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- ItemTime‐Dependent Cation Selectivity of Titanium Carbide MXene in Aqueous Solution(Weinheim : Wiley-VCH, 2022) Wang, Lei; Torkamanzadeh, Mohammad; Majed, Ahmad; Zhang, Yuan; Wang, Qingsong; Breitung, Ben; Feng, Guang; Naguib, Michael; Presser, VolkerElectrochemical ion separation is a promising technology to recover valuable ionic species from water. Pseudocapacitive materials, especially 2D materials, are up-and-coming electrodes for electrochemical ion separation. For implementation, it is essential to understand the interplay of the intrinsic preference of a specific ion (by charge/size), kinetic ion preference (by mobility), and crystal structure changes. Ti3C2Tz MXene is chosen here to investigate its selective behavior toward alkali and alkaline earth cations. Utilizing an online inductively coupled plasma system, it is found that Ti3C2Tz shows a time-dependent selectivity feature. In the early stage of charging (up to about 50 min), K+ is preferred, while ultimately Ca2+ and Mg2+ uptake dominate; this unique phenomenon is related to dehydration energy barriers and the ion exchange effect between divalent and monovalent cations. Given the wide variety of MXenes, this work opens the door to a new avenue where selective ion-separation with MXene can be further engineered and optimized.
- ItemHigh-Quality Graphene Using Boudouard Reaction(Weinheim : Wiley-VCH, 2022) Grebenko, Artem K.; Krasnikov, Dmitry V.; Bubis, Anton V.; Stolyarov, Vasily S.; Vyalikh, Denis V.; Makarova, Anna A.; Fedorov, Alexander; Aitkulova, Aisuluu; Alekseeva, Alena A.; Gilshtein, Evgeniia; Bedran, Zakhar; Shmakov, Alexander N.; Alyabyeva, Liudmila; Mozhchil, Rais N.; Ionov, Andrey M.; Gorshunov, Boris P.; Laasonen, Kari; Podzorov, Vitaly; Nasibulin, Albert G.Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in general opens avenues for breakthrough graphene-catalyst composite production.
- ItemTailoring Intermolecular Interactions Towards High‐Performance Thermoelectric Ionogels at Low Humidity(Weinheim : Wiley-VCH, 2022) Zhao, Wei; Sun, Tingting; Zheng, Yiwei; Zhang, Qihao; Huang, Aibin; Wang, Lianjun; Jiang, WanDevelopment of ionic thermoelectric (iTE) materials is of immense interest for efficient heat-to-electricity conversion due to their giant ionic Seebeck coefficient (Si), but challenges remain in terms of relatively small Si at low humidity, poor stretchability, and ambiguous interaction mechanism in ionogels. Herein, a novel ionogel is reported consisting of polyethylene oxide (PEO), polyethylene oxide-polypropylene oxide-polyethylene oxide (P123), and 1-ethyl-3-methylimidazolium acetate (Emim:OAC). By delicately designing the interactions between ions and polymers, the migration of anions is restricted due to their strong binding with the hydroxyl groups of polymers, while the transport of cations is facilitated through segmental motions due to the increased amorphous regions, thereby leading to enlarged diffusion difference between the cations and anions. Moreover, the plasticizing effect of P123 and Emim:OAC can increase the elongation at break. As a consequence, the ionogel exhibits excellent properties including high Si (18 mV K−1 at relative humidity of 60%), good ionic conductivity (1.1 mS cm−1), superior stretchability (787%), and high stability (over 80% retention after 600 h). These findings show a promising strategy to obtain multifunctional iTE materials by engineering the intermolecular interactions and demonstrate the great potential of ionogels for harvesting low-grade heat in human-comfortable humidity environments.
- ItemAuger- and X-ray Photoelectron Spectroscopy at Metallic Li Material: Chemical Shifts Related to Sample Preparation, Gas Atmosphere, and Ion and Electron Beam Effects(Basel : MDPI, 2022) Oswald, SteffenLi-based batteries are a key element in reaching a sustainable energy economy in the near future. The understanding of the very complex electrochemical processes is necessary for the optimization of their performance. X-ray photoelectron spectroscopy (XPS) is an accepted method used to improve understanding around the chemical processes at the electrode surfaces. Nevertheless, its application is limited because the surfaces under investigation are mostly rough and inhomogeneous. Local elemental analysis, such as Auger electron spectroscopy (AES), could assist XPS to gain more insight into the chemical processes at the surfaces. In this paper, some challenges in using electron spectroscopy are discussed, such as binding energy (BE) referencing for the quantitative study of chemical shifts, gas atmospheric influences, or beam damage (including both AE and XP spectroscopy). Carefully prepared and surface-modified metallic lithium material is used as model surface, considering that Li is the key element for most battery applications.
- ItemActive Matrix Flexible Sensory Systems: Materials, Design, Fabrication, and Integration(Weinheim : Wiley-VCH Verlag GmbH & Co. KGaA, 2022) Bao, Bin; Karnaushenko, Dmitriy D.; Schmidt, Oliver G.; Song, Yanlin; Karnaushenko, DaniilA variety of modern applications including soft robotics, prosthetics, and health monitoring devices that cover electronic skins (e-skins), wearables as well as implants have been developed within the last two decades to bridge the gap between artificial and biological systems. During this development, high-density integration of various sensing modalities into flexible electronic devices becomes vitally important to improve the perception and interaction of the human bodies and robotic appliances with external environment. As a key component in flexible electronics, the flexible thin-film transistors (TFTs) have seen significant advances, allowing for building flexible active matrices. The flexible active matrices have been integrated with distributed arrays of sensing elements, enabling the detection of signals over a large area. The integration of sensors within pixels of flexible active matrices has brought the application scenarios to a higher level of sophistication with many advanced functionalities. Herein, recent progress in the active matrix flexible sensory systems is reviewed. The materials used to construct the semiconductor channels, the dielectric layers, and the flexible substrates for the active matrices are summarized. The pixel designs and fabrication strategies for the active matrix flexible sensory systems are briefly discussed. The applications of the flexible sensory systems are exemplified by reviewing pressure sensors, temperature sensors, photodetectors, magnetic sensors, and biosignal sensors. At the end, the recent development is summarized and the vision on the further advances of flexible active matrix sensory systems is provided.
- ItemHigh‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries(Weinheim : Wiley-VCH, 2022) Lin, Ling; Wang, Kai; Sarkar, Abhishek; Njel, Christian; Karkera, Guruprakash; Wang, Qingsong; Azmi, Raheleh; Fichtner, Maximilian; Hahn, Horst; Schweidler, Simon; Breitung, BenHigh-entropy sulfides (HESs) containing 5 equiatomic transition metals (M), with different M:S ratios, are prepared by a facile one-step mechanochemical approach. Two new types of single-phase HESs with pyrite (Pa-3) and orthorhombic (Pnma) structures are obtained and demonstrate a homogeneously mixed solid solution. The straightforward synthesis method can easily tune the desired metal to sulfur ratio for HESs with different stoichiometries, by utilizing the respective metal sulfides, even pure metals, and sulfur as precursor chemicals. The structural details and solid solution nature of HESs are studied by X-ray diffraction, transmission electron microscopy, energy-dispersive X-ray spectroscopy, electron energy loss spectroscopy, X-ray photoelectron spectroscopy, inductively coupled plasma optical emission spectroscopy, and Mössbauer spectroscopy. Since transition metal sulfides are a very versatile material class, here the application of HESs is presented as electrode materials for reversible electrochemical energy storage, in which the HESs show high specific capacities and excellent rate capabilities in secondary Li-ion batteries.
- ItemIn situ detection of cracks during laser powder bed fusion using acoustic emission monitoring(Amsterdam : Elsevier, 2022) Seleznev, Mikhail; Gustmann, Tobias; Friebel, Judith Miriam; Peuker, Urs Alexander; Kühn, Uta; Hufenbach, Julia Kristin; Biermann, Horst; Weidner, AnjaDespite rapid development of laser powder bed fusion (L-PBF) and its monitoring techniques, there is still a lack of in situ crack detection methods, among which acoustic emission (AE) is one of the most sensitive. To elaborate on this topic, in situ AE monitoring was applied to L-PBF manufacturing of a high-strength Al92Mn6Ce2 (at. %) alloy and combined with subsequent X-ray computed tomography. By using a structure borne high-frequency sensor, even a simple threshold-based monitoring was able to detect AE activity associated with cracking, which occurred not only during L-PBF itself, but also after the build job was completed, i.e. in the cooling phase. AE data analysis revealed that crack-related signals can easily be separated from the background noise (e.g. inert gas circulation pump) through their specific shape of a waveform, as well as their energy, skewness and kurtosis. Thus, AE was verified to be a promising method for L-PBF monitoring, enabling to detect formation of cracks regardless of their spatial and temporal occurrence.
- ItemAn AI-based open recommender system for personalized labor market driven education(Amsterdam [u.a.] : Elsevier Science, 2022) Tavakoli, Mohammadreza; Faraji, Abdolali; Vrolijk, Jarno; Molavi, Mohammadreza; Mol, Stefan T.; Kismihók, GáborAttaining those skills that match labor market demand is getting increasingly complicated, not in the last place in engineering education, as prerequisite knowledge, skills, and abilities are evolving dynamically through an uncontrollable and seemingly unpredictable process. Anticipating and addressing such dynamism is a fundamental challenge to twenty-first century education. The burgeoning availability of data, not only on the demand side but also on the supply side (in the form of open educational resources) coupled with smart technologies, may provide a fertile ground for addressing this challenge. In this paper, we propose a novel, Artificial Intelligence (AI) driven approach to the development of an open, personalized, and labor market oriented learning recommender system, called eDoer. We discuss the complete system development cycle starting with a systematic user requirements gathering, and followed by system design, implementation, and validation. Our recommender prototype (1) derives the skill requirements for particular occupations through an analysis of online job vacancy announcements
- ItemEffect of Fans’ Placement on the Indoor Thermal Environment of Typical Tunnel-Ventilated Multi-Floor Pig Buildings Using Numerical Simulation(Basel : MDPI AG, 2022) Wang, Xiaoshuai; Cao, Mengbing; Hu, Feiyue; Yi, Qianying; Amon, Thomas; Janke, David; Xie, Tian; Zhang, Guoqiang; Wang, KaiyingAn increasing number of large pig farms are being built in multi-floor pig buildings (MFPBs) in China. Currently, the ventilation system of MFPB varies greatly and lacks common standards. This work aims to compare the ventilation performance of three popular MFPB types with different placement of fans using the Computational Fluid Dynamics (CFD) technique. After being validated with field-measured data, the CFD models were extended to simulate the air velocity, air temperature, humidity, and effective temperature of the three MFPBs. The simulation results showed that the ventilation rate of the building with outflowing openings in the endwall and fans installed on the top of the shaft was approximately 25% less than the two buildings with fans installed on each floor. The ventilation rate of each floor increased from the first to the top floor for both buildings with a shaft, while no significant difference was observed in the building without a shaft. Increasing the shaft’s width could mitigate the variation in the ventilation rate of each floor. The effective temperature distribution at the animal level was consistent with the air velocity distribution. Therefore, in terms of the indoor environmental condition, the fans were recommended to be installed separately on each floor.
- ItemOptical Anisotropy and Momentum-Dependent Excitons in Dibenzopentacene Single Crystals(Washington, DC : ACS Publications, 2022) Graf, Lukas; Liu, Fupin; Naumann, Marco; Roth, Friedrich; Debnath, Bipasha; Büchner, Bernd; Krupskaya, Yulia; Popov, Alexey A.; Knupfer, MartinHigh-quality single crystals of the organic semiconductor (1,2;8,9)-dibenzopentacene were grown via physical vapor transport. The crystal structure─unknown before─was determined by single-crystal X-ray diffraction; polarization-dependent optical absorption measurements display a large anisotropy in the ac plane of the crystals. The overall Davydov splitting is ∼110 meV, which is slightly lower than that in the close relative pentacene (120 meV). Momentum-dependent electron energy-loss spectroscopy measurements show a clear exciton dispersion of the Davydov components. An analysis of the dispersion using a simple 1D model indicates smaller electron- and hole-transfer integrals in dibenzopentacene as compared to pentacene. The spectral weight distribution of the excitation spectra is strongly momentum-dependent and demonstrates a strong momentum-dependent admixture of Frenkel excitons, charge-transfer excitons, and vibrational modes.