Layered double hydroxides (LDH) have been extensively investigated for charge storage, however, their development is hampered by the sluggish reaction dynamics. Herein, triggered by mismatching integration of Mn sites, we configured wrinkled Mn/NiCo-LDH with strains and defects, where promoted mass & charge transport behaviors were realized. The well-tailored Mn/NiCo-LDH displays a capacity up to 518 C g⁻¹ (1 A g⁻¹), a remarkable rate performance (78%@100 A g⁻¹) and a long cycle life (without capacity decay after 10,000 cycles). We clarified that the moderate electron transfer between the released Mn species and Co²⁺ serves as the pre-step, while the compressive strain induces structural deformation with promoted reaction dynamics. Theoretical and operando investigations further demonstrate that the Mn sites boost ion adsorption/transport and electron transfer, and the Mn-induced effect remains active after multiple charge/discharge processes. This contribution provides some insights for controllable structure design and modulation toward high-efficient energy storage.

The sodium (Na) superionic conductor is a key component that could revolutionize the energy density and safety of conventional Na-ion batteries. However, existing Na superionic conductors are primarily based on a single-anion framework, each presenting inherent advantages and disadvantages. Here we introduce a family of amorphous Na-ion conductors (Na₂O₂–MCl_y, M = Hf, Zr and Ta) based on the dual-anion framework of oxychloride. Benefiting from a dual-anion chemistry and with the resulting distinctive structures, Na₂O₂–MCl_y electrolytes exhibit room-temperature ionic conductivities up to 2.0 mS cm⁻¹, wide electrochemical stability windows and desirable mechanical properties. All-solid-state Na-ion batteries incorporating amorphous Na₂O₂–HfCl₄ electrolyte and a Na_0.85Mn_0.5Ni_0.4Fe_0.1O₂ cathode exhibit a superior rate capability and long-term cycle stability, with 78% capacity retention after 700 cycles under 0.2 C (1C = 120 mA g⁻¹) at room temperature. The discoveries in this work could trigger a new wave of enthusiasm for exploring new superionic conductors beyond those based on a single-anion framework.

Solid-state batteries are attractive energy storage systems as a result of their inherent safety, but their development hinges on advanced solid-state electrolytes (SSEs). Most SSEs remain largely confined to single-anion systems (e.g., sulfides, oxides, halides, and polymers). Through mixed-anion design strategy, we develop crystalline Li ₃ Ta ₃ O ₄ Cl ₁₀ (LTOC) and its derivatives with excellent ionic conductivities (up to 13.7 millisiemens per centimeter at 25°C) and electrochemical stability. The LTOC structure features mixed-anion spiral chains, consisting of corner-shared oxygen and terminal chlorine atoms, which induces continuous “tetrahedron-tetrahedron” Li-ion migration pathways with low energy barriers. Additionally, LTOC demonstrates holistic cathode compatibility, enabling solid-state batteries operation at 4.9 volts versus Li/Li ⁺ and low temperature, down to −50°C. These findings describe a promising class of superionic conductors for high-performance solid-state batteries.

Two‐dimensional (2D) layered transition metal carbides/nitrides, called MXenes, are attractive alternative electrode materials for electrochemical energy storage. Owing to their metallic electrical conductivity and low ion diffusion barrier, MXenes are promising anode materials for sodium‐ion batteries (SIBs). Herein, we report on a new 2D carbonitride MXene, viz., Ti₂C_0.5N_0.5T_x (T_x stands for surface terminations), and the only second carbonitride after Ti₃CNT_x so far. A new type of in situ HF (HCl/KF) etching condition was employed to synthesize multilayer Ti₂C_0.5N_0.5T_x powders from Ti₂AlC_0.5N_0.5. Spontaneous intercalation of tetramethylammonium followed by sonication in water allowed for large‐scale delamination of this new titanium carbonitride into 2D sheets. Multilayer Ti₂C_0.5N_0.5T_x powders showed higher specific capacities and larger electroactive surface area than those of Ti₂CT_x powders. Multilayer Ti₂C_0.5N_0.5T_x powders show a specific capacity of 182 mAh g⁻¹ at 20 mA g⁻¹, the highest among all reported MXene electrodes as SIBs with excellent cycling stability. image

The lightweight, rechargeable lithium‐ion battery is one of the dominant energy storage devices globally in portable electronics due to its high energy density, no memory effect, wide operating voltage, lightweight, and good charge efficiency. However, due to safety concerns, the depletion of lithium reserves, and the corresponding increase of cost, an alternative battery system becomes more and more desirable. To develop alternative battery systems with low cost and high material abundance, for example, sodium, magnesium, zinc, and calcium, it is important to understand the chemical and electronic structure of materials. Soft X‐ray spectroscopy, for example, X‐ray absorption spectroscopy (XAS), X‐ray emission spectroscopy (XES), and resonant inelastic soft X‐ray scattering (RIXS), is an element‐specific technique with sensitivity to the local chemical environment and structural order of the element of interest. Modern soft X‐ray systems enable operando experiments that can be applied to amorphous and crystalline samples, making it a powerful tool for studying the electronic and structural changes in electrode and electrolyte species. In this article, the application of in situ/operando (soft) X‐ray spectroscopy in beyond lithium‐ion batteries is reviewed to demonstrate how such spectroscopic characterizations could facilitate the interpretation of interfacial phenomena under in situ/operando condition and subsequent development of the beyond lithium‐ion batteries.