Operando acoustic emission monitoring of degradation processes in lithium-ion batteries with a high-entropy oxide anode

In recent years, high-entropy oxides are receiving increasing attention for electrochemical energy-storage applications. Among them, the rocksalt (Co$_{0.2}$Cu$_{0.2}$Mg$_{0.2}$Ni$_{0.2}$Zn$_{0.2}$)O (HEO) has been shown to be a promising high-capacity anode material. Because high-entropy oxides constitute a new class of electrode materials, systematic understanding of their behavior during ion insertion and extraction is yet to be established. Here, we probe the conversion-type HEO material in lithium half-cells by acoustic emission (AE) monitoring. Especially the clustering of AE signals allows for correlations of acoustic events with various processes. The initial cycle was found to be the most acoustically active because of solid-electrolyte interphase formation and chemo-mechanical degradation. In the subsequent cycles, AE was mainly detected during delithiation, a finding we attribute to the progressive crack formation and propagation. Overall, the data confirm that the AE technology as a non-destructive operando technique holds promise for gaining insight into the degradation processes occurring in battery cells during cycling

The Sound of Batteries: An Operando Acoustic Emission Study of the LiNiO2_{2} Cathode in Li–Ion Cells

The development of advanced Li‐ion batteries relies on the implementation of high‐capacity Ni‐rich layered oxide cathode materials, such as NCM and NCA, among others. However, fast performance decay because of intrinsic chemical and structural instabilities hampers their practical application. Hence, thoroughly understanding degradation processes is crucial to overcome current limitations. To monitor instabilities of electrode materials under realistic operating conditions, the application of nondestructive operando techniques is required. While structural changes of crystalline phases can be studied by X‐ray diffraction, microstructural changes (e. g., particle fracture) cannot be easily accessed in situ and are therefore mostly investigated ex situ. Here, we use acoustic emission (AE) measurements to probe a potential next‐generation cathode material in real‐time. Specifically, we focus on LiNiO$_{2}$(LNO) and demonstrate that AE events in different frequency ranges can be correlated with the formation of the cathode solid‐electrolyte interphase and the mechanical degradation during electrochemical cycling

Design-of-experiments-guided optimization of slurry-cast cathodes for solid-state batteries

Laboratory research into bulk-type solid-state batteries (SSBs) has been focused predominantly on powder-based, pelletized cells and has been sufficient to evaluate fundamental limitations and tailor the constituents to some degree. However, to improve experimental reliability and for commercial implementation of this technology, competitive slurry-cast electrodes are required. Here, we report on the application of an approach guided by design of experiments (DoE) to evaluate the influence of the type/content of polymer binder and conductive carbon additive on the cyclability and processability of Li$_{1+x}$(Ni$_{0.6}$Co$_{0.2}$Mn$_{0.2}$)$_{1}$−xO$_{2}$ (NCM622) cathodes in SSB cells using lithium thiophosphate solid electrolytes. The predictions are verified by charge-discharge and impedance spectroscopy measurements. Furthermore, structural changes and gas evolution are monitored via X-ray diffraction and differential electrochemical mass spectrometry, respectively, in an attempt to rationalize and support the DoE results. In summary, the optimized combination of polymer binder and conductive carbon additive leads to high electrochemical performance and good processability

High-entropy energy materials: Challenges and new opportunities

The essential demand for functional materials enabling the realization of new energy technologies has triggered tremendous efforts in scientific and industrial research in recent years. Recently, high-entropy materials, with their unique structural characteristics, tailorable chemical composition and correspondingly tunable functional properties, have drawn increasing interest in the fields of environmental science and renewable energy technology. Herein, we provide a comprehensive review of this new class of materials in the energy field. We begin with discussions on the latest reports on the applications of high-entropy materials, including alloys, oxides and other entropy-stabilized compounds and composites, in various energy storage and conversion systems. In addition, we describe effective strategies for rationally designing high-entropy materials from computational techniques and experimental aspects. Based on this overview, we subsequently present the fundamental insights and give a summary of their potential advantages and remaining challenges, which will ideally provide researchers with some general guides and principles for the investigation and development of advanced high-entropy materials