Li‐rich layered oxide cathodes with conventional transition metal cation and unique oxygen anion redox reactions deliver high capacities in Li‐ion batteries. However, the oxygen redox process causes ...the oxygen release, voltage fading/hysteresis, and sluggish electrochemical kinetics, which undermine the performance of these materials. By combining operando quick‐scanning X‐ray absorption spectroscopy with online gas chromatography, the effect of the local electronic structure is elucidated on the reaction mechanism and electrochemical kinetics of Li‐rich cathodes. The local electronic structure of Li‐rich cathodes varies with the excess Li (i.e., Li2MnO3 phase) and Ni contents. Compared to the Li‐rich cathodes with higher amounts of Li2MnO3 phase (high excess lithium content (HLC) cathode), those with lower Li2MnO3 contents (low excess lithium content (LLC) cathode) exhibit reversible anion redox reactions and suppressed voltage hysteresis. The cation oxidation process of LLC cathode is kinetically slower than that of HLC cathode and the cation oxidation potential is shifted, likely due to the local coordination associated with different Li/O ratios. The obtained insights into the effect of local electronic structure on the reaction mechanism and kinetics provide a better understanding and control of Li‐rich cathodes.
This research reveals the reaction mechanism and electrochemical kinetics of Li‐rich cathodes using in operando quick‐scanning X‐ray absorption spectroscopy. With the control of Li2MnO3 domain, cation migration and voltage decay were suppressed. The electrochemical stability and kinetics of tradition metal (TM) redox can be tuned by modifying the local coordination structure of Li‐rich cathode.
MoO3/V2O5 hybrid nanobilayers are successfully prepared by the sol–gel method with a spin- coating technique followed by heat -treatment at 350 °C in order to achieve a good crystallinity. The ...composition, morphology, and microstructure of the nanobilayers are characterized by a scanning electron microscope (SEM) and X-ray diffractometer (XRD) that revealed the a grain size of around 20–30 nm, and belonging to the monoclinic phase. The samples show good reversibility in the cyclic voltammetry studies and exhibit an excellent response to the visible transmittance. The electrochromic (EC) window displayed an optical transmittance changes (ΔT) of 22.65% and 31.4% at 550 and 700 nm, respectively, with the rapid response time of about 8.2 s for coloration and 6.3 s for bleaching. The advantages, such as large optical transmittance changes, rapid electrochromism control speed, and excellent cycle durability, demonstrated in the electrochromic cell proves the potential application of MoO3/V2O5 hybrid nanobilayers in electrochromic devices.
Stress variation induced bandgap tuning and surface wettability switching of spinel nickel ferrite (NiFe2O4, NFO) films were demonstrated and directly driven by phase transition via a post-annealing ...process. Firstly, the as-deposited NFO films showed hydrophilic surface with water contact angle (CA) value of 80 ± 1°. After post-annealing with designed temperatures ranged from 400 to 700 °C in air ambience for 1 hour, we observed that the crystal structure was clearly improved from amorphous-like/ nanocrystalline to polycrystalline with increasing post-annealing temperature and this phenomenon is attributed to the improved crystallinity combined with relaxation of internal stress. Moreover, super-hydrophilic surface (CA = 14 ± 1°) was occurred due to the remarkable grain structure transition. The surface wettability could be adjusted from hydrophilicity to super-hydrophilicity by controlling grain morphology of NFO films. Simultaneously, the saturation magnetization (Ms) values of NFO films at room temperature increased up to 273 emu/cm3 accompanied with transitions of the phase and grain structure. We also observed an exceptionally tunable bandgap of NFO in the range between 1.78 and 2.72 eV under phase transition driving. Meanwhile, our work demonstrates that direct grain morphology combined with the stress tuning can strongly modulate the optical, surface and magnetic characteristics in multifunctional NFO films.
Abstract
Among many transition-metal oxides, Fe
3
O
4
anode based lithium ion batteries (LIBs) have been well-investigated because of their high energy and high capacity. Iron is known for elemental ...abundance and is relatively environmentally friendly as well contains with low toxicity. However, LIBs based on Fe
3
O
4
suffer from particle aggregation during charge–discharge processes that affects the cycling performance. This study conjectures that iron agglomeration and material performance could be affected by dopant choice, and improvements are sought with Fe
3
O
4
nanoparticles doped with 0.2% Ti. The electrochemical measurements show a stable specific capacity of 450 mAh g
−1
at 0.1 C rate for at least 100 cycles in Ti doped Fe
3
O
4
. The stability in discharge capacity for Ti doped Fe
3
O
4
is achieved, arising from good electronic conductivity and stability in microstructure and crystal structure, which has been further confirmed by density functional theory (DFT) calculation. Detailed distribution function of relaxation times (DFRTs) analyses based on the impedance spectra reveal two different types of Li ion transport phenomena, which are closely related with the electron density difference near the two Fe-sites. Detailed analyses on EIS measurements using DFRTs for Ti doped Fe
3
O
4
indicate that improvement in interfacial charge transfer processes between electrode and Li metal along with an intermediate lithiated phase helps to enhance the electrochemical performance.
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•Glancing angle deposition method is firstly used for preparing naturally hydrophobic ZnO films.•Ultra-flat ZnO textured films exhibited good crystallinity and excellent visible ...transparency (higher than 80%).•FTIR/ATR investigations confirmed the interfacial water molecules near the surface of ultra-flat ZnO films.•The natural hydrophobicity and wetting state can be attributed to the surface grain morphology and surface absorption of hydrocarbon.
Ultra-flat Zinc oxide (ZnO) films with natural hydrophobicity were sputtered onto glass substrates by glancing angle deposition (GLAD) method without addition of active oxygen at room temperature under different glancing angles relating to the sample holder. The sample holder was positioned at glancing angles of 0° and 30°, and the sputtering power was fixed at 75W with low argon (Ar) pressure of 1×10−2Torr during deposition process. According to analysis of surface composition and structure, the naturally hydrophobic wetting state can be attributed to the different grain structure and hydrocarbon adsorbates on the top of the film surface. On the other hand, the interfacial water molecules near the surface of ultra-flat ZnO films are confirmed belong to the hydrophobic hydrogen structure by Fourier transform infrared/attenuated total reflection. In addition, the water contact angle was significantly improved by a simple factor of glancing angle. The water contact angle value of ultra-flat ZnO films increased from 90° to 98° while the sample holder is with glancing angle of 30°. Moreover, our present ultra-flat ZnO films also exhibited excellent transparency over 80%, and the surface wetting switched from hydrophobic to hydrophilic states after exposing in ultraviolet (UV) surroundings. Then, the ZnO films could be freely and stably reversed back to hydrophobicity after stored in dark surroundings. This present study not only demonstrates that the natural wettability of ultra-flat ZnO films is strongly associated with surface composition and structure, but also provides an easy way to modulate and improve the surface wettability. This also extends the potential applications of ultra-flat ZnO thin films and aids a profound understanding for device design and material development.
Cobalt Iron Yttrium (CoFeY) magnetic film was made using the sputtering technique in order to investigate the connection between the thickness and annealing procedures. The sample was amorphous as a ...result of an insufficient thermal driving force according to X-ray diffraction (XRD) examination. The maximum low-frequency alternate-current magnetic susceptibility (χac) values were raised in correlation with the increased thickness and annealing temperatures because the thickness effect and Y addition improved the spin exchange coupling. The best value for a 50 nm film at annealing 300 °C for χac was 0.20. Because electron carriers are less constrained in their conduction at thick film thickness and higher annealing temperatures, the electric resistivity and sheet resistance are lower. At a thickness of 40 nm, the film’s maximum surface energy during annealing at 300 °C was 28.7 mJ/mm2. This study demonstrated the passage of photon signals through the film due to the thickness effect, which reduced transmittance. The best condition was found to be 50 nm with annealing at 300 °C in this investigation due to high χac, strong adhesion, and low resistivity, which can be used in magnetic fields.
The energetic particles bombardment can produce large internal stress in the zinc oxide (ZnO) thin film, and it can be used to intentionally modify the surface characteristics of ZnO films. In this ...article, we observed that the internal stress increased from -1.62 GPa to -0.33 GPa, and the naturally wettability of the textured ZnO nanostructured films changed from hydrophobicity to hydrophilicity. According to analysis of surface chemical states, the naturally controllable wetting behavior can be attributed to hydrocarbon adsorbates on the nanostructured film surface, which is caused by tunable internal stress. On the other hand, the interfacial water molecules near the surface of ZnO nanostructured films have been identified as hydrophobic hydrogen structure by Fourier transform infrared/attenuated total reflection. Moreover, a remarkable near-band-edge emission peak shifting also can be observed in PL spectra due to the transition of internal stress state. Furthermore, our present ZnO nanostructured films also exhibited excellent transparency over 80% with a wise surface wetting switched from hydrophobic to hydrophilic states after exposing in ultraviolet (UV) surroundings. Our work demonstrated that the internal stress of the thin film not only induced natural wettability transition of ZnO nanostructured films, but also in turn affected the surface properties such as surface chemisorption.
Rainfall measurement is subjected to various uncertainties due to the complexity of measurement techniques and atmosphere characteristics associated with weather type. Thus, this article presents a ...video-based disdrometer to analyze raindrop images by introducing artificial intelligence technology for the rainfall rate. First, a high-speed CMOS camera is integrated into a planar LED as a backlight source for appropriately acquiring falling raindrops in different positions. The falling raindrops can be illuminated and used for further image analysis. Algorithms developed for raindrop detection and trajectory identification are employed. In a field test, a rainfall event of 42 continuous hours has been measured by the proposed disdrometer that is validated against a commercial PARSIVEL 2 disdrometer and a tipping bucket rain gauge at the same area. In the evaluation for 5-min rainfall images, the results of the trajectory identification are within the precision of 87.8%, recall of 98.4%, and F1 score of 92.8%, respectively. Furthermore, the performance exhibits that the rainfall rate and raindrop size distribution (RSD) obtained by the proposed disdrometer are remarkably consistent with those of PARSIVEL 2 disdrometer. The results suggest that the proposed disdrometer based on the continuous movements of the falling raindrops can achieve accurate measurements and eliminate the potential errors effectively in the real-time monitoring of rainfall.
A facile solution process was employed to prepare CsPbI3 as an anode material for Li-ion batteries. Rietveld refinement of the X-ray data confirms the orthorhombic phase of CsPbI3 at room ...temperature. As obtained from bond valence calculations, strained bonds between Pb and I are identified within PbI6 octahedral units. Morphological study shows that the as-prepared δ-CsPbI3 forms a nanorod-like structure. The XPS analysis confirm the presence of Cs (3d, 4d), Pb (4d, 4f, 5d) and I (3p, 3d, 4d). The lithiation process involves both intercalation and conversion reactions, as confirmed by cyclic voltammetry (CV) and first-principles calculations. Impedance spectroscopy coupled with the distribution function of relaxation times identifies charge transfer processes due to Li metal foil and anode/electrolyte interfaces. An initial discharge capacity of 151 mAhg−1 is found to continuously increase to reach a maximum of ~275 mAhg−1 at 65 cycles, while it drops to ~240 mAhg−1 at 75 cycles and then slowly decreases to 235 mAhg−1 at 100 cycles. Considering the performance and structural integrity during electrochemical performance, δ-CsPbI3 is a promising material for future Li-ion battery (LIB) application.
X-ray diffraction (XRD) analysis showed that metal oxide peaks appear at 2θ = 47.7°, 54.5°, and 56.3°, corresponding to Yb2O3 (440), Co2O3 (422), and Co2O3 (511). It was found that oxide formation ...plays an important role in magnetic, electrical, and surface energy. For magnetic and electrical measurements, the highest alternating current magnetic susceptibility (χac) and the lowest resistivity (×10−2 Ω·cm) were 0.213 and 0.42, respectively, and at 50 nm, it annealed at 300 °C due to weak oxide formation. For mechanical measurement, the highest value of hardness was 15.93 GPa at 200 °C in a 50 nm thick film. When the thickness increased from 10 to 50 nm, the hardness and Young’s modulus of the Co60Fe20Yb20 film also showed a saturation trend. After annealing at 300 °C, Co60Fe20Yb20 films of 40 nm thickness showed the highest surface energy. Higher surface energy indicated stronger adhesion, allowing for the formation of multilayer thin films. The optimal condition was found to be 50 nm with annealing at 300 °C due to high χac, strong adhesion, high nano-mechanical properties, and low resistivity.