| 1. |
- Ajjan, Fátima, 1986-, et al.
(author)
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Doped Conjugated Polymer Enclosing a Redox Polymer : Wiring Polyquinones with Poly(3,4‐Ethylenedioxythiophene)
- 2020
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In: Advanced Energy and Sustainability Research. - : John Wiley & Sons. - 2699-9412. ; 1:2
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Journal article (peer-reviewed)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.
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| 2. |
- Braun, Mats
(author)
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Postfunctionalism, Identity and the Visegrad Group
- 2020
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In: Journal of Common Market Studies. - : John Wiley & Sons. - 0021-9886 .- 1468-5965. ; 58:4, s. 925-940
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Journal article (peer-reviewed)abstract
- This article elaborates on the development of the Visegrad group (V4), consisting of the Czech Republic, Hungary, Poland and Slovakia, in relation to the European integration process in the aftermath of its many crises. The article suggests that the so-called migration crisis that started in 2015 for the V4 countries constitutes a situation that, in the existing literature, has been described as a postfunctionalist moment. However, in the V4 countries a postfunctionalist moment does not merely suggest reluctance to agree to further integration and in general a turn to EU criticism, but a strengthening of the four countries' shared V4 identity as well. To elaborate on the way that the V4's handling of the migration issue contributes to V4 identity-building, the article argues that the postfunctionalist literature needs to be supplemented by insights from social constructivism. The article utilises a narrative analysis to examine the way that a V4 identity is under construction.
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| 3. |
- Chen, Yongzhen, 1990-, et al.
(author)
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Experimental and Theoretical Investigation into the Polaron Structure of K-Doped Polyfluorene Films
- 2021
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In: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 125:1, s. 937-945
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Journal article (peer-reviewed)abstract
- The evolution of the electronic structure and optical transition upon n-doping of poly(9,9-dioctylfluorene) (PFO) films is elucidated with photoelectron spectroscopy, optical absorption, density functional theory (DFT), and time-dependent DFT (TD-DFT) calculations. Optical absorption measurements extending into near infrared show two low-energy absorption features at low doping ratios and an additional peak at a higher energy of similar to 2.2 eV that disappears with increasing doping ratios. A gap state (i.e., polaronic state) close to the Fermi level and a significantly destabilized highest valence band appear in the experimentally measured ultraviolet photoelectron spectra. These experimental results are interpreted by the TD-DFT calculations, which show that the lower energy peaks originate from the excitation from polaronic states to the conduction band, while the higher energy peak mainly originates from the destabilized valence band to conduction band transitions and only appears at low doping ratios (c(red) <= 50%, 0.5 potassium atom per fluorene monomer). The DFT calculations further indicate that polaron pairs rather than bipolarons are preferentially formed at high doping ratios. Comparing the results of doped glassy and beta-phase films, we find that the ordered segments in the beta-phase film disappear due to the dopant (potassium) insertion, resulting in a similar polaronic structure.
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| 4. |
- Chen, Yongzhen, 1990-, et al.
(author)
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Image-force effects on energy level alignment at electron transport material/cathode interfaces
- 2020
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In: Journal of Materials Chemistry C. - : ROYAL SOC CHEMISTRY. - 2050-7526 .- 2050-7534. ; 8:1, s. 173-179
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Journal article (peer-reviewed)abstract
- Electron transport materials (ETMs) are widely used as interlayers to lower the cathode electrode work function in organic solar cells and organic light-emitting diodes, for example. The usual interpretation for their operating principle is a chemical interaction between the ETM and the electrode, inducing partial or integer charge transfer or collectively an intrinsic dipole moment caused by preferential molecular orientation. Herein, we systematically explore the commonly used ETM bathophenanthroline (BPhen) deposited on a series of conducting substrates. The energetics at the BPhen interface follows the typical integer charge transfer (ICT) model with an extra displacement of the vacuum level by up to -1.4 eV. The extra displacement is ascribed to the "double dipole step" formed by the positive and negative charged species and their induced image charges when they are close to the surface of substrates. After n-type doping the displacement is further increased to -1.8 eV, yielding a larger work function modification than obtained using typical electrolytes and zwitterions as cathode interlayer.
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| 5. |
- Chen, Yongzhen, et al.
(author)
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In Situ Spectroscopic and Electrical Investigations of Ladder-type Conjugated Polymers Doped with Alkali Metals
- 2022
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In: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 55:16, s. 7294-7302
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Journal article (peer-reviewed)abstract
- Ladder-type conjugated polymers exhibit a remarkable performance in (opto)electronic devices. Their double-stranded planar structure promotes an extended pi-conjugation compared to inter-ring-twisted analogues, providing an excellent basis for exploring the effects of charge localization on polaron formation. Here, we investigated alkali-metal n -doping of the ladder-type conjugated polymer (polybenzimidazobenzophe-nanthroline) (BBL) through detailed in situ spectroscopic and electrical characterizations. Photoelectron spectroscopy and ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy indicate polaron formation upon potassium (K) doping, which agrees well with theoretical predictions. The semiladder BBB displays a similar evolution in the valence band with the appearance of two new features below the Fermi level upon K-doping. Compared to BBL, distinct differences appear in the UV-vis-NIR spectra due to more localized polaronic states in BBB. The high conductivity (2 S cm(-1)) and low activation energy (44 meV) measured for K-doped BBL suggest disorder-free polaron transport. An even higher conductivity (37 S cm(-1)) is obtained by changing the dopant from K to lithium (Li). We attribute the enhanced conductivity to a decreased perturbation of the polymer nanostructure induced by the smaller Li ions. These results highlight the importance of polymer chain planarity and dopant size for the polaronic state in conjugated polymers.
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| 6. |
- Chen, Yongzhen, 1990-, et al.
(author)
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Understanding Interface Dipoles at an Electron Transport Material/Electrode Modifier for Organic Electronics
- 2021
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In: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:39, s. 47218-47225
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Journal article (peer-reviewed)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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| 7. |
- Dahl, Martin, 1984-, et al.
(author)
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Impacts of land-use change and urban development on carbon sequestration in tropical seagrass meadow sediments
- 2022
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In: Marine Environmental Research. - : Elsevier BV. - 0141-1136 .- 1879-0291. ; 176
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Journal article (peer-reviewed)abstract
- Seagrass meadows store significant carbon stocks at a global scale, but land-use change and other anthropogenic activities can alter the natural process of organic carbon (Corg) accumulation. Here, we assessed the carbon accumulation history of two seagrass meadows in Zanzibar (Tanzania) that have experienced different degrees of disturbance. The meadow at Stone Town has been highly exposed to urban development during the 20th century, while the Mbweni meadow is located in an area with relatively low impacts but historical clearing of adjacent mangroves. The results showed that the two sites had similar sedimentary Corg accumulation rates (22–25 g m−2 yr−1) since the 1940s, while during the last two decades (∼1998 until 2018) they exhibited 24–30% higher accumulation of Corg, which was linked to shifts in Corg sources. The increase in the δ13C isotopic signature of sedimentary Corg (towards a higher seagrass contribution) at the Stone Town site since 1998 points to improved seagrass meadow conditions and Corg accumulation capacity of the meadow after the relocation of a major sewage outlet in the mid–1990s. In contrast, the decrease in the δ13C signatures of sedimentary Corg in the Mbweni meadow since the early 2010s was likely linked to increased Corg run-off of mangrove/terrestrial material following mangrove deforestation. This study exemplifies two different pathways by which land-based human activities can alter the carbon storage capacity of seagrass meadows (i.e. sewage waste management and mangrove deforestation) and showcases opportunities for management of vegetated coastal Corg sinks.
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| 8. |
- Hartley, Philippa, et al.
(author)
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SKA Science Data Challenge 2: analysis and results
- 2023
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In: Monthly Notices of the Royal Astronomical Society. - 0035-8711 .- 1365-2966. ; 523:2, s. 1967-1993
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Journal article (peer-reviewed)abstract
- The Square Kilometre Array Observatory (SKAO) will explore the radio sky to new depths in order to conduct transformational science. SKAO data products made available to astronomers will be correspondingly large and complex, requiring the application of advanced analysis techniques to extract key science findings. To this end, SKAO is conducting a series of Science Data Challenges, each designed to familiarize the scientific community with SKAO data and to drive the development of new analysis techniques. We present the results from Science Data Challenge 2 (SDC2), which invited participants to find and characterize 233 245 neutral hydrogen (H i) sources in a simulated data product representing a 2000 h SKA-Mid spectral line observation from redshifts 0.25-0.5. Through the generous support of eight international supercomputing facilities, participants were able to undertake the Challenge using dedicated computational resources. Alongside the main challenge, 'reproducibility awards' were made in recognition of those pipelines which demonstrated Open Science best practice. The Challenge saw over 100 participants develop a range of new and existing techniques, with results that highlight the strengths of multidisciplinary and collaborative effort. The winning strategy - which combined predictions from two independent machine learning techniques to yield a 20 per cent improvement in overall performance - underscores one of the main Challenge outcomes: that of method complementarity. It is likely that the combination of methods in a so-called ensemble approach will be key to exploiting very large astronomical data sets.
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| 9. |
- Li, Xiaofei, et al.
(author)
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Profiling spatiotemporal gene expression of the developing human spinal cord and implications for ependymoma origin
- 2023
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In: Nature Neuroscience. - : Springer Nature. - 1097-6256 .- 1546-1726. ; 26:5, s. 891-901
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Journal article (peer-reviewed)abstract
- The authors created a comprehensive developmental cell atlas for spatiotemporal gene expression of the human spinal cord, revealed species-specific regulation during development and used the atlas to infer novel markers for pediatric ependymomas. The spatiotemporal regulation of cell fate specification in the human developing spinal cord remains largely unknown. In this study, by performing integrated analysis of single-cell and spatial multi-omics data, we used 16 prenatal human samples to create a comprehensive developmental cell atlas of the spinal cord during post-conceptional weeks 5-12. This revealed how the cell fate commitment of neural progenitor cells and their spatial positioning are spatiotemporally regulated by specific gene sets. We identified unique events in human spinal cord development relative to rodents, including earlier quiescence of active neural stem cells, differential regulation of cell differentiation and distinct spatiotemporal genetic regulation of cell fate choices. In addition, by integrating our atlas with pediatric ependymomas data, we identified specific molecular signatures and lineage-specific genes of cancer stem cells during progression. Thus, we delineate spatiotemporal genetic regulation of human spinal cord development and leverage these data to gain disease insight.
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| 10. |
- Petsagkourakis, Ioannis, et al.
(author)
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Improved Performance of Organic Thermoelectric Generators Through Interfacial Energetics
- 2023
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In: Advanced Science. - : WILEY. - 2198-3844. ; 10:20
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Journal article (peer-reviewed)abstract
- The interfacial energetics are known to play a crucial role in organic diodes, transistors, and sensors. Designing the metal-organic interface has been a tool to optimize the performance of organic (opto)electronic devices, but this is not reported for organic thermoelectrics. In this work, it is demonstrated that the electrical power of organic thermoelectric generators (OTEGs) is also strongly dependent on the metal-organic interfacial energetics. Without changing the thermoelectric figure of merit (ZT) of polythiophene-based conducting polymers, the generated power of an OTEG can vary by three orders of magnitude simply by tuning the work function of the metal contact to reach above 1000 mu W cm(-2). The effective Seebeck coefficient (S-eff) of a metal/polymer/metal single leg OTEG includes an interfacial contribution (V-inter/Delta T) in addition to the intrinsic bulk Seebeck coefficient of the polythiophenes, such that S-eff = S + V-inter/Delta T varies from 22.7 mu V K-1 [9.4 mu V K-1] with Al to 50.5 mu V K-1 [26.3 mu V K-1] with Pt for poly(3,4-ethylenedioxythiophene):p-toluenesulfonate [poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate)]. Spectroscopic techniques are used to reveal a redox interfacial reaction affecting locally the doping level of the polymer at the vicinity of the metal-organic interface and conclude that the energetics at the metal-polymer interface provides a new strategy to enhance the performance of OTEGs.
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