| 1. |
- Bradley, Siobhan J., et al.
(författare)
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Heterogeneity in the fluorescence of graphene and graphene oxide quantum dots
- 2017
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Ingår i: Microchimica Acta. - : Springer Science and Business Media LLC. - 0026-3672 .- 1436-5073. ; 184:3, s. 871-878
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Tidskriftsartikel (refereegranskat)abstract
- Heterogeneity is an inherent property of a wealth of real-world nanomaterials and yet rarely in the reporting of new properties is its effect sufficiently addressed. Graphene quantum dots (GQDs) – fluorescent, nanoscale fragments of graphene - are an extreme example of a heterogeneous nanomaterial. Here, top-down approaches – by far the most predominant – produce batches of particles with a distribution of sizes, shapes, extent of oxidation, chemical impurities and more. This makes characterization of these materials using bulk techniques particularly complex and comparisons of properties across different synthetic methods uninformative. In particular, it hinders the understanding of the structural origin of their fluorescence properties. We present a simple synthetic method, which produces graphene quantum dots with very low oxygen content that can be suspended in organic solvents, suggesting a very pristine material. We use this material to illustrate the limitations of interpreting complex data sets generated by heterogeneous materials and we highlight how misleading this “pristine” interpretation is by comparison with graphene oxide quantum dots synthesized using an established protocol. In addition, we report on the solvatochromic properties of these particles, discuss common characterization techniques and their limitations in attributing properties to heterogeneous materials.
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| 2. |
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| 3. |
- Craighero, Mariavittoria, 1995, et al.
(författare)
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Impact of Oligoether Side-Chain Length on the Thermoelectric Properties of a Polar Polythiophene
- 2024
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Ingår i: ACS Applied Electronic Materials. - : AMER CHEMICAL SOC. - 2637-6113. ; 6:5, s. 2909-2916
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Forskningsöversikt (refereegranskat)abstract
- Conjugated polymers with oligoether side chains make up a promising class of thermoelectric materials. In this work, the impact of the side-chain length on the thermoelectric and mechanical properties of polythiophenes is investigated. Polymers with tri-, tetra-, or hexaethylene glycol side chains are compared, and the shortest length is found to result in thin films with the highest degree of order upon doping with the p-dopant 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F(4)TCNQ). As a result, a stiff material with an electrical conductivity of up to 830 +/- 15 S cm(-1) is obtained, resulting in a thermoelectric power factor of about 21 mu W m(-1) K-2 in the case of as-cast films. Aging at ambient conditions results in an initial decrease in thermoelectric properties but then yields a highly stable performance for at least 3 months, with values of about 200 S cm(-1) and 5 mu W m(-1) K-2. Evidently, identification of the optimal side-chain length is an important criterion for the design of conjugated polymers for organic thermoelectrics.
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| 4. |
- Diaz de Zerio Mendaza, Amaia, 1986, et al.
(författare)
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Neat C60:C70 buckminsterfullerene mixtures enhance polymer solar cell performance
- 2014
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry (RSC). - 2050-7488 .- 2050-7496. ; 2:35, s. 14354-14359
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate that bulk-heterojunction blends based on neat, unsubstituted buckminsterfullerenes (C60, C70) and a thiophene–quinoxaline copolymer (TQ1) can be readily processed from solution. Atomic force and transmission electron microscopy as well as photoluminescence spectroscopy reveal that thin films with a fine-grained nanostructure can be spin-coated, which display a good photovoltaic performance. Replacement of substituted fullerenes with C60 or C70 only results in a small drop in open-circuit voltage from 0.9 V to about 0.8 V. Thus, a power conversion efficiency of up to 2.9% can be maintained if C70 is used as the acceptor material. Further improvement in photovoltaic performance to 3.6% is achieved, accompanied by a high internal quantum efficiency of 75%, if a 1 : 1 C60:C70 mixture is used as the acceptor material, due to its improved solubility in ortho-dichlorobenzene.
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| 5. |
- Dyson, M., et al.
(författare)
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Structure/Property/Processing Relationships for Organic Solar Cells
- 2018
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Ingår i: RSC Nanoscience and Nanotechnology. - : The Royal Society of Chemistry. - 1757-7136. - 9781782626749 ; 2018-January:45, s. 182-225
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Bokkapitel (övrigt vetenskapligt/konstnärligt)abstract
- Rapid developments in the field of organic solar cells have been driven by this technology's potentially advantageous traits: the environmentally friendly, low-cost generation of energy with the possibility of large area manufacturing of flexible, lightweight, semi-transparent devices, with predicted low energy payback times. Major step changes leading to vastly improved devices with ever-increasing performance have been achieved through new insights into materials design and an improved understanding of the often complex microstructure and phase morphology of organic solar cell systems. This chapter summarises the advances in synthesis, concentrating on the relevant structure/property relations and how the chemical structure affects processing and the microstructure. This is followed by a detailed discussion of classical materials science approaches that assist in gaining insights into complex materials systems, such as organic solar cell blends from the molecular to the micrometre scale, with a focus on polymer-based systems and how to apply this knowledge to future larger area processing of organic photovoltaic architectures.
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| 6. |
- Elmas, S., et al.
(författare)
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Platinum Terpyridine Metallopolymer Electrode as Cost-Effective Replacement for Bulk Platinum Catalysts in Oxygen Reduction Reaction and Hydrogen Evolution Reaction
- 2017
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Ingår i: ACS Sustainable Chemistry & Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 5:11, s. 10206-10214
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Tidskriftsartikel (refereegranskat)abstract
- Conducting polymers consisting of metal-selective coordination units and a highly conductive backbone, so-called metallopolymers, are interesting materials exposing single atoms for photo/electrocatalysis and thus represent a potential low-cost alternative for bulk or nano particulate platinum group metals (PGMs). We synthesized and fully characterized an electropolymerisable monomer bearing a pendant terpyridine unit for the selective complexation of PGMs. Electrocatalytic tests of the resulting metallopolymer, poly-[(tThTerpy)PtCl]Cl, revealed activity both in the oxygen reduction reaction and hydrogen evolution reaction. Rotating disk experiments showed the direct four-electron reduction of molecular oxygen to water at low angular velocities of the rotating electrode. Furthermore, the fabrication of Pt metallopolymers proved to be simple, nonhazardous and versatile. This proof-of-concept opens up the possibility for developing future low-cost electro-and photocatalysts to replace current systems.
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| 7. |
- Feron, K., et al.
(författare)
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Utilizing Energy Transfer in Binary and Ternary Bulk Heterojunction Organic Solar Cells
- 2016
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Ingår i: ACS Applied Materials & Interfaces. - : American Chemical Society (ACS). - 1944-8252 .- 1944-8244. ; 8:32, s. 20928-20937
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Tidskriftsartikel (refereegranskat)abstract
- Energy transfer has been identified as an important process in ternary organic solar cells. Here, we develop kinetic Monte Carlo (KMC) models to assess the impact of energy transfer in ternary and binary bulk heterojunction systems. We used fluorescence and absorption spectroscopy to determine the energy disorder and Forster radii for poly(3-hexylthiophene-2,5-diyl), [6,6]-phenyl-C61-butyric acid methyl ester, 4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl]squaraine (DIBSq), and poly(2,5-thiophene-alt-4,9-bis(2-hexyldecyl)-4,9-dihydrodithieno[3,2-c:3 ',2'-h][1,5]naphthyridine-5,10-dione). Heterogeneous energy transfer is found to be crucial in the exciton dissociation process of both binary and ternary organic semiconductor systems. Circumstances favoring energy transfer across interfaces allow relaxation of the electronic energy level requirements, meaning that a cascade structure is not required for efficient ternary organic solar cells. We explain how energy transfer can be exploited to eliminate additional energy losses in ternary bulk heterojunction solar cells, thus increasing their open-circuit voltage without loss in short-circuit current. In particular, we show that it is important that the DIBSq is located at the electron donor acceptor interface; otherwise charge carriers will be trapped in the DIBSq domain or excitons in the DIBSq domains will not be able to dissociate efficiently at an interface. KMC modeling shows that only small amounts of DIBSq (
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| 8. |
- Gedefaw, Desta Antenehe, 1971, et al.
(författare)
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Conjugated polymers based on benzodithiophene and fluorinated quinoxaline for bulk heterojunction solar cells: thiophene versus thieno[3,2-b]thiophene as π-conjugated spacers
- 2014
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Ingår i: Polymer Chemistry. - 1759-9954 .- 1759-9962. ; 5:6, s. 2083-2093
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Tidskriftsartikel (refereegranskat)abstract
- Two conjugated donor–acceptor copolymers based on a benzodithiophene donor unit and a fluorinated quinoxaline acceptor unit, spaced with either thiophene or thieno[3,2-b]thiophene π-bridges, were designed and synthesized. The effect of different π-bridges and of the processing conditions on the optical, electrical, morphological and photovoltaic properties of the polymer:fullerene blend films were investigated. The polymer containing the thieno[3,2-b]thiophene π-bridge (PBDTFQ-TT) showed a red-shifted absorption and enhanced charge carrier mobility, as compared to its analogue with the thiophene π-bridge (PBDTFQ-T), due to its narrower optical gap (by ~ 0.1 eV) and stronger inter-chain interactions, favored by the structural planarity and increased linearity of the polymer backbone, as also supported by DFT calculations. The blend of PBDTFQ-TT and PC61BM ([6,6]-phenyl-C61-butyric acid methyl ester), compared to the PBDTFQ-T:PC61BM one processed in the same conditions (by blade-coating technique), showed greatly enhanced photovoltaic performance, with more than doubled power conversion efficiency (PCE up to 5.60% for the best device) due to the increased short-circuit current density and fill factor. However, similar PCEs were also achieved for PBDTFQ-T:PC61BM-based devices by optimizing the processing conditions through the addition of 1,8-diiodooctane (DIO) as the solvent additive. Through morphological and electrical analysis of the films, produced with and without additive, it was observed that the addition of DIO greatly enhances the self-organization, and consequently the charge mobility, of the thiophene π-bridge-based polymer, while it was detrimental for the nanoscale morphology and photovoltaic performances of the thieno[3,2-b]thiophene π-bridge-based polymer in the corresponding blend.
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| 9. |
- Gedefaw, Desta Antenehe, 1971, et al.
(författare)
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Optimization of the power conversion efficiency in high bandgap pyridopyridinedithiophene-based conjugated polymers for organic photovoltaics by the random terpolymer approach
- 2017
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Ingår i: European Polymer Journal. - : Elsevier BV. - 0014-3057. ; 91, s. 92-99
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Tidskriftsartikel (refereegranskat)abstract
- We report that the organic photovoltaic (OPV) performance of wide band gap pyridopyridinedithiophene-based conjugated polymers can be significantly improved by employing the random terpolymer approach for the development of new pyridopyridinedithiophene-based conjugated polymers. This is demonstrated by the synthesis of the alternating copolymer (P1) consisting of 3,3?-difluoro-2,2?-bithiophene and pyridopyridinedithiophene and the random terpolymer (P2) containing pyridopyridinedithiophene 3,3?-difluoro-2,2?-bithiophene and thiophene. OPV devices fabricated by P1 and P2 in combination with PC61BM and PC71BM in an inverted device configuration exhibited power conversion efficiencies (PCEs) of 1.5% and 4.0%, respectively. We identified that the main reason for the enhanced performance of the OPV devices based on the P2 random copolymer was the improved morphology (miscibility) between P2 and PCBM as compared to P1. More specifically, atomic force microscopy (AFM) and scanning electron microscopy (SEM) studies revealed that the P1 based films showed rougher surface with clear crystallization/precipitation of the polymer chains even after the addition of chloronaphthalene (CN) to the chloroform processing solvent which significantly limited the short circuit current density (JSC), fill factor (FF) and overall performance of the prepared photovoltaic devices. On the other hand, P2 based films showed better miscibility with the acceptor particularly when processed using 5% CN containing chloroform solvent giving a respectable improvement in the PCE of the photovoltaic devices.
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| 10. |
- Gedefaw, Desta Antenehe, 1971, et al.
(författare)
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Synthesis and characterization of benzodithiophene and benzotriazole-based polymers for photovoltaic applications
- 2016
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Ingår i: Beilstein Journal of Organic Chemistry. - : Beilstein Institut. - 1860-5397. ; 12, s. 1629-1637
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Tidskriftsartikel (refereegranskat)abstract
- Two high bandgap benzodithiophene-benzotriazole-based polymers were synthesized via palladium-catalysed Stille coupling reaction. In order to compare the effect of the side chains on the opto-electronic and photovoltaic properties of the resulting polymers, the benzodithiophene monomers were substituted with either octylthienyl (PTzBDT-1) or dihexylthienyl (PTzBDT-2) as side groups, while the benzotriazole unit was maintained unaltered. The optical characterization, both in solution and thin-film, indicated that PTzBDT-1 has a red-shifted optical absorption compared to PTzBDT-2, likely due to a more planar conformation of the polymer backbone promoted by the lower content of alkyl side chains. The different aggregation in the solid state also affects the energetic properties of the polymers, resulting in a lower highest occupied molecular orbital (HOMO) for PTzBDT-1 with respect to PTzBDT-2. However, an unexpected behaviour is observed when the two polymers are used as a donor material, in combination with PC61BM as acceptor, in bulk heterojunction solar cells. Even though PTzBDT-1 showed favourable optical and electrochemical properties, the devices based on this polymer present a power conversion efficiency of 3.3%, considerably lower than the efficiency of 4.7% obtained for the analogous solar cells based on PTzBDT-2. The lower performance is presumably attributed to the limited solubility of the PTzBDT-1 in organic solvents resulting in enhanced aggregation and poor intermixing with the acceptor material in the active layer.
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