| 1. |
- Wang, Chuanfei, 1986-
(författare)
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Electronic Structure of π-Conjugated Materials and Their Effect on Organic Photovoltaics
- 2017
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The great tunability of structure and electronic properties of π-conjugated organic molecules/polymers combined with other advantages such as light weight and flexibility etc., have made organic-based electronics the focus of an exciting still-growing field of physics and chemistry for more than half a century. The application of organic electronics has led to the appearance of wide range of organic electronic devices mainly including organic light emitting diodes (OLED), organic field effect transistors (OFET) and organic solar cells (OSC). The application of the organic electronic devices mainly is limited by two dominant parameters, i.e., their performance and stability. Up to date, OLED has been successfully commercialized in the market while the OSC are still on the way to commercialization hindered by low efficiency and inferior stability. Understanding the energy levels of organic materials and energy level alignment of the devices is crucial to control the efficiency and stability of the OSC. In this thesis, energy levels measured by different methods are studied to explore their relationship with device properties, and the strategies on how to design efficient and stable OSC based on energy level diagrams are provided.Cyclic Voltammetry (CV) is a traditional and widely used method to probe the energy levels of organic materials, although there is little consensus on how to relate the oxidation/reduction potential ((Eox/Ered) to the vacuum level. Ultraviolet Photoelectron Spectroscopy (UPS) can be used to directly detect vertical ionization potential (IP) of organic materials. In this thesis, a linear relationship of IP and Eox was found, with a slope equal to unity. The relationship provides for easy conversion of values obtained by the two techniques, enabling complementarily use in designing and fabricating efficient and stable OSC. A popular rule of thumb is that the offset between the LUMO levels of donor and acceptor should be 0.3 eV, according to which a binary solar cell with the minimum voltage losses around 0.49 V was designed here.Introduction of the ternary blend as active layer is an efficient way to improve both efficiency and stability of the OSC. Based on our studied energy-level diagram within the integer charge transfer (ICT) model, we designed ternary solar cells with enhanced open circuit voltage for the first time and improved thermal stability compared to reference binary ones. The ternary solar cell with minimum voltage losses was developed by combining two donor materials with same ionization potential and positive ICT energy while featuring complementary optical absorption. Furthermore, the fullerene acceptor was chosen so that the energy of the positive ICT state of the two donor polymers is equal to the energy of negative ICT state of the fullerene, which can enhance dissociation of all polymer donor and fullerene acceptor excitons and suppress bimolecular and trap-assistant recombination.Rapid development of non-fullerene acceptors in the last two years affords more recipes of designing both efficient and stabile OSC. We show in this thesis how non-fullerene acceptors successfully can be used to design ternary solar cells with both enhanced efficiency and thermal stability. Besides improving the efficiency of the devices, understanding of the stability and degradation mechanism is another key issue. The degradation of conjugated molecules/polymers often follow many complicated pathways and at the same time many factors for degradation are coupled with each other. Therefore, the degradation of non-fullerene acceptors was investigated in darkness by photoelectron spectroscopy in this thesis with the in-situ method of controlling exposure of O2 and water vapor separately.
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| 2. |
- Xu, Weidong, 1988-, et al.
(författare)
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Rational molecular passivation for high-performance perovskite light-emitting diodes
- 2019
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Ingår i: Nature Photonics. - : Springer Nature Publishing AG. - 1749-4885 .- 1749-4893. ; 13:6, s. 418-424
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Tidskriftsartikel (refereegranskat)abstract
- A major efficiency limit for solution-processed perovskite optoelectronic devices, for example light-emitting diodes, is trap-mediated non-radiative losses. Defect passivation using organic molecules has been identified as an attractive approach to tackle this issue. However, implementation of this approach has been hindered by a lack of deep understanding of how the molecular structures influence the effectiveness of passivation. We show that the so far largely ignored hydrogen bonds play a critical role in affecting the passivation. By weakening the hydrogen bonding between the passivating functional moieties and the organic cation featuring in the perovskite, we significantly enhance the interaction with defect sites and minimize non-radiative recombination losses. Consequently, we achieve exceptionally high-performance near-infrared perovskite light-emitting diodes with a record external quantum efficiency of 21.6%. In addition, our passivated perovskite light-emitting diodes maintain a high external quantum efficiency of 20.1% and a wall-plug efficiency of 11.0% at a high current density of 200 mA cm−2, making them more attractive than the most efficient organic and quantum-dot light-emitting diodes at high excitations.
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| 3. |
- Qin, Leiqiang, 1987-, et al.
(författare)
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Flexible Solid-State Asymmetric Supercapacitors with Enhanced Performance Enabled by Free-Standing MXene-Biopolymer Nanocomposites and Hierarchical Graphene-RuOx Paper Electrodes
- 2020
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Ingår i: Batteries & Supercaps. - : WILEY-V C H VERLAG GMBH. - 2566-6223. ; 3:7, s. 604-610
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Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional (2D) transition metal carbides and carbonitrides, called MXenes, with metallic conductivity and hydrophilic surfaces, show great promise as electrode materials for supercapacitors. A major drawback of 2D nanomaterials is the re-stacking of the nanosheets, which prevents full utilization of surface area and blocks the access of the electrolyte. In this study, a free-standing nanocomposite paper electrode is realized by combining Mo1.33C MXene and positively charged biopolymer lignin (the second most abundant biopolymer in nature, L-DEA). The self-assembled layered architecture with alternating polymer and MXene flakes increases the interlayer space to promote ion transport, and with combining charge storage capability of the lignin derivative and MXene in an interpenetrating MXene/L-DEA nanocomposite, which offers an impressive capacitance of 503.7 F g(-1). Moreover, we demonstrate flexible solid-state asymmetric supercapacitors (ASCs) using Mo1.33C@L-DEA as the negative electrode and electrochemically exfoliated graphene with ruthenium oxide (EG@RuOx) as the positive electrode. This asymmetric device operates at a voltage window of 1.35 V, which is about two times wider than that of a symmetric Mo1.33C@L-DEA based supercapacitor. Finally, the ASCs can deliver an energy density of 51.9 Wh kg(-1) at a power density of 338.5 W kg(-1), with 86 % capacitance retention after 10000 charge-discharge cycles.
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| 4. |
- Adam, Rania Elhadi, 1978-, et al.
(författare)
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Graphene-based plasmonic nanocomposites for highly enhanced solar-driven photocatalytic activities
- 2019
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Ingår i: RSC Advances. - Cambridge : Royal Meteorological Society. - 2046-2069. ; 9:52, s. 30585-30598
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Tidskriftsartikel (refereegranskat)abstract
- High-efficiency photocatalysts are crucial for the removal of organic pollutants and environmental sustainability. In the present work, we report on a new low-temperature hydrothermal chemical method, assisted by ultrasonication, to synthesize disruptive plasmonic ZnO/graphene/Ag/AgI nanocomposites for solar-driven photocatalysis. The plasmonic nanocomposites were investigated by a wide range of characterization techniques, confirming successful formation of photocatalysts with excellent degradation efficiency. Using Congo red as a model dye molecule, our experimental results demonstrated a photocatalytic reactivity exceeding 90% efficiency after one hour simulated solar irradiation. The significantly enhanced degradation efficiency is attributed to improved electronic properties of the nanocomposites by hybridization of the graphene and to the addition of Ag/AgI which generates a strong surface plasmon resonance effect in the metallic silver further improving the photocatalytic activity and stability under solar irradiation. Scavenger experiments suggest that superoxide and hydroxyl radicals are responsible for the photodegradation of Congo red. Our findings are important for the fundamental understanding of the photocatalytic mechanism of ZnO/graphene/Ag/AgI nanocomposites and can lead to further development of novel efficient photocatalyst materials.
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| 5. |
- Adam, Rania Elhadi, 1978-, et al.
(författare)
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Synthesis of Mg-doped ZnO NPs via a chemical low-temperature method and investigation of the efficient photocatalytic activity for the degradation of dyes under solar light
- 2020
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Ingår i: Solid State Sciences. - : Elsevier. - 1293-2558 .- 1873-3085. ; 99
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Tidskriftsartikel (refereegranskat)abstract
- Doped semiconductors nanostructures (NSs) have shown great interest as a potential for green and efficient photocatalysis activities. Magnesium (Mg)-doped zinc oxide (ZnO) nanoparticles (NPs) has been synthesized by a one-step chemical low temperature (60 °C) co-precipitation method without further calcination and their photocatalytic performance for photodegradation of Methylene blue (MB) dye under the illumination of solar light is investigated. The crystal structure of the synthesized NPs is examined by X-ray diffraction (XRD). XRD data indicates a slight shift towards higher 2θ angle in Mg-doped samples as compared to the pure ZnO NPs which suggest the incorporation of Mg2+ into ZnO crystal lattice. X-ray photoelectron spectroscopy (XPS), UV–Vis spectrophotometer and cathodoluminescence (CL) spectroscopy, were used to study electronics, and optical properties, respectively. The XPS analysis confirms the substitution of the Zn2+ by the Mg2+ into the ZnO crystal lattice in agreement with the XRD data. The photocatalytic activities showed a significant enhancement of the Mg-doped ZnO NPs in comparison with pure ZnO NPs. Hole/radical scavengers were used to reveal the mechanism of the photodegradation. It was found that the addition of the Mg to the ZnO lattices increases the absorption of the hydroxyl ions at the surface of the NPs and hence acts as a trap site leading to decrease the electron-hole pair and consequently enhancing the photodegradation.
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| 6. |
- Chen, Shangzhi, et al.
(författare)
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Unraveling vertical inhomogeneity in vapour phase polymerized PEDOT:Tos films
- 2020
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 8, s. 18726-18734
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Tidskriftsartikel (refereegranskat)abstract
- The conducting polymer poly(3,4-ethylenedioxythiophene) (PEDOT) forms a promising alternative to conventional inorganic conductors, where deposition of thin films via vapour phase polymerization (VPP) has gained particular interest owing to high electrical conductivity within the plane of the film. The conductivity perpendicular to the film is typically much lower, which may be related not only to preferential alignment of PEDOT crystallites but also to vertical stratification across the film. In this study, we reveal non-linear vertical microstructural variations across VPP PEDOT:Tos thin films, as well as significant differences in doping level between the top and bottom surfaces. The results are consistent with a VPP mechanism based on diffusion-limited transport of polymerization precursors. Conducting polymer films with vertical inhomogeneity may find applications in gradient-index optics, functionally graded thermoelectrics, and optoelectronic devices requiring gradient doping.
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| 7. |
- Chen, Yongzhen, 1990-, et al.
(författare)
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Understanding Interface Dipoles at an Electron Transport Material/Electrode Modifier for Organic Electronics
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:39, s. 47218-47225
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Tidskriftsartikel (refereegranskat)abstract
- Interface dipoles formed at an electrolyte/electrode interface have been widely studied and interpreted using the "double dipole step" model, where the dipole vector is determined by the size and/or range of motion of the charged ions. Some electron transport materials (ETMs) with lone pairs of electrons on heteroatoms exhibit a similar interfacial behavior. However, the origin of the dipoles in such materials has not yet been explored in great depth. Herein, we systematically investigate the influence of the lone pair of electrons on the interface dipole through three pyridine derivatives B2-B4PyMPM. Experiments show that different positions of nitrogen atoms in the three materials give rise to different hydrogen bonds and molecular orientations, thereby affecting the areal density and direction of the lone pair of electrons. The interface dipoles of the three materials predicted by the "double dipole step" model are in good agreement with the ultraviolet photoelectron spectroscopy results both in spin-coated and vacuum-deposited films. These findings help to better understand the ETMs/electrode interfacial behaviors and provide new guidelines for the molecular design of the interlayer.
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| 8. |
- Elhadi Adam, Rania, et al.
(författare)
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ZnO/Ag/Ag2WO4 photo-electrodes with plasmonic behavior for enhanced photoelectrochemical water oxidation
- 2019
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Ingår i: RSC Advances. - : Royal Society of Chemistry. - 2046-2069. ; 9:15, s. 8271-8279
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Tidskriftsartikel (refereegranskat)abstract
- Ag-based compounds are excellent co-catalyst that can enhance harvesting visible light and increase photo-generated charge carrier separation owing to its surface plasmon resonance (SPR) effect in photoelectrochemical (PEC) applications. However, the PEC performance of a ZnO/Ag/Ag2WO4 heterostructure with SPR behavior has not been fully studied so far. Here we report the preparation of a ZnO/Ag/Ag2WO4 photo-electrode with SPR behavior by a low temperature hydrothermal chemical growth method followed by a successive ionic layer adsorption and reaction (SILAR) method. The properties of the prepared samples were investigated by different characterization techniques, which confirm that Ag/Ag2WO4 was deposited on the ZnO NRs. The Ag2WO4/Ag/ZnO photo-electrode showed an enhancement in PEC performance compared to bare ZnO NRs. The observed enhancement is attributed to the red shift of the optical absorption spectrum of the Ag2WO4/Ag/ZnO to the visible region (>400 nm) and to the SPR effect of surface metallic silver (Ag0) particles from the Ag/Ag2WO4 that could generate electron–hole pairs under illumination of low energy visible sun light. Finally, we proposed the PEC mechanism of the Ag2WO4/Ag/ZnO photo-electrode with an energy band structure and possible electron–hole separation and transportation in the ZnO/Ag/Ag2WO4 heterostructure with SPR effect for water oxidation. ER
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| 9. |
- Ibupoto, Zafar, et al.
(författare)
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MoSx@NiO Composite Nanostructures : An Advanced Nonprecious Catalyst for Hydrogen Evolution Reaction in Alkaline Media
- 2019
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Ingår i: Advanced Functional Materials. - : John Wiley & Sons. - 1616-301X .- 1616-3028. ; 29:7
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Tidskriftsartikel (refereegranskat)abstract
- The design of the earth‐abundant, nonprecious, efficient, and stable electrocatalysts for efficient hydrogen evolution reaction (HER) in alkaline media is a hot research topic in the field of renewable energies. A heterostructured system composed of MoSx deposited on NiO nanostructures (MoSx@NiO) as a robust catalyst for water splitting is proposed here. NiO nanosponges are applied as cocatalyst for MoS2 in alkaline media. Both NiO and MoS2@NiO composites are prepared by a hydrothermal method. The NiO nanostructures exhibit sponge‐like morphology and are completely covered by the sheet‐like MoS2. The NiO and MoS2 exhibit cubic and hexagonal phases, respectively. In the MoSx@NiO composite, the HER experiment in 1 m KOH electrolyte results in a low overpotential (406 mV) to produce 10 mA cm−2 current density. The Tafel slope for that case is 43 mV per decade, which is the lowest ever achieved for MoS2‐based electrocatalyst in alkaline media. The catalyst is highly stable for at least 13 h, with no decrease in the current density. This simple, cost‐effective, and environmentally friendly methodology can pave the way for exploitation of MoSx@NiO composite catalysts not only for water splitting, but also for other applications such as lithium ion batteries, and fuel cells.
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| 10. |
- Li, Zaifang, et al.
(författare)
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A Free-Standing High-Output Power Density Thermoelectric Device Based on Structure-Ordered PEDOT:PSS
- 2018
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Ingår i: Advanced Electronic Materials. - : Wiley-VCH Verlagsgesellschaft. - 2199-160X. ; 4:2
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Tidskriftsartikel (refereegranskat)abstract
- A free-standing high-output power density polymeric thermoelectric (TE) device is realized based on a highly conductive (approximate to 2500 S cm(-1)) structure-ordered poly(3,4-ethylenedioxythiophene):polystyrene sulfonate film (denoted as FS-PEDOT:PSS) with a Seebeck coefficient of 20.6 mu V K-1, an in-plane thermal conductivity of 0.64 W m(-1) K-1, and a peak power factor of 107 mu W K-2 m(-1) at room temperature. Under a small temperature gradient of 29 K, the TE device demonstrates a maximum output power density of 99 +/- 18.7 mu W cm(-2), which is the highest value achieved in pristine PEDOT:PSS based TE devices. In addition, a fivefold output power is demonstrated by series connecting five devices into a flexible thermoelectric module. The simplicity of assembling the films into flexible thermoelectric modules, the low out-of-plane thermal conductivity of 0.27 W m(-1) K-1, and free-standing feature indicates the potential to integrate the FS-PEDOT:PSS TE modules with textiles to power wearable electronics by harvesting human bodys heat. In addition to the high power factor, the high thermal stability of the FS-PEDOT:PSS films up to 250 degrees C is confirmed by in situ temperature-dependent X-ray diffraction and grazing incident wide angle X-ray scattering, which makes the FS-PEDOT:PSS films promising candidates for thermoelectric applications.
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