TU/e), the Netherlands. Currently, he is conducting his research at Forschungszentrum Jülich (Germany). His research interests focus on the design and development of effective strategies for high-performance Li-S batteries. Dmitri L. Danilov, Ph.D., has a background in physics and mathematics and obtained his M.Sc. at the Saint-Petersburg University in 1993. In 2003, he got Ph.D. degree from the University of Tilburg.In 2002, he joined Eurandom institute in Eindhoven University of Technology, being involved in various national and international research projects. His current research interests include mathematical modeling of complex electrochemical systems, including Li-ion and NiMH batteries, ageing and degradation processes, thin-film batteries, and advanced characterization methods. Starting 2017, he joined IEK-9 in the Forschungszentrum Jülich.

The growing demand for sustainable energy storage devices requires rechargeable lithium‐ion batteries (LIBs) with higher specific capacity and stricter safety standards. Ni‐rich layered transition metal oxides outperform other cathode materials and have attracted much attention in both academia and industry. Lithium‐ion batteries composed of Ni‐rich layered cathodes and graphite anodes (or Li‐metal anodes) are suitable to meet the energy requirements of the next generation of rechargeable batteries. However, the instability of Ni‐rich cathodes poses serious challenges to large‐scale commercialization. This paper reviews various degradation processes occurring at the cathode, anode, and electrolyte in Ni‐rich cathode‐based LIBs. It highlights the recent achievements in developing new stabilization strategies for the various battery components in future Ni‐rich cathode‐based LIBs.

Extensive efforts have been made to improve the Li‐ionic conductivity of solid electrolytes (SE) for developing promising all‐solid‐state Li‐based batteries (ASSB). Recent studies suggest that minimizing the existing interface problems is even more important than maximizing the conductivity of SE. Interfaces are essential in ASSB, and their properties significantly influence the battery performance. Interface problems, arising from both physical and (electro)chemical material properties, can significantly inhibit the transport of electrons and Li‐ions in ASSB. Consequently, interface problems may result in interlayer formation, high impedances, immobilization of moveable Li‐ions, loss of active host sites available to accommodate Li‐ions, and Li‐dendrite formation, all causing significant storage capacity losses and ultimately battery failures. The characteristic differences of interfaces between liquid‐ and solid‐type Li‐based batteries are presented here. Interface types, interlayer origin, physical and chemical structures, properties, time evolution, complex interrelations between various factors, and promising interfacial tailoring approaches are reviewed. Furthermore, recent advances in the interface‐sensitive or depth‐resolved analytical tools that can provide mechanistic insights into the interlayer formation and strategies to tailor the interlayer formation, composition, and properties are discussed.

Ni-rich LiNi0.6Co0.2Mn0.2O2 nanomaterials with a high percentage of exposed {010} facets have been prepared by surfactant-assisted hydrothermal synthesis followed by solid-state reaction. Characterization by X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) confirmed that the particles have enhanced the growth of nanocrystal planes in favor of Li-ion diffusion. Electrochemical tests show these cathode materials endow a large Li-ion diffusion coefficient, which leads to a superior rate capability and cyclability, suggesting these cathode materials are highly beneficial for practical application in Li-ion batteries.

Rechargeable lithium–sulfur (Li–S) batteries, which originate from the merits of extraordinary theoretical specific energy density, abundant resources, and eco-friendly character, have received ever-growing attention. However, their practical applications are seriously hampered because of the poor conductive property of the sulfur and the discharging products, severe dissolution and migration of lithium polysulfide intermediates, and huge volumetric variation of sulfur particles upon cycling. Here, double-shelled Co3O4 and carbon (Co3O4/C) hollow nanocages as sulfur host materials are reported. The double-shelled structures can significantly boost the adsorption of soluble polysulfides and the electrical conductivity of sulfur cathodes. Consequently, the prepared S@Co3O4/C cathodes achieve considerable capacity enhancement and excellent rate capability, combining the durable cycling life at 1 C for 500 cycles, in which the overall capacity fading remains as low as 0.083% per cycle. Upper-plateau (Q H) and lower-plateau (Q L) capacities, static adsorption of polysulfides, and X-ray photoelectron spectroscopy (XPS) analyses unveil the underlying nature of the chemical interactions between polysulfide species and the sulfur host. The present results will favor the design and screening of prospective host materials to boost future Li–S batteries.

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LiGePS (LGPS) is the fastest known Li-ion conductor to date due to the formation of one-dimensional channels with a very high Li mobility. A knowledge-based optimization of such materials for use, for example, as solid electrolyte in all-solid-state batteries requires, however, a more comprehensive understanding of Li ion conduction that considers mobility in all three dimensions, mobility between crystallites and different phases, as well as their distributions within the material. The spin alignment echo (SAE) nuclear magnetic resonance (NMR) technique is suitable to directly probe slow Li ion hops with correlation times down to about 10 s, but distinction between hopping time constants and relaxation processes may be ambiguous. This contribution presents the correlation of the Li spin lattice relaxation (SLR) time constants (T) with the SAE decay time constant τ to distinguish between hopping time constants and signal decay limited by relaxation in the τ distribution. A pulse sequence was employed with two independently varied mixing times. The obtained multidimensional time domain data was processed with an algorithm for discrete Laplace inversion that does not use a non-negativity constraint to deliver 2D SLR-SAE correlation maps. Using the full echo transient, it was also possible to estimate the NMR spectrum of the Li ions responsible for each point in the correlation map. The signal components were assigned to different environments in the LGPS structure.

High rate capability and long-term cycling spindle-like LiTi 2 (PO 4 ) 3 /C anode and needle-like Li 3 V 2 (PO 4 ) 3 cathode have been evaluated in half-cell, and combined to fabricate an advanced fast cyclable all phosphate lithium-ion battery. The electrode materials with well-defined morphology were prepared by a solvothermal reaction followed by annealing, delivering capacities of 115.0 and 118.1 mAh · g −1 at 25 • C over 200 cycles at 0.5 C, respectively. For the full cell assembly, no prelithiation process is needed for the selected electrode pair due to their mutually matched capacity and stoichiometric amount of lithium-ions. The fabricated full cell, with an output voltage of more than 1.5 V, inherits a superior rate capability and cycling performance of its electrodes. A discharge capacity of 36 mAh · g −1 at 30 C (about 30% of the initial discharge capacity at 0.1 C) and a capacity retention of ∼35% at 5 C over 1000 cycles has been achieved. Furthermore, one of the most important reasons for the capacity fading in the full cell during long-term cycling is found to be a decomposition and structural degradation of Lithium-ion batteries are widely used in portable electronics and are a promising energy storage system for electric vehicles because of their high energy density and long cycle life.1,2 However, current lithium-ion battery technologies are still far from satisfaction to meet the increasingly diverse range of applications. For instance, the use of lithium-ion cells in large scale applications, such as electric vehicles, demands high charge/discharge cycling performance and an inherent high thermal stability.3,4 Micro-lithium-ion batteries which can be applied to human body require in first instance the considerations of safety issue and cycling performance. 5,6 For the development of a novel type of lithium-ion battery like all-solid-state lithium-ion battery, one of the urgent needs to be addressed is to improve the ionic and electronic conductivity among the whole battery system. 7,8 Additionally, high rate performance and long cycle life are required for lithium-ion battery as stationary application for power management. To advance the battery technologies according the desired applications, it is important to explore the cathode and anode materials, and match them reasonably and to investigate their electrochemical performances. [10][11][12] have attracted much attention because more than two formula units of Li-ions can possibly intercalate/deintercalate into/from their host crystal structure during discharge/charge at a moderate working potential. On the basis of the crystal structure in these cathode materials, the use of phosphate polyanions (PO 4 ) 3− is considered as a potential alternative to oxide-based cathodes. The strong P−O bonds and the framework of (PO 4 ) 3− anions can guarantee both the dynamic and thermal stabilities required to fulfill the safety requisites in high-power applications.18 More than that, phosphate materials are also believed to be superior candidates of an...