Facile solid-state synthesis of a layered Co-free, Ni-rich cathode material for all-solid-state batteries

Layered Ni-rich oxides are attractive cathode active materials for secondary battery applications. Combining them with inorganic superionic conductors and high-capacity anodes can significantly increase energy density. Herein we successfully synthesized spherical secondary particles of a Mn-substituted LiNiO$_2$, LiNi$_{0.95}$Mn$_{0.05}$O$_2$ (a Co-free NMX material), for use in bulk-type lithium-thiophosphate-based all-solid-state batteries

The effect of configurational entropy on acoustic emission of P2-type layered oxide cathodes for sodium-ion batteries

Sodium-ion batteries (SIBs) see intensive research and commercialization efforts, aiming to establish them as an alternative to lithium-ion batteries. Among the reported cathode material families for SIBs, Na-deficient P2-type layered oxides are promising candidates, benefiting from fast sodium diffusion and therefore high charge/discharge rates. However, upon sodium extraction at high potentials, a transition from the P2 to O2 phase occurs, with the corresponding change in cell volume resulting in particle fracture and capacity degradation. A possible solution to this is to increase configurational entropy by introducing more elements into the transition-metal layer (so-called high-entropy concept), leading to some kind of structural stabilization. In this work, the acoustic emission (AE) of a series of P2-type layered oxide cathodes with increasing configurational entropy [Na0.67(Mn0.55Ni0.21Co0.24)O2, Na0.67(Mn0.45Ni0.18Co0.24Ti0.1Mg0.03)O2 and Na0.67(Mn0.45Ni0.18Co0.18Ti0.1Mg0.03Al0.04Fe0.02)O2] is recorded during SIB operation and correlated to the materials properties, namely change in c lattice parameter and cracking behavior. A structure-property relationship between entropy, manifested in the extent of phase transition, and detected AE is derived, supported by the classification of signals by peak frequency. This classification in combination with microscopy imaging allows to distinguish between inter- and intragranular fracture. Relatively more intergranular and less intragranular crack formation is observed with increasing configurational entropy

Transition-metal interdiffusion and solid electrolyte poisoning in all-solid-state batteries revealed by cryo-TEM

Using scanning transmission electron microscopy, along with electron energy loss spectroscopy, under cryogenic conditions, we demonstrate transition-metal dissolution from a layered Ni-rich oxide cathode material and subsequent diffusion into the bulk of a lithium thiophosphate solid electrolyte during electrochemical cycling. This problem has previously only been considered for liquid-electrolyte-based batteries

The Effect of Single versus Polycrystalline Cathode Particles on All‐Solid‐State Battery Performance

Lithium-thiophosphate-based all-solid-state batteries (ASSBs) are increasingly attracting attention for high-density electrochemical energy storage. In this work, the cycling performance of single and polycrystalline forms of LiNi$_{x}$Co$_{y}$Mn$_{z}$O$_{2}$ (NCM, with ≥83% Ni content) cathode active materials in ASSB cells with an Li$_{4}$Ti$_{5}$O$_{12}$ composite anode is explored, and the advantages and disadvantages of both morphologies are discussed. The virtual lack of grain boundaries in the quasi-single-crystalline material is found to contribute to improved stability by eliminating the tendency of Ni-rich NCM particles to crack during cycling, due to volume differences between the lithiated and delithiated phases. Although the higher crack resistance mitigates effects of chemical oxidation of the lithium thiophosphate solid electrolyte, the cells suffer from electrochemical side reactions occurring at the cathode interfaces. However, coating the single-crystal particles with a protective LiNbO$_{3}$ overlayer helps to stabilize the interface between cathode active material and solid electrolyte, leading to a capacity retention of 93% after 200 cycles (with q$_{dis}$ ≈ 160 mAh g$_{NCM}$$^{-1}$ or 1.7 mAh cm$^{-2}$ at C/5 rate and 45 °C). Overall, this work highlights the importance of addressing electro-chemo-mechanical phenomena in ASSB electrodes

Advanced Nanoparticle Coatings for Stabilizing Layered Ni‐Rich Oxide Cathodes in Solid‐State Batteries

Improving the interfacial stability between cathode active material (CAM) and solid electrolyte (SE) is a vital step toward the development of high-performance solid-state batteries (SSBs). One of the challenges plaguing this field is an economical and scalable approach to fabricate high-quality protective coatings on the CAM particles. A new wet-coating strategy based on preformed nanoparticles is presented herein. Nonagglomerated nanoparticles of the coating material (≤5 nm, exemplified for ZrO$_{2}$) are prepared by solvothermal synthesis, and after surface functionalization, applied to a layered Ni-rich oxide CAM, LiNi$_{0.85}$Co$_{0.10}$Mn$_{0.05}$O$_{2}$ (NCM85), producing a uniform surface layer with a unique structure. Remarkably, when used in pelletized SSBs with argyrodite Li$_{6}$PS$_{5}$Cl as SE, the coated NCM85 is found to exhibit superior lithium-storage properties (q$_{dis}$ ≈ 204 mAh g$_{NCM85}$$^{-1}$ at 0.1 C rate and 45 °C) and good rate capability. The key to the observed improvement lies in the homogeneity of coating, suppressing interfacial side reactions while simultaneously limiting gas evolution during operation. Moreover, this strategy is proven to have a similar effect in liquid electrolyte-based Li-ion batteries and can potentially be used for the application of other, even more favorable, nanoparticle coatings

The Boundary Proportion Differential Control Method of Micro-Deformable Manipulator with Compensator Based on Partial Differential Equation Dynamic Model

It is challenging to accurately judge the actual end position of the manipulator—regarded as a rigid body—due to the influence of micro-deformation. Its precise and efficient control is a crucial problem. To solve the problem, the Hamilton principle was used to establish the partial differential equation (PDE) dynamic model of the manipulator system based on the infinite dimension of the working environment interference and the manipulator space. Hence, it resolves the common overflow instability problem in the micro-deformable manipulator system modeling. Furthermore, an infinite-dimensional radial basis function neural network compensator suitable for the dynamic model was proposed to compensate for boundary and uncertain external interference. Based on this compensation method, a distributed boundary proportional differential control method was designed to improve control accuracy and speed. The effectiveness of the proposed model and method was verified by theoretical analysis, numerical simulation, and experimental verification. The results show that the proposed method can effectively improve the response speed while ensuring accuracy

Automatic Registration for Panoramic Images and Mobile LiDAR Data Based on Phase Hybrid Geometry Index Features

The registration of panoramic images and mobile light detection and ranging (LiDAR) data is quite challenging because different imaging mechanisms and viewing angle differences generate significant geometric and radiation distortions between the two multimodal data sources. To address this problem, we propose a registration method for panoramic images and mobile LiDAR data based on the hybrid geometric structure index feature of phase. We use the initial GPS/IMU to transform the mobile LiDAR data into an intensity map and align the two images to complete registration. Firstly, a novel feature descriptor called a hybrid geometric structure index of phase (HGIFP) is built to capture the structural information of the images. Then, a set of corresponding feature points is obtained from the two images using the constructed feature descriptor combined with a robust false-match elimination algorithm. The average pixel distance of the corresponding feature points is used as the error function. Finally, in order to complete the accurate registration of the mobile LiDAR data and panoramic images and improve computational efficiency, we propose the assumption of local motion invariance of 3D–2D corresponding feature points and minimize the error function through multiple reprojections to achieve the best registration parameters. The experimental results show that the method in this paper can complete the registration of panoramic images and the mobile LiDAR data under a rotation error within 12° and a translation error within 2 m. After registration, the average error of rotation is about 0.15°, and the average error of translation is about 1.27 cm. Moreover, it achieves a registration accuracy of less than 3 pixels in all cases, which outperforms the current five state-of-the-art methods, demonstrating its superior registration performance

Automatic Registration for Panoramic Images and Mobile LiDAR Data Based on Phase Hybrid Geometry Index Features

The registration of panoramic images and mobile light detection and ranging (LiDAR) data is quite challenging because different imaging mechanisms and viewing angle differences generate significant geometric and radiation distortions between the two multimodal data sources. To address this problem, we propose a registration method for panoramic images and mobile LiDAR data based on the hybrid geometric structure index feature of phase. We use the initial GPS/IMU to transform the mobile LiDAR data into an intensity map and align the two images to complete registration. Firstly, a novel feature descriptor called a hybrid geometric structure index of phase (HGIFP) is built to capture the structural information of the images. Then, a set of corresponding feature points is obtained from the two images using the constructed feature descriptor combined with a robust false-match elimination algorithm. The average pixel distance of the corresponding feature points is used as the error function. Finally, in order to complete the accurate registration of the mobile LiDAR data and panoramic images and improve computational efficiency, we propose the assumption of local motion invariance of 3D–2D corresponding feature points and minimize the error function through multiple reprojections to achieve the best registration parameters. The experimental results show that the method in this paper can complete the registration of panoramic images and the mobile LiDAR data under a rotation error within 12° and a translation error within 2 m. After registration, the average error of rotation is about 0.15°, and the average error of translation is about 1.27 cm. Moreover, it achieves a registration accuracy of less than 3 pixels in all cases, which outperforms the current five state-of-the-art methods, demonstrating its superior registration performance