During the past decades, Li-ion batteries have been one of the most important energy storage devices. Large-scale energy storage requires Li-ion batteries which possess high energy density, low cost, and high safety. Other than advanced battery materials, in-depth understanding of the intrinsic mechanism correlated with cell reaction is also essential for the development of high-performance Li-ion battery. Advanced characterization techniques, especially neutron-based techniques, have greatly promoted Li-ion battery researches. In this review, the characteristics or capabilities of various neutron-based characterization techniques, including elastic neutron scattering, quasi-elastic neutron scattering, neutron imaging, and inelastic neutron scattering, for the related Li-ion-battery researches are summarized. The design of in-situ/operando environment is also discussed. The comprehensive survey on neutron-based characterizations for mechanism understanding will provide guidance for the further study of high-performance Li-ion batteries.

Fracture occurred in electrodes of the lithium-ion battery compromises the integrity of the electrode structure and would exert bad influence on the cell performance and cell safety. Mechanisms of the electrode-level fracture and how this fracture would affect the electrochemical performance of the battery are of great importance for comprehending and preventing its occurrence. Fracture occurring at the electrode level is complex, since it may involve fractures in or between different components of the electrode. In this review, three typical types of electrode-level fractures are discussed: the fracture of the active layer, the interfacial delamination, and the fracture of metallic foils (including the current collector and the lithium metal electrode). The crack in the active layer can serve as an effective indicator of degradation of the electrochemical performance. Interfacial delamination usually follows the fracture of the active layer and is detrimental to the cell capacity. Fracture of the current collector impacts cell safety directly. Experimental methods and modeling results of these three types of fractures are concluded. Reasonable explanations on how these electrode-level fractures affect the electrochemical performance are sorted out. Challenges and unsettled issues of investigating these fracture problems are brought up. It is noted that the state-of-the-art studies included in this review mainly focus on experimental observations and theoretical modeling of the typical mechanical damages. However, quantitative investigations on the relationship between the electrochemical performance and the electrode-level fracture are insufficient. To further understand fractures in a multi-scale and multi-physical way, advancing development of the cross discipline between mechanics and electrochemistry is badly needed.

The structure-activity relationship of functional materials is an everlasting and desirable research question for material science researchers, where characterization and calculation tools are the keys to deciphering this intricate relationship. Here, we choose rechargeable battery materials as an example and introduce the most representative advanced characterization and calculation methods in four different scales: real space, energy, momentum space, and time. Current research methods to study battery material structure, energy level transition, dispersion relations of phonons and electrons, and time-resolved evolution are reviewed. From different views, various expression forms of structure and electronic structure are presented to understand the reaction processes and electrochemical mechanisms comprehensively in battery systems. According to the summary of the present battery research, the challenges and perspectives of advanced characterization and calculation techniques for the field of rechargeable batteries are further discussed.

Battery materials are of vital importance in powering a clean and sustainable society. Improving their performance relies on a clear and fundamental understanding of their properties, in particular, structural properties. Pair distribution function (PDF) analysis, which takes into account both Bragg scattering and diffuse scattering, can probe structures of both crystalline and amorphous phases in battery materials. This review first introduces the principle of PDF, followed by its application in battery materials. It shows that PDF is an effective tool in studying a series of key scientific topics in battery materials. They range from local ordering, nano-phase quantification, anion redox reaction, to lithium storage mechanism, and so on.

Safety requirements stimulate Na-based batteries to evolve from high-temperature Na-S batteries to room-temperature Na-ion batteries (NIBs). Even so, NIBs may still cause thermal runaway due to the external unexpected accidents and internal high activity of electrodes or electrolytes, which has not been comprehensively summarized yet. In this review, we summarize the significant advances about the failure mechanisms and related strategies to build safer NIBs from the selection of electrodes, electrolytes and the construction of electrode/electrolyte interfaces. Considering the safety risk, the thermal behaviors are emphasized which will deepen the understanding of thermal stability of different NIBs and accelerate the exploitation of safe NIBs.

Although the lithium-ion batteries (LIBs) have been increasingly applied in consumer electronics, electric vehicles, and smart grid, they still face great challenges from the continuously improving requirements of energy density, power density, service life, and safety. To solve these issues, various studies have been conducted surrounding the battery design and management methods in recent decades. In the hope of providing some inspirations to the research in this field, the state of the art of design and management methods for LIBs are reviewed here from the perspective of process systems engineering. First, different types of battery models are summarized extensively, including electrical model and multi-physics coupled model, and the parameter identification methods are introduced correspondingly. Next, the model based battery design methods are reviewed briefly on three different scales, namely, electrode scale, cell scale, and pack scale. Then, the battery model based battery management methods, especially the state estimation methods with different model types are thoroughly compared. The key science and technology challenges for the development of battery systems engineering are clarified finally.