| 1. |
- Ajjan, Fátima, 1986-, et al.
(författare)
-
Doped Conjugated Polymer Enclosing a Redox Polymer : Wiring Polyquinones with Poly(3,4‐Ethylenedioxythiophene)
- 2020
-
Ingår i: Advanced Energy and Sustainability Research. - : John Wiley & Sons. - 2699-9412. ; 1:2
-
Tidskriftsartikel (refereegranskat)abstract
- The mass implementation of renewable energies is limited by the absence of efficient and affordable technology to store electrical energy. Thus, the development of new materials is needed to improve the performance of actual devices such as batteries or supercapacitors. Herein, the facile consecutive chemically oxidative polymerization of poly(1-amino-5-chloroanthraquinone) (PACA) and poly(3,4-ethylenedioxythiophene (PEDOT) resulting in a water dispersible material PACA-PEDOT is shown. The water-based slurry made of PACA-PEDOT nanoparticles can be processed as film coated in ambient atmosphere, a critical feature for scaling up the electrode manufacturing. The novel redox polymer electrode is a nanocomposite that withstands rapid charging (16 A g−1) and delivers high power (5000 W kg−1). At lower current density its storage capacity is high (198 mAh g−1) and displays improved cycling stability (60% after 5000 cycles). Its great electrochemical performance results from the combination of the redox reversibility of the quinone groups in PACA that allows a high amount of charge storage via Faradaic reactions and the high electronic conductivity of PEDOT to access to the redox-active sites. These promising results demonstrate the potential of PACA-PEDOT to make easily organic electrodes from a water-coating process, without toxic metals, and operating in non-flammable aqueous electrolyte for large scale pseudocapacitors.
|
|
| 2. |
- Bian, Qingzhen, 1988-
(författare)
-
Excitonic and charge carrier transport in organic materials and device applications
- 2020
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- With the potential for future commercial use, organic electronics have been intensively studied for the last few decades. To exploit the next generation of high-performance devices, detailed study of the underlying physics is essential. Excitonic and charge carrier transport plays a critical role in device performance and related studies have attracted a lot of attention in recent decades. This thesis particularly focused on excitonic and charge carrier transport in organic materials and related device applications.In natural light harvesting systems, such as the reaction centers of purple bacteria, quantum coherence has been proposed to be present as a contributor to the related charge and energy transport processes, and almost 100% charge conversion is present in these efficient biological systems. This high energy conversion efficiency inspires the idea that if a similar strategy was used in artificial energy conversion devices such as organic photovoltaics, etc., this could significantly enhance the device’s performance. In the first study, the charge separation process in some donor/acceptor blends was investigated. The contribution of quantum coherence to device performance was studied in detail using several steady state and ultrafast transient techniques. In one efficient donor/acceptor blend, a pronounced coherence of charge separation was identified, which contributed to the enhancement of the photocurrent generation, which finally resulted in efficient device performance.For the light emitting diodes, triplet excitons harvesting plays a critical role in device performance. In the thermally activated delayed fluorescence (TADF) materials, due to an efficient reverse intersystem process from triplet excitons to singlet excitons, the losses due to triplet excitons were suppressed. As a result, a desired high quantum yield has been achieved. To enhance device efficiency, the detailed study of the upconversion physics between triplet and singlet is needed. Previous studies have proposed some physical models to explain this efficient upconversion process, while the nature of this physical process is still under debate and unclear. In my second work, we studied the exciton kinetics in two different TADF materials. These TADF materials were inserted in a protein fibril host, and the resulting protein scaffold was able to modify the geometric configuration of the related TADF molecule. As a result, an enhancement of the photoluminescence quantum yield was achieved.To achieve efficient device performance in organic electronics, the physical processes at the metal/material interface and charge carrier injection/extraction, also play a critical role. Efficient charge injection can be achieved by Ohmic contact, and charge injection/extraction of metal/organic materials has been intensively studied in the last few decades. In my third study, an efficient hole transport material based on the biopolymer DNA was introduced. A hole doping process was found in the hybrid materials and contributes to the Ohmic contacts. The hybrid material can be used in different organic electronics devices, such as field effect transistors, light emitting diodes and solar cells, and thus demonstrates a general application capability.In organic photovoltaics, the loss from the open circuit photovoltages has been an Achilles’ heel for further enhancement of device performance. The voltage loss includes the radiative and non-radiative value, and intensive studies have focused on how to suppress losses from the non-radiative channel. In my fourth study, the non-radiative voltage loss was studied in a series of terpolymer blends and ternary blends. Compared to the ternary blends, a decreased nonradiative loss was found in the terpolymer blends.
|
|
| 3. |
- Bian, Qingzhen, 1988-, et al.
(författare)
-
Vibronic coherence contributes to photocurrent generation in organic semiconductor heterojunction diodes
- 2020
-
Ingår i: Nature Communications. - : NATURE PUBLISHING GROUP. - 2041-1723. ; 11:1
-
Tidskriftsartikel (refereegranskat)abstract
- Charge separation dynamics after the absorption of a photon is a fundamental process relevant both for photosynthetic reaction centers and artificial solar conversion devices. It has been proposed that quantum coherence plays a role in the formation of charge carriers in organic photovoltaics, but experimental proofs have been lacking. Here we report experimental evidence of coherence in the charge separation process in organic donor/acceptor heterojunctions, in the form of low frequency oscillatory signature in the kinetics of the transient absorption and nonlinear two-dimensional photocurrent spectroscopy. The coherence plays a decisive role in the initial 200 femtoseconds as we observe distinct experimental signatures of coherent photocurrent generation. This coherent process breaks the energy barrier limitation for charge formation, thus competing with excitation energy transfer. The physics may inspire the design of new photovoltaic materials with high device performance, which explore the quantum effects in the next-generation optoelectronic applications.
|
|
| 4. |
- Fernandez-Benito, Amparo, et al.
(författare)
-
Green and Scalable Biopolymer-Based Aqueous Polyelectrolyte Complexes for Zinc-Ion Charge Storage Devices
- 2023
-
Ingår i: ChemElectroChem. - : WILEY-V C H VERLAG GMBH. - 2196-0216. ; 10:2
-
Tidskriftsartikel (refereegranskat)abstract
- Green and scalable materials are essential to fulfill the need of electrification for transitioning into a fossil-fuels free society, and sustainability is a requirement for all new technologies. Rechargeable batteries are one of the most important elements for electrification, enabling the transition to mobile electronics, electrical vehicles and grid storage. We here report synthesis and characterization of polyelectrolyte complexes of alginate and chitosan, both biopolymers deriving from the sea, for transport of zinc ions in hydrogel electrolytes. We have used vibrational spectroscopy, thermal measurements and microscopy, as well as transport measurements with ohmic or blocking contacts. The transference number for zinc ions is close to 1, the conductivity is approximate to 10 mS/cm, with stability at Zn interfaces seen through 7000 cycles in symmetric zinc//zinc cell. A zinc ion aqueous electrolyte was prepared from blends of chitosan and alginate, by using a simple and scalable route. These green zinc ion electrolytes exhibit a stability window up to 2 V, a zinc ion transference number close to 1, and electrochemical cyclability over 7000 cycles at interfaces to zinc. This biologically derived polyelectrolyte complex offers many possibilities for optimizing transport and stability at electrode interfaces.image
|
|
| 5. |
- Harillo-Baños, Albert, et al.
(författare)
-
High-Throughput Screening of Blade-Coated Polymer:Polymer Solar Cells: Solvent Determines Achievable Performance
- 2022
-
Ingår i: ChemSusChem. - : Wiley. - 1864-5631 .- 1864-564X. ; 15:4
-
Tidskriftsartikel (refereegranskat)abstract
- Optimization of a new system for organic solar cells is a multiparametric analysis problem that requires substantial efforts in terms of time and resources. The strong microstructure-dependent performance of polymer:polymer cells makes them particularly difficult to optimize, or to translate previous knowledge from spin coating into more scalable techniques. In this work, the photovoltaic performance of blade-coated devices was studied based on the promising polymer:polymer system PBDB-T and PF5-Y5 as donor and acceptor, respectively. Using the recently developed high-throughput methodology, the system was optimized for multiple variables, including solvent system, active layer composition, ratio, and thickness, among others, by fabricating more than 500 devices with less than 24 mg of each component. As a result, the power conversion efficiency of the blade-coated devices varied from 0.08 to 6.43 % in the best device. The performed statistical analysis of the large experimental data obtained showed that solvent selection had the major impact on the final device performance due to its influence on the active layer microstructure. As a conclusion, the use of the plot of the device efficiency in the Hansen space was proposed as a powerful tool to guide solvent selection in organic photovoltaics.
|
|
| 6. |
- Kuang, Chaoyang, 1988-
(författare)
-
Interface-Assisted Perovskite Modulations for High-Performance Light-Emitting Diodes
- 2021
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Metal halide perovskites have emerged as a class of promising materials for a wide range of optoelectronic devices. Compared with traditional inorganic and organic semiconductors, perovskite materials can be easily processed via solution-based techniques at low temperatures and exhibit high photo-luminescence efficiency, outstanding colour purity, and superior charge transport properties, showing great promise for cost-effective and high-performance light-emitting diodes (LEDs).Since the first demonstration of room-temperature operating perovskite-based LEDs (PeLEDs) in 2014, various useful strategies on optimizing perovskite emissive materials and device structures have been developed, leading to notably enhanced device performance of PeLEDs during the last several years. Nevertheless, despite rapid progress in improving the external quantum efficiencies (EQEs) of PeLEDs, which are now approaching those of commercialized technologies, the operational stability of state-of-the-art PeLEDs remains poor, presenting a critical challenge for their practical applications and commercialization. Besides, a majority of the optimization strategies demonstrated for PeLEDs derivate from those developed for either perovskite photovoltaics or prevailing light-emitting technologies, e.g., organic- and quantum-dot-based LEDs. Although these strategies are helpful, more comprehensive investigations and in-depth understanding of factors affecting the property of perovskite emissive layers and the device performance of ensuing PeLEDs are highly desirable to foster further advancements of this promising technology.In this thesis, we focus our study on near-infrared PeLEDs based on triiodide perovskite emissive layers processed from precursor solutions. We systematically investigate the critical effects of precursors, substrates, and additives on the film quality of perovskite emissive layers. With the indepth understanding of the perovskite crystallization process, we developed a range of effective interface-assisted strategies on modulating the perovskite emissive layers, which enable us to achieve PeLEDs with high EQEs and excellent long-term operational stability beyond the state-of-the-art.In the first study, we unveiled the synergistic effect of precursor stoichiometry and interfacial reactions for PeLEDs. We reveal that ZnO efficiently deprotonates the organic cations, which promotes the formation of highly emissive perovskites from precursor solution with excess organic components, leading to the achievement of PeLEDs with a high EQE of 19.6 %. In the second study, we presented that such ZnO deprotonation process of excess organic cations can also assist the cation exchange process between cesium-formamidinium (FA-Cs) cation exchange, enabling low-temperature fabrication of pure-phase Cs-FA mixed cation perovskite films with widely tunable emissions peaking between 715 nm and 800 nm as well as high-performance devices with peak EQEs over 15%.In spite of enhanced device efficiency realized by the perovskite crystallization modulation, this ZnO deprotonation process places a detrimental effect on the stability of the PeLEDs, which can be accelerated by Joule heating and high electric fields during the device operation. In the third study, we, therefore, demonstrated the role of ZnO in catalyzing an efficient amidation reaction between incorporated dicarboxylic acid additives and excess FAI, preventing the above-mentioned harmful interfacial reaction. With this strategy, the operational half lifetime of the resulting PeLEDs was improved to 682 hours at 20 mA/cm2 while maintaining a high device efficiency of 18.6%.In the last work, we emphasized that the rational design of molecular reactions between two additives (diamine and triacrylate) and perovskite components with the assistance of ZnO substrates can subsequently eliminate the negative effect introduced by additive, reduce the defect density and enhance the crystal orientation in the perovskite emissive layers. The rational understanding of interfacial interactions between perovskite, additives, and ZnO, enabled us to achieve PeLEDs with a device efficiency of 23.8% as well as an outstanding operational stability T70 (reduction to 70% of initial efficiency) lifetime of 290 hours at 20 mA/cm2.The study in this thesis developed effective interface-assisted modulation strategies for high-quality perovskites towards highly efficient and stable PeLEDs for commercialization. A thorough understanding of perovskite chemistry-property-performance modulation assisted by interfaces is indispensable for the future development of PeLEDs and our study took an important step.
|
|
| 7. |
- Liu, Lianlian, 1988-, et al.
(författare)
-
Black Charcoal for Green and Scalable Wooden Electrodes for Supercapabatteries
- 2022
-
Ingår i: Energy Technology. - : Wiley-VCH Verlag GMBH. - 2194-4288 .- 2194-4296. ; 10:3
-
Tidskriftsartikel (refereegranskat)abstract
- A green, though black, sustainable and low-cost carbon material-charcoal produced from wood-is developed for electricity storage. Charcoal electrodes are fabricated by ball-milling charcoal and adding protein nanofibril binders. The charcoal electrode presents a capacitance of 360 F g(-1) and a conductivity of 0.2 S m(-1). A pair of redox peaks is observed in the cyclic voltammetry and assigned to originate from quinone groups. Compared with other wooden electrodes, these charcoal electrodes display better cycling stability with 88% capacity retention after 1000 cycles. Their discharge capacity is 2.5 times that of lignosulfonate/graphite hybrid electrodes.
|
|
| 8. |
- Liu, Lianlian, 1988-
(författare)
-
Renewable and Scalable Energy Storage Materials Derived from Quinones in Biomass
- 2020
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Currently there is an urgent need to reduce the use of fossil fuels, and efficient sustainable energy harvesters from sun and wind have been developed and are widely used for electricity generation. Storage of electrical energy is accordingly necessary to accommodate the time varying supply of wind and solar electricity. Quinones (Q) are attractive as energy storage materials due to their high theoretical charge density and the renewable and abundant source – biomass. Plant-based biomass materials – such as lignin and humic acids – contain redox active Q-groups that potentially could be used for electricity storage instead of simply burning the biomass, which releases CO2, CH4, NOx, and SOx. Lignin accounts for 20-30% of the biomass weight and contains a sizable fraction of Q-structures. However, utilization of lignin for large scale energy storage is still a challenging task, as lignin is electrically insulating and conductive materials are required to get access to the generated electrons in the bulk. Various relatively expensive materials, such as conductive polymers and various carbon materials (carbon nanotubes, active carbon, graphene, etc.) have been combined with lignin, resulting in hybrid materials for energy storage. However, as the scale required for production of charge storage devices is huge it is of outmost importance to reduce the cost and therefore investigate low-cost conductive materials. In this thesis, common graphite flakes are combined with the lignin derivative lignosulphonate (LS) via a solvent free ball-milling process, followed by treatment with water and resulting in a paste that can be processed into electrodes. Similarly, humic acid derived from peat, lignite that contains a large amount of Q-groups is also fabricated into electrode with graphite via the ball-milling process. In order to further reduce the impact on environment during the extraction of Q-materials from biomass, barks that contain as much as 30% of lignin are directly used for energy storage via co-milling with pristine graphite to generate the biomass/graphite hybrid material electrodes. However, larger weight fraction of Q are required to further improve the electrochemical performance of these electrodes and Q chemicals (QCs) that also originate from biomass are introduced to fabricate the QCs/graphite electrodes with an increased capacity. Additionally, self-discharge mechanism is studied on the LS/graphite hybrid material electrodes, which provides instructions to achieve a low self-discharge rate.Overall, this study has brought us one step forward on the establishing of scalable, sustainable, and cost-effective energy storage systems using aqueous electrolytes.
|
|
| 9. |
- Liu, Yanfeng, 1992-
(författare)
-
Studying Morphology Formation and Charge Separation in Organic Solar Cells
- 2021
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- We are currently living in the era of automation and artificial intelligence, which requires more energy than ever before. Meanwhile, the reduction of carbon footprint is needed for keeping the environment sustainable. Exploring green energy is crucial. Solar power is one of the green energy sources. The apparatus that converts solar energy to electricity is a solar cell. Organic solar cells (OSCs), employing organic materials absorbing solar radiation and converting to electricity have got extensive attention in the last decades due to their unique advantages like lightweight, semi-transparency, and potential industrialization. In most cases, an OSC composes of two different organic semiconductors as electron donor and acceptor to form a photoactive layer with a bulk heterojunction (BHJ) structure, and sandwiched between the electron and hole transport layers and then two electrodes. The morphology of the BHJ plays a crucial role in the device's performance, and it is a result of a complicated interplay between donor, acceptor, and solvent during the film drying from a solution. Thus, in-situ monitoring the film drying during solvent evaporation could deepen understanding of the mechanism of the morphology formation. A versatile multiple spectroscopic setup is assembled for this purpose, which can record laser scattering, steady-state photoluminescence (PL), time-resolved photoluminescence (TRPL), and white-light absorption during film formation. By comparing the drying dynamics of three different blend systems with their corresponding pristine films, we find that the blend film formation and its final morphology are more dominated by the component with a higher molecular weight. Different PL and TRPL quenching profiles between fullerene- and non-fullerene-based systems provide hints about different donor-acceptor interactions. Moreover, with the help of TRPL, the relative change of quantum yield during film formation can be calculated. Besides, this setup is also proved suitable for studying mechanisms behind device optimization processes, like the usage of solvent additives. One of the unique features of OSCs based on non-fullerene acceptors is the highly efficient hole transfer from the acceptor to the donor, sometimes even under zero or negative energetic offsets. However, in these cases the mechanism of hole transfer has not been fully understood. By studying hole transfer at the donor:acceptor interface in different material systems and device configurations, we highlight the role of electric field on the charge separation of OSCs when energetic offsets are not enough. To achieve better device performance, engineering the photoelectric properties of interfacial layers is equally essential. A good interfacial layer can facilitate carrier extraction and reduce carrier recombination. We demonstrate that adding MXenes into the PEDOT:PSS can increase the conductivity of this composite hole transport layer, without sacrificing its optical transparency and work function.
|
|
| 10. |
- Rodriguez Martinez, Xabier, et al.
(författare)
-
Laminated Organic Photovoltaic Modules for Agrivoltaics and Beyond: An Outdoor Stability Study of All-Polymer and Polymer:Small Molecule Blends
- 2023
-
Ingår i: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 33:10
-
Tidskriftsartikel (refereegranskat)abstract
- The integration of organic photovoltaic (OPV) modules on greenhouses is an encouraging practice to offset the energy demands of crop growth and provide extra functionality to dedicated farmland. Nevertheless, such OPV devices must meet certain optical and stability requirements to turn net zero energy greenhouse systems a reality. Here a donor:acceptor polymer blend is optimized for its use in laminated devices while matching the optical needs of crops. Optical modeling is performed and a greenhouse figure-of-merit is introduced to benchmark the trade-off between photovoltaic performance and transparency for both chloroplasts and humans. Balanced donor:acceptor ratios result in better-performing and more thermally stable devices than acceptor-enriched counterparts. The optimized polymer blend and state-of-the-art polymer:small-molecule blends are next transferred to 25 cm(2) laminated modules processed entirely from solution and in ambient conditions. The modules are mounted on a greenhouse as standalone or 4-terminal tandem configurations and their outdoor stability is tracked for months. The study reveals degradation modes undetectable under laboratory conditions such as module delamination, which accounts for 10-20% loss in active area. Among the active layers tested, polymer:fullerene blends are the most stable and position as robust light harvesters in future building-integrated OPV systems.
|
|
| 11. |
- Rodriguez Martinez, Xabier, et al.
(författare)
-
Matching electron transport layers with a non-halogenated and low synthetic complexity polymer:fullerene blend for efficient outdoor and indoor organic photovoltaics
- 2022
-
Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 10:19, s. 10768-10779
-
Tidskriftsartikel (refereegranskat)abstract
- The desired attributes of organic photovoltaics (OPV) as a low cost and sustainable energy harvesting technology demand the use of non-halogenated solvent processing for the photoactive layer (PAL) materials, preferably of low synthetic complexity (SC) and without compromising the power conversion efficiency (PCE). Despite their record PCEs, most donor-acceptor conjugated copolymers in combination with non-fullerene acceptors are still far from upscaling due to their high cost and SC. Here we present a non-halogenated and low SC ink formulation for the PAL of organic solar cells, comprising PTQ10 and PC61BM as donor and acceptor materials, respectively, showing a record PCE of 7.5% in blade coated devices under 1 sun, and 19.9% under indoor LED conditions. We further study the compatibility of the PAL with 5 different electron transport layers (ETLs) in inverted architecture. We identify that commercial ZnO-based formulations together with a methanol-based polyethyleneimine-Zn (PEI-Zn) chelated ETL ink are the most suitable interlayers for outdoor conditions, providing fill factors as high as 74% and excellent thickness tolerance (up to 150 nm for the ETL, and >200 nm for the PAL). In indoor environments, SnO2 shows superior performance as it does not require UV photoactivation. Semi-transparent devices manufactured entirely in air via lamination show indoor PCEs exceeding 10% while retaining more than 80% of the initial performance after 400 and 350 hours of thermal and light stress, respectively. As a result, PTQ10:PC61BM combined with either PEI-Zn or SnO2 is currently positioned as a promising system for industrialisation of low cost, multipurpose OPV modules.
|
|
| 12. |
- Wang, Heyong, 1989-
(författare)
-
High-Quality Perovskite Films for Efficient and Stable Light-Emitting Diodes
- 2020
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Metal halide perovskites have attracted significant attention for light-emitting applications, because of their excellent properties, such as high photoluminescence quantum yields (PLQYs), good charge mobility, narrow emission bandwidth, readily tunable emission spectra ranging from ultraviolet to near-infrared, and solution processability. Since the first room-temperature perovskite-based light-emitting diodes (PeLEDs) reported in 2014, tremendous efforts have been made to promote the efficiencies of PeLEDs, including theoretical simulation, materials design, and device engineering. To reach the ultimate goal of commercialization, PeLEDs with both high-efficiency and long-term operational stability are desired. Achieving high-quality perovskite emissive films is key towards this goal. Centering around the high-quality perovskite films, in this thesis, we demonstrate effective synthesis strategies for the deposition of high-quality perovskite films (including both three-dimensional and mixed-dimensional perovskites) and investigate the effects of ion migration in the perovskite films on the performance of PeLEDs.Due to the fast crystallization nature of perovskites and the low formation energy of defects, controlling the crystallization processes of these films has proved to be an effective approach for achieving high-quality perovskite films. For three-dimensional (3D) perovskite films, we have controlled the formation of these films through the assistance of molecules with the amino group. Herein, we have chosen an electron-transport molecule with two amino groups, 4,4’-diaminodiphenyl sulfone (DDS), to control the crystallization process of perovskite films (Paper 1). The resulting perovskite films consists of in-situ formed high quality perovskite nanocrystals embedded in the electron-transport molecular matrix, resulting in improved PLQYs and structural stability. PeLEDs based on these perovskite films have exhibited both high efficiency and long operational stability.In addition, we have investigated the formation of mixed-dimensional perovskite films. Efficient PeLEDs based on mixed-dimensional perovskite films were fabricated with tin dioxide (SnO2) as an electron transport layer (Paper 3). We also note that the deposition methods have a significant impact on the morphology and optical properties of prepared mixed-dimensional perovskite films (Paper 4). In addition, we provide an effective method to extend the deposition of mixed-dimensional perovskite films, replacing organic ammonium halides with amines in the perovskite precursor solutions to form organic spacer cations through the in-situ protonation process of amines (Paper 2).In spite of these efforts, the performance of PeLEDs is still far from the commercialization standard, partially limited by ion migration. In Paper 5, we discuss impacts of mobile ions in the perovskite films on the performance of PeLEDs. We find that a dynamic redistribution of mobile ions can change current density of a device, leading to EQE/hysteresis during forward and reverse voltage scan and enhanced EQE under constant driving voltages. In addition, we have found that excess mobile ions in the perovskite layer can aggravate the hysteresis and shorten the operational stability of PeLEDs.In this thesis, we also discuss the remaining key challenges in the PeLED field, including the achievement of high-performance blue, white, and lead-free PeLEDs, as well as possible strategies to address these challenges. We hope that our research findings provide insights into the basic science behind the perovskite materials, and broadly benefit other optoelectronic communities, such as perovskite solar cells, flexible electronics, and so on.
|
|
| 13. |
- Wang, Lei, 1989-
(författare)
-
Protein Nanomaterials: : Functionalization, Self-assembly, and Applications
- 2020
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- As one of the major classes of materials that is relevant to biological function of our daily life, proteins are highly interesting in both biological and material science. Self-assembled protein amyloid nanostructures have been considered not only as aggregates in pathological tissue, but also as a kind of advanced one dimension materials in material science perspective due to their favorable characteristics including high aspect ratio, abundant surface charge groups, high stability, and tunable surface properties. The Protein nanofibrils (PNFs) can be self-assembly derived from a wide range of proteins, which isolated from natural and renewable sources, means it is relative cheap, environmentally friendly, and sustainable. The PNFs will contain additional functionalized properties for further applications by functionalizing with other materials such as fluorophores or conducting materials. An easy method is to utilize mechanochemistry, such as the use of a shaker mixer mill for grinding operation as well as hand grinding by mortar and pestle, helping mixing materials into fine powder thus helping the insoluble compounds and protein mixture to be water dispersible. Also, the liquid assisting ball milling exfoliation was achieved by high impact force to fracture the graphite and shear force to exfoliate the layered structure. In this thesis, interesting new properties of protein hybrids have been studied mainly focusing on two aspects: 1) by co-grinding hydrophobic dyes and proteins, a protein hydrophobic compound hybrid is obtained and following by inducing fibrils formation. The resulting functionalized PNFs thus have the fibril structure properties as well as the properties from incorporated compounds. By further self-assembly the functionalized PNFs to films, the materials transfer from micro to macrostructure. Besides, the protein act as surfactant for disperse hydrophobic probes for detection of Cu2+. 2) by milling the protein or protein nanofibrils dispersion with graphite, Graphene nanoplatelets (GNPs) is exfoliated and the GNPs ink functionalized by PNFs converted to devices and shows good properties for thermoelectrical voltage generation and water evaporation induced energy generation. Throughout the study of the thesis, we summarize how the protein hybrid materials was investigated. By demonstrating dyes functionalized PNFs and further PNFs films, as well as GNPs-PNFs hybrids acting as active materials on thermoelectrical and evaporation induced energy generating devices, we show the protein hybrid materials a promise new breakthrough in optical or energy generating aspects.
|
|
| 14. |
- Yu, Hongling, 1987-
(författare)
-
Color Tuning for Perovskite Light-Emitting Diodes
- 2020
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Metal halide perovskites (MHPs) are recognized as promising semiconductor materials for a variety of optical and electrical device applications due to their cost-effective and outstanding optoelectronic properties. As one of the most significant applications, perovskite light-emitting diodes (PeLEDs) hold promise for future lighting and display technologies, attributed to their high photoluminescence quantum yield (PLQY), high color purity, and tunable emission color. The emission colors of PeLEDs can be tuned by mixing the halide anions, adjusting the size of perovskite nanocrystals, or changing the dimensionality of perovskites. However, in practice, all these different approaches have their own advantages and challenges. This thesis centres around the color tunability of perovskites, aiming to develop PeLEDs with different colors using different approaches.We first demonstrate red and near-infrared PeLEDs using a straightforward approach – in situ solution-processed perovskite quantum dots (PQDs). PQDs prepared from colloidal approaches are widely reported and used in LEDs. In contrast, PQDs prepared from the in situ approaches are hardly reported, although they have advantages for device applications. By employing aromatic ammonium iodide (1-naphthylmethyl ammonium iodide, NMAI) as an agent into perovskite precursor solutions, together with annealing temperature modulation, we obtain in situ grown PQDs delivering high external quantum efficiencies (EQEs) of up to 11.0% with tunable electroluminescence (EL) spectra (667 - 790 nm). Our in situ generated PQDs based on pure-halogen perovskites can be easily obtained through a simple deposition process and free of phase segregation, making them a more promising approach for tuning the emission colors of perovskite LEDs.We then move to blue PeLEDs using cesium-based mixed-Br/Cl perovskites. Although mixed halides are a straightforward strategy to tune the emission color, PeLEDs based on this approach suffer from poor color stability, which is attributed to surface defects at grain boundaries. Under the condition of optical excitations, light density over a certain value (a threshold), oxygen, and surface defects at perovskite grain boundaries are found to be key factors inducing photoluminescence (PL) spectral instability of CsPb(Br1−xClx)3 perovskites. Upon electrical bias, defects at grain boundaries provide undesirable halide migration channels, responsible for EL spectral instability issues. Through effective defect passivation, the PL spectral resistance to oxygen is enhanced; moreover, high-performance and color-stable blue PeLEDs are achieved, delivering a maximum luminance of 5351 cd m–2 and a peak EQE of 4.55% with a peak emission wavelength at 489 nm. These findings provide new insights into the color instability issue of mixed halide blue perovskites, against which we also demonstrate an effective strategy.We finally realize single-emissive-layer (EML) white PeLEDs by employing a mixed halide perovskite film as the EML. In spite of high-performance monochromatic blue, green, and red colors, the development of white PeLEDs, especially for single-EML ones, remains a very big challenge. By effective modulation of the halide salt precursors, we achieve single-EML white PeLEDs with Commission Internationale de L’Eclairage (CIE) coordinates of (0.33, 0.33), close to those (0.3128, 0.3290) of the CIE standard illuminant D65. This work not only provides a successful demonstration of a single-EML white PeLED, but also provides useful guidelines for the future development of highperformance single-EML white PeLEDs.
|
|
| 15. |
- Yu, Jianwei, 1992-
(författare)
-
The Influence of Energy Levels on Voltage Losses and Charge Generation in Organic Solar Cells
- 2022
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Organic solar cells (OSCs) are a next-generation photovoltaic technology that convert solar energy to electrical energy. They have attracted great attention due to their advantages of low cost, ease of synthesis, light weight, mechanical flexibility, and roll-to-roll processability. In the past decades, owing to the development of the materials, device optimization and the understanding of the working mechanism, the power conversion efficiency (PCE) has been boosted to ~19%. However, the efficiency of the OSCs is still not comparable to the conventional inorganic solar cells and emerging perovskite solar cells due to the large open-circuit voltage loss (Vloss). In addition, it is also important to obtain efficient charge generation while reducing the Vloss. Thus, understanding the loss mechanisms in the OSCs is significant for achieving further improvement.In this thesis, a novel small-molecule donor named ZR1 was used to fabricate all-small-molecule OSCs (SM-OSCs), which shows efficient charge separation and transport with the optimized hierarchical morphologies, obtaining a breakthrough efficiency of 13.34% with a low Vloss (0.54 eV) in SM-OSCs. In this system, the energy offsets between the donor and acceptor (ΔHOMO or ΔLUMO) play an important role in the open-circuit voltage (VOC) of the OSCs. According to the optoelectronic reciprocity introduced in this thesis, the sub-gap absorption and emission by charge transfer (CT) states lead to large radiative and non-radiative recombination losses. The results show that the decreased HOMO offsets between donor and acceptor can effectively reduce both radiative and non-radiative recombination losses from the CT states, resulting in a suppressed Vloss.In addition to the SM-OSCs, we also study the Vloss and charge generation in the all-polymer OSCs (all- PSCs). A series of polymer acceptors were designed and applied in all-PSCs. In this work, all devices with negligible LUMO offsets show high VOCs of 1.02-1.15 V and good short-circuit currents (JSCs) of 8.87-15.16 mA cm−2 as well as small Vlosss. This study reveals that the small Vloss and the effective charge generation can also be realized simultaneously in all-PSCs with small energy offsets.Next, we found that introducing a third component can also reduce Vloss. In this work, we start with the fundamental photophysical processes which determine the VOCs of the devices and provide a universal approach framework well explaining the VOC of ternary OSCs (TOSCs) in different situations. By combining experimental investigations with theoretical simulations, we highlight the significant influence of the thermal population arising from the guest component-related CT states and local excited (LE)states on the non-radiative recombination losses in TOSCs. Firmly based on our new understanding, we provide design rules for enhancing the VOC in TOSCs: 1) high emission yield for the guest binary system; close charge-transfer energies between two binary systems; 2) high miscibility of the guest component with the low-optical-gap component in the host binary blends.In the all-PSCs work we did before, we find the small Vloss and the effective charge generation can be achieved simultaneously with small energy offsets, which can be also observed in other non-fullerene based OSCs. It was found that some of non-fullerene acceptors based OSCs can realize an efficient charge generation and a suppressed charge recombination process with small energy offsets (< 0.3 eV) between the donor and the acceptor, leading to a low Vloss, a high JSC, and a high fill factor (FF) simultaneously. Here, we investigate a series of OSCs blends with different HOMO offsets between donor and in a large range of ~ 0 to 0.50 eV. Along with decreasing HOMO offsets, the blends show reduced Vlosss. For the JSC and the FF, we observe a maximum value at an optimal energetic offset around 0.2-0.3 eV and the optimal energetic offset appears at different values for different non-fullerene acceptors. Through the analysis of the ultrafast transient absorption, we find inefficient charge generation when the HOMO offset is close to zero, which attributed to the back transfer of a hole from the donor to the acceptor. The affected charge generation at the small HOMO offsets is probably the main reason for the deceased JSC and FF. This study demonstrates the existence of optimal energy offsets for achieving high-performance OSCs.
|
|
| 16. |
- Yuan, Yusheng, 1992-
(författare)
-
Development of Functionalized Protein Materials
- 2022
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Many proteins are available as side-streams from food production, and in some cases even from industrial waste-streams. This means that proteins are available in large scale and at a relatively low price. As protein are highly complex molecules it is interesting to try to use protein as starting materials in for applications in materials science. Most proteins have the ability to self-assemble into nanofibrils. These fibrils have a regular repeating substructure that consists of β-strands running perpendicular to the fibril axis, resulting in cross-β sheets that run parallel along the fibril axis. The extended β-sheets structure results in the formation of hydrophobic grooves that can act as potential binding sites organic molecules. This means that the functionality of the material may be modified by addition of e.g. light emitting molecules or drug molecules. By such functionalization the protein material may accordingly be suitable for applications such as light-conversion materials (e.g. for use as coatings of light emitting diodes (LEDs)) or for drug-delivery. For such applications, the protein fibrils must be processes into macroscopic structures such as films or gels. Against this background, we employ the food proteins hen egg white lysozyme and β-lactoglobulin as model proteins for fibrillation and functionalization. Through a mechanochemical process the hydrophobic dyes can conveniently be combined with proteins, that can be converted into functionalized protein nanofibrils by liquid-phase self-assembly. By employing protein fibrils functionalized with three dyes, we have been able to form films that enables conversion of UV light to white light (and can thus be employed as a coating on UV-LEDs) with protein fibrils functionalized with multiple dyes. By mixing biodegradable polymers with functionalized protein fibrils, luminescent bioplastic films can be prepared that are processable when wet; a cut film will also self-heal if water is applied. We have also turned functionalized protein fibrils into gel states, including hydrogels or aerogels. In the case of protein fibrils functionalized with Hydantoins (a type of drug molecule) hydrogels were prepared, and the release of the drug was investigated. In addition, aerogels can be prepared from hydrogels by freeze drying, and in this manner lightweight functionalized aerogels are achieved. By functionalization with an electrically conductive polymer, an elastic conductive aerogel is formed that employed as a piezoelectric pressure sensor. In summary a wide range of materials have been prepared suitable for various applications demonstrating the flexibility of the developed functionalization methodology and that the structural richness of protein self-assembly can be employed to prepare a wide variety of types of materials of varying functionality.
|
|
| 17. |
- Zhang, Huotian
(författare)
-
Loss Mechanisms In Non-Fullerene Organic Solar Cells
- 2021
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Photovoltaics are one of the most important sustainable energy sources in the 21st century. Among photovoltaics, organic solar cells (OSCs) offer many advantages such as ease of processing, lightweight, the potential for flexibility, and tunable properties. Its peculiar nature and complexity present a fascinating charm, attracting many researchers. Thanks to researchers' efforts, the power conversion efficiency (PCE) of OSCs has been boosted from 1% to 19% during the last three decades. Despite the exciting PCE, some problems remain to be solved, for example, the large voltage loss and long-term stability. The aim of this thesis is to understand the fundamental physics of the state-of-the-art OSCs, especially the loss mechanism. Ultimately, properly understanding the mechanisms will sever as the basis of OSCs further improvements and commercialization. This work focuses on the loss mechanisms of OSCs, particularly the open-circuit voltage and the fill factor. The beginning of this thesis introduces basic concepts regarding semiconductors physics and donor-acceptor OSCs. This part explains how a photon is used to generate electricity and the fundamentals of organic electronics. Subsequently, the detailed balance in a solar cell is reviewed, which is the basis of voltage loss analysis. In this part, we see how the input, recombination, and output form a balance. Then, the way to determine the voltage loss is shown, and the latest understandings in reducing the loss are reviewed. The fill factor, as a measure of the quality of a solar cell, is a complex parameter, especially in OSCs.The latter part of this thesis starts from the photophysical processes in an OSC, and then relates intrinsic parameters to the fill factor. The figure of merits has been employed to express the fill factor analytically. In the end, experimental methods and basic principles for the previous analysis are introduced, including Fourier transform infrared spectroscopy, the external quantum efficiency of photovoltaics (EQEPV), spectrograph for electroluminescence or photoluminescence, transient absorption, and time-delayed collection field. Overall, the thesis combined thermal dynamics and charge dynamics to analyze voltage losses and fill factor losses. The author hopes this work can contribute to a better understanding of the loss mechanisms OSCs.
|
|
