sensitized solar cells (DSSCs), has been designed, synthesized and characterized both experimentally and theoretically. The structure of the novel donor-acceptor--bridge-acceptor (D-A-pi-A) dye incorporates a triphenylamine (TPA) segment and 4-(benzo[c][1,2,5]thiadiazol-4-ylethynyl)benzoic acid (BTEBA). The triphenylamine unit is widely used as an electron donor for photosensitizers, owing to its nonplanar molecular configuration and excellent electron-donating capability, whereas 4-(benzo[c][1,2,5]thiadiazol-4-ylethynyl)benzoic acid is used as an electron acceptor unit. The influences of I-3(-)/I-, [Co(bpy)(3)](3+/2+) and [Cu(tmby)(2)](2+/+) (tmby=4,4,6,6-tetramethyl-2,2-bipyridine) as redox electrolytes on the DSSC device performance were also investigated. The maximal monochromatic incident photon-to-current conversion efficiency (IPCE) reached 81% and the solar light to electrical energy conversion efficiency of devices with [Cu(tmby)(2)](2+/+) reached 7.15%. The devices with [Co(bpy)(3)](3+/2+) and I-3(-)/I- electrolytes gave efficiencies of 5.22% and 6.14%, respectively. The lowest device performance with a [Co(bpy)(3)](3+/2+)-based electrolyte is attributed to increased charge recombination.
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| 38. |
- Ferdowsi, Parnian, et al.
(författare)
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Molecular Engineering of Simple Metal-Free Organic Dyes Derived from Triphenylamine for Dye-Sensitized Solar Cell Applications
- 2020
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 13:1, s. 212-220
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Tidskriftsartikel (refereegranskat)abstract
- Two new metal-free organic sensitizers, L156 and L224, were designed, synthesized, and characterized for application in dye-sensitized solar cells (DSCs). The structures of the dyes contain a triphenylamine (TPA) segment and 4-(benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid as electron-rich and -deficient moieties, respectively. Two different pi bridges, thiophene and 4,8-bis(4-hexylphenyl)benzo[1,2-b:4,5-b ']dithiophene, were used for L156 and L224, respectively. The influence of iodide/triiodide, [Co(bpy)(3)](2+/3+) (bpy=2,2 '-bipyridine), and [Cu(tmby)(2)](2+/+) (tmby=4,4 ',6,6 '-tetramethyl-2,2 '-bipyridine) complexes as redox electrolytes and 18 NR-T and 30 NR-D transparent TiO2 films on the DSC device performance was investigated. The L156-based DSC with [Cu(tmby)(2)](2+/+) complexes as the redox electrolyte resulted in the best performance of 9.26 % and a remarkably high open-circuit voltage value of 1.1 V (1.096 V), with a short-circuit current of 12.2 mA cm(-2) and a fill factor of 0.692, by using 30 NR-D TiO2 films. An efficiency of up to 21.9 % was achieved under a 1000 lx indoor light source, which proved that dye L156 was also an excellent candidate for indoor applications. The maximal monochromatic incident-photon-to-current conversion efficiency of L156-30 NR-D reached up to 70 %.
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| 39. |
- Galkin, Maxim, et al.
(författare)
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Selective Route to 2-Propenyl Aryls Directly from Wood by a Tandem Organosolv and Palladium-Catalysed Transfer Hydrogenolysis
- 2014
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 7:8, s. 2154-2158
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Tidskriftsartikel (refereegranskat)abstract
- A tandem organosolv pulping and Pd-catalysed transfer hydrogenolysis depolymerisation and deoxygenation has been developed. The tandem process generated 2-methoxy-4-(prop-1-enyl)phenol in 23 % yield (92 % theoretical monomer yield) starting from pine wood and 2,6-dimethoxy-4-(prop-1-enyl)phenol in 49 % yield (92 % theoretical monomer yield) starting from birch wood. Only endogenous hydrogen from wood was consumed, and the reaction was performed using green solvents.
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| 40. |
- Galkin, Maxim V., et al.
(författare)
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Hydrogen-free catalytic fractionation of woody biomass
- 2016
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 9:23, s. 3280-3287
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Tidskriftsartikel (refereegranskat)abstract
- The pulping industry could become a biorefinery if the lignin and hemicellulose components of the lignocellulose are valorized. Conversion of lignin into well-defined aromatic chemicals is still a major challenge. Lignin depolymerization reactions often occur in parallel with irreversible condensation reactions of the formed fragments. Here, we describe a strategy that markedly suppresses the undesired condensation pathways and allows to selectively transform lignin into a few aromatic compounds. Notably, applying this strategy to woody biomass at organosolv pulping conditions, the hemicellulose, cellulose, and lignin were separated and in parallel the lignin was transformed into aromatic monomers. In addition, we were able to utilize a part of the lignocellulose as an internal source of hydrogen for the reductive lignin transformations. We hope that the presented methodology will inspire researchers in the field of lignin valorization as well as pulp producers to develop more efficient biomass fractionation processes in the future.
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