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Mijalkov, Mite; Gerboles, Blanca Zufiria; Vereb, Daniel; Lüdge, Kathy; Brunner, Daniel; Volpe, Giovanni; Pereira, Joana B.
Uncovering vulnerable connections in the aging brain using reservoir computing. - In: Emerging Topics in Artificial Intelligence (ETAI) 2023, (2023), PC1265508

We used reservoir computing to explore the changes in the connectivity patterns of whole-brain anatomical networks derived by diffusion-weighted imaging, and their impact on cognition during aging. The networks showed optimal performance at small densities. This performance decreased with increasing density, with the rate of decrease being strongly associated with age and performance on behavioural tasks measuring cognitive function. This suggests that a network core of anatomical hubs is crucial for optimal functioning, while weaker connections are more susceptible to aging effects. This study highlights the potential utility of reservoir computing in understanding age-related changes in cognitive function.



https://doi.org/10.1117/12.2677364
Xu, Changfan; Qiu, Jiajia; Dong, Yulian; Li, Yueliang; Shen, Yonglong; Zhao, Huaping; Kaiser, Ute; Shao, Guosheng; Lei, Yong
Dual-functional electrode promoting dendrite-free and CO2 utilization enabled high-reversible symmetric Na-CO2 batteries. - In: Energy & Environmental Materials, ISSN 2575-0356, Bd. n/a (2023), n/a, e12626, S. 1-10

Sodium-carbon dioxide (Na-CO2) batteries are regarded as promising energy storage technologies because of their impressive theoretical energy density and CO2 reutilization, but their practical applications are restricted by uncontrollable sodium dendrite growth and poor electrochemical kinetics of CO2 cathode. Constructing suitable multifunctional electrodes for dendrite-free anodes and kinetics-enhanced CO2 cathodes is considered one of the most important ways to advance the practical application of Na-CO2 batteries. Herein, RuO2 nanoparticles encapsulated in carbon paper (RuCP) are rationally designed and employed as both Na anode host and CO2 cathode in Na-CO2 batteries. The outstanding sodiophilicity and high catalytic activity of RuCP electrodes can simultaneously contribute to homogenous Na+ distribution and dendrite-free sodium structure at the anode, as well as strengthen discharge and charge kinetics at the cathode. The morphological evolution confirmed the uniform deposition of Na on RuCP anode with dense and flat interfaces, delivering enhanced Coulombic efficiency of 99.5% and cycling stability near 1500 cycles. Meanwhile, Na-CO2 batteries with RuCP cathode demonstrated excellent cycling stability (>350 cycles). Significantly, implementation of a dendrite-free RuCPNa anode and catalytic-site-rich RuCP cathode allowed for the construction of a symmetric Na-CO2 battery with long-duration cyclability, offering inspiration for extensive practical uses of Na-CO2 batteries.



https://doi.org/10.1002/eem2.12626
Tang, Xinyue; Lv, Xincha; Lou, Jiayi; Fan, Tieyan; Chen, Heng; Wang, Wenxin; Zhang, Shangcong; Zhao, Huaping; Zhang, Qingcheng; Wang, Shun; Lei, Yong
Rational design of a hierarchical candied-haws-like NiCo2O4Ni,Co-(HCO3)2 heterostructure for the electrochemical performance enhancement of supercapacitors. - In: ACS applied energy materials, ISSN 2574-0962, Bd. 6 (2023), 19, S. 9905-9914

Designing core-shell heterostructures with multicomponents, more electroactive sites, hierarchical structures, and stable geometrical configurations is an effective approach to enhance the electrochemical properties of supercapacitors. Herein, we report the fabrication of a hierarchical candied-haws-like NiCo2O4NiCo-hydrocarbonate heterostructure on Ni foam (NiCo2O4@NiCo-HCs), which consists of NiCo2O4 nanowires acting as “rebars” that are tightly strung with NiCo-HC nanoparticles. The strong interfacial reaction between the NiCo2O4 “core” and the NiCo-HC “shell” accelerates the charge transfer within the heterostructure, while the hierarchical structure containing quantities of paths and pores provides fast ion diffusion throughout the whole electrode, hence remarkably boosting the electrochemical performance of a NiCo2O4@NiCo-HC electrode. As expected, the NiCo2O4@NiCo-HC electrode shows a high specific capacitance of 3216.4 F g-1 at a current density of 1 A g-1 and 2259.9 F g-1 even at 20 A g-1 (1.6-fold that of the NiCo2O4 electrode and 5.5-fold that of NiCo-HCs). In addition, an assembled asymmetric supercapacitor NiCo2O4@NiCo-HCs//AC delivers a high energy density of 47.46 Wh kg-1 at a power density of 708.94 W kg-1, together with 96.2% capacitance retention after 6000 cycles, surpassing most of the reported analogues. These results suggest that our hierarchical candied-haws-like heterostructure design is potential for the performance enhancement of supercapacitors.



https://doi.org/10.1021/acsaem.3c01421
Shen, Fengxia; Shi, Xinbo; Shi, Jin
Novel bipolar membrane electrolyzer for CO2 reduction to CO in organic electrolyte with Cl2 and NaOH produced as byproducts. - In: Journal of CO2 utilization, ISSN 2212-9839, Bd. 77 (2023), 102595, S. 1-10

Electrochemical reduction of CO2 to valuable products, powered by renewable energy, provides a promising strategy for reducing our dependence on fossil fuels. But up to now, no technology has been implemented for large-scale industrial applications. Without massive utilization of CO2, many vital practical problems, such as reducing CO2 emissions, storing renewable energy, and alleviating environmental pollution, cannot be resolved through this route. Herein, we propose a novel electrolyzer for CO2 electro-reduction, which is separated into three chambers by a bipolar membrane and a cation exchange membrane. In the cathodic chamber, CO2 is reduced to CO in organic electrolytes. In the anodic chamber, Cl- is oxidized to Cl2 in NaCl aqueous solution. In the central chamber, NaOH is obtained. The generated CO and Cl2 can be used as feedstock to produce phosgene (CO+Cl2 =COCl2). Through this route, phosgene can be produced from CO2 and NaCl, with NaOH generated as a byproduct. By substantially increasing the product value, we can promote CO2 electro-reduction technology to industrial applications.



https://doi.org/10.1016/j.jcou.2023.102595
Wieboldt, Rieke; Lindt, Kevin; Pohlmeier, Andreas; Mattea, Carlos; Stapf, Siegfried; Haber-Pohlmeier, Sabina
Effects of salt precipitation in the topmost soil layer investigated by NMR. - In: Applied magnetic resonance, ISSN 1613-7507, Bd. 54 (2023), 11/12, S. 1607-1631

The drying of highly concentrated aqueous salt solutions in sand and soil has been investigated by one-dimensional spatially resolved low-field relaxation measurements of 1H nuclei in water as well as high-field MRI of 1H and 23Na nuclei of water and sodium ions. Water evaporates until the solutions in the solid matrix reach saturation conditions, when salt begins to crystallize. Depending on salt type and conditions, such as actual soil water content and air humidity, this crystallization can occur above (efflorescent) or below (subflorescent) the soil surface. Both effects occur in nature and affect the evaporation behavior of water. The formation of salt precipitate domains is demonstrated by MRI, where the precipitate domains remain penetrable to water. Complete drying is achieved in the top 2 mm of soil with the exception of strongly hygroscopic perchlorates which maintain a constant amount of liquid water under ambient laboratory conditions and dry air. This situation is considered similar to the co-existence of perchlorates and water in strongly eutectic mixtures on Mars.



https://doi.org/10.1007/s00723-023-01568-1
Wang, Zhongwu; Ma, Yining; Guo, Shujing; Yuan, Liqian; Hu, Yongxu; Huang, Yinan; Chen, Xiaosong; Ji, Deyang; Bi, Jinshun; Lei, Yong; Han, Cheng; Li, Liqiang; Hu, Wenping
Suppressing the intrinsic photoelectric response of organic semiconductors for highly-photostable organic transistors. - In: Small, ISSN 1613-6829, Bd. 19 (2023), 50, 2304634, S. 1-8

Suppressing the photoelectric response of organic semiconductors (OSs) is of great significance for improving the operational stability of organic field-effect transistors (OFETs) in light environments, but it is quite challenging because of the great difficulty in precisely modulating exciton dynamics. In this work, photostable OFETs are demonstrated by designing the micro-structure of OSs and introducing an electrical double layer at the OS/polyelectrolyte dielectric interface, in which multiple exciton dynamic processes can be modulated. The generation and dissociation of excitons are depressed due to the small light-absorption area of the microstripe structure and the excellent crystallinity of OSs. At the same time, a highly efficient exciton quenching process is activated by the electrical double layer at the OS/polyelectrolyte dielectric interface. As a result, the OFETs show outstanding tolerance to the light irradiation of up to 306 mW&hahog;cm−2, which far surpasses the solar irradiance value in the atmosphere (≈138 mW&hahog;cm−2) and achieves the highest photostability ever reported in the literature. The findings promise a general and practicable strategy for the realization of photostable OFETs and organic circuits.



https://doi.org/10.1002/smll.202304634
Hu, Ping; Dong, Yulian; Wu, Zhijun; Fu, Qun; Zhao, Huaping; Lei, Yong
Bimetallic-based composites for potassium-ion storage: challenges and perspectives. - In: Inorganic chemistry frontiers, ISSN 2052-1553, Bd. 10 (2023), 16, S. 4668-4694

Potassium ion batteries (PIBs) are important for the development of energy storage systems as an effective complement to lithium ion batteries (LIBs) owing to the abundance of potassium resources in the earth's crust to meet the needs of large-scale energy storage systems. To this end, numerous studies have focused on anode materials, which can provide high capacity for PIBs. Bimetallic-based compounds (ABXs) achieve higher capacity and structural diversity due to their different chemical compositions and rich spatial structures. Moreover, the synergistic effect of the two metals makes the structure of ABXs more stable. Hence, ABXs are one of the most promising anode materials. This review focuses on performance optimization strategies (such as metal base selection, structural design, voltage regulation, and electrolyte optimization) and the electrochemical properties of ABXs. Finally, the current challenges and research prospectives of ABXs are presented. This review is expected to provide new perspectives and deeper insights into the study of ABXs as anode materials for PIBs and large-scale energy storage devices.



https://doi.org/10.1039/D3QI00585B
Xu, Dongbo; Zhang, Song; Yu, Yangfei; Zhang, Shu; Ding, Qijia; Lei, Yong; Shi, Weidong
Ultrathin metal Ni layer on ZnO/TiO2 photoelectrodes with excellent photoeletrochemical performance in multiple electrolyte solutions. - In: Fuel, ISSN 1873-7153, Bd. 351 (2023), 128774

It is well known that the oxygen vacancy (Ovac) as the electron-donor dopant in semiconductor can increase the electron-holes separation in photoeletrochemical (PEC) water splitting. Furthermore, the metal Ni can promote the hydrogen evolution reaction (HER) on the surface of semiconductor. In this paper, the ZnO/TiO2 photoelectrodes with rich Ovac was synthesized by electrostatic adsorption through using ZIF-8 as the precursor. Then the ultrathin Ni layer with about 7 nm was deposited on the surface of ZnO/TiO2 (Ni/ZnO/TiO2) by vacuum thermal evaporation method. The Ni/ZnO/TiO2 photoelectrodes showed the highest photocurrent than ZnO/TiO2, Ni/ TiO2 and pure TiO2 photoelectrodes. The durability of Ni/ZnO/TiO2 photoelectrodes was keeping for 10 h in multiple electrolyte solutions under AM 1.5 G illumination and the photocurrent decline can be ignored. The UV-vis absorption spectra demonstrated that the ultrathin Ni layer showed plasma with ZnO/TiO2 for enhancing the water splitting performance. Furthermore, the ultrathin Ni layer enhanced the photogenerated charges transfer for improving the PEC performance. This work provides a new method for ultrathin metal Ni layer with Ovac semiconductor photoelectrode to improve the PEC performance in multiple electrolyte solutions.



https://doi.org/10.1016/j.fuel.2023.128774
Zeußel, Lisa; Schober, Andreas; Ullmann, Fabian; Krischok, Stefan; Heinrich, Doris; Singh, Sukhdeep
Visible-light-assisted donor-acceptor-Stenhouse-adduct-based reversible photoswitching on a laser-structurable OrmoComp substrate. - In: ACS applied polymer materials, ISSN 2637-6105, Bd. 5 (2023), 10, S. 8631-8640

Laser-assisted nanolithography of commercially available photoresists is offering a limitless designing opportunity in the micro- and nanostructuring of 3D organotypic cell culture scaffolds. Among them, chemically functionalized OrmoComp has shown promising improvement in cell adhesion that paves the way to assemble cellular entities on a desirable geometry. Establishing a photoswitchable chemistry on the OrmoComp surface may offer an additional degree of freedom to manipulate the surface chemistry locally and selectively. We have established the methods for functionalization of the photopolymerized OrmoComp surface with visible-light-switchable donor-acceptor Stenhouse adducts. Unlike other polymers, a photopolymerized OrmoComp surface appears to be optimal for reversible photothermal switching, offering the possibility to influence surface properties like absorption and hydrophilicity tremendously. Light-assisted chemical modulation between colored triene-2-ol and colorless cyclopentenone can be achieved to a size region as narrow as 20 μm. Thermal reversion to the original triene-2-ol state can be analyzed spectroscopically and observed with the naked eye.



https://doi.org/10.1021/acsapm.3c01766
Mathew, Sobin; Reiprich, Johannes; Narasimha, Shilpashree; Abedin, Saadman; Kurtash, Vladislav; Thiele, Sebastian; Scheler, Theresa; Hähnlein, Bernd; Schaaf, Peter; Jacobs, Heiko O.; Pezoldt, Jörg
Gate-tunable hysteresis response of field effect transistor based on sulfurized Mo. - In: AIP Advances, ISSN 2158-3226, Bd. 13 (2023), 9, 095224, S. 095224-1-095224-7

Hysteresis effects and their tuning with electric fields and light were studied in thin film molybdenum disulfide transistors fabricated from sulfurized molybdenum films. The influence of the back-gate voltage bias, voltage sweep range, illumination, and AlOx encapsulation on the hysteresis effect of the back-gated field effect transistors was studied and quantified. This study revealed the distinctive contribution of MoS2 surface, MoS2/SiO2 interface defects and their associated traps as primary sources of of hysteresis.



https://doi.org/10.1063/5.0165868