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Lithium- and sodium-rich layered transition-metal oxides have recently been attracting significant interest because of their large capacity achieved by additional oxygen-redox reactions. However, layered transition-metal oxides exhibit structural degradation such as cation migration, layer exfoliation or cracks upon deep charge, which is a major obstacle to achieve higher energy-density batteries. Here we demonstrate a self-repairing phenomenon of stacking faults upon desodiation from an oxygen-redox layered oxide Na 2 RuO 3 , realizing much better reversibility of the electrode reaction. The phase transformations upon charging A 2 MO 3 (A: alkali metal) can be dominated by three-dimensional Coulombic attractive interactions driven by the existence of ordered alkali-metal vacancies, leading to counterintuitive self-repairing of stacking faults and progressive ordering upon charging. The cooperatively ordered vacancy in lithium-/sodium-rich layered transition-metal oxides is shown to play an essential role, not only in generating the electro-active nonbonding 2 p orbital of neighbouring oxygen but also in stabilizing the phase transformation for highly reversible oxygen-redox reactions. Here the authors report the evolution of stacking faults in Na 2 RuO 3 showing that there is progressive cation ordering upon charging and notably the stacking faults can disappear. This behavior is driven by cooperative Coulombic interactions and can contribute to stabilizing the phase transformations.

Anode‐less solid‐state batteries offer a pathway to maximize energy density while simplifying device manufacturing. However, the absence of an initial lithium (Li) reservoir demands precise control over Li deposition, a process usually hindered by interfacial instability and the lithiophobic nature of commonly employed current collectors (CCs). Therefore, effective interfacial design is crucial. In this regard, metallic and oxide interlayers offer a promising strategy to improve Li deposition, but detailed insights into their electrochemical behavior in combination with solid electrolytes (SEs) remain poorly understood. Accordingly, we engineer 50 nm thick zinc (Zn) and copper oxide (Cu2O) interlayers sputtered directly onto the LLZO SE, covered by a 600 nm thick Cu CC. The interlayer composition and Li deposition behavior were investigated by using a range of techniques. The results demonstrate that Zn interlayers facilitate Li deposition via in situ formation of Li–Zn alloys. Differently, the Cu2O interlayers drive Li2O formation, which contributes to more homogeneous Li deposition. The stability of alloying and conversion processes are studied to assess the impact on cycling performance. Overall, this work provides insights into the implementation of alloying and conversion‐based interlayers in solid‐state anode‐less systems and highlights key performance‐limiting factors, offering interfacial design strategies for further improvement. Schematic illustration of the nanometric Zn and Cu2O interlayers deposited by sputtering for anode‐less solid‐state batteries, accompanied by the voltage profile during the initial lithium plating process.

High‐voltage cathodes such as LiMn1.5Ni0.5O4 (LNMO) offer promising energy density but suffer from interfacial degradation accelerated at elevated voltages and temperatures. Here, we present a comprehensive comparative study of three Li3PO4 coating methods (precipitation, sol–gel, and dry sol–gel routes) applied to commercial LNMO powders. Coating quality and intimacy are systematically assessed using a correlative, multitechnique approach including 7Li and 31P solid‐state NMR, X‐ray diffraction, and electrochemical testing. A key insight from this study is the use of ssNMR relaxation behavior as a sensitive probe of coating intimacy to the active phase. The methodology is validated on commercial LNMO and reproduced in a lab‐synthesized LNMO to demonstrate reproducibility across particle morphologies. Among all methods, the sol–gel route produced a uniform ∼20 nm coating with optimal surface contact, translating to improved rate capability and outstanding high‐temperature cycling stability (87% retention after 100 cycles at 50 °C compared to 29% for the non‐coated LNMO), while retaining rate capability. These findings establish a practical framework for designing robust interfacial coatings in high‐voltage lithium‐ion battery materials. This study evaluates three Li3PO4 coating methods (precipitation, sol‐gel and dry sol‐gel) for enhancing the cycling stability of LiMn1.5Ni0.5O4 high‐voltage cathodes. We introduce a coating assesment methodology using solid‐state nuclear magnetic resonance, X‐ray diffraction, and electrochemical testing to assess coating quality. The sol‐gel method shows superior uniformity, improving rate capability and high‐temperature cycling stability, with implications for battery material design.

P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 layered oxide is a promising high energy density cathode material for sodium-ion batteries. However, one of its drawbacks is the poor long-term stability in the operating voltage window of 1.5–4.25 V vs Na + /Na that prevents its commercialization. In this work, additional light is shed on the origin of capacity fading, which has been analyzed using a combination of experimental techniques and theoretical methods. Electrochemical impedance spectroscopy has been performed on P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 half-cells operating in two different working voltage windows, one allowing and one preventing the high voltage phase transition occurring in P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 above 4.0 V vs Na + /Na; so as to unveil the transport properties at different states of charge and correlate them with the existing phases in P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 . Supporting X-ray photoelectron spectroscopy experiments to elucidate the surface properties along with theoretical calculations have concluded that the formed electrode-electrolyte interphase is very thin and stable, mainly composed by inorganic species, and reveal that the structural phase transition at high voltage from P2- to “Z”/OP4-oxygen stacking is associated with a drastic increased in the bulk electronic resistance of P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 electrodes which is one of the causes of the observed capacity fading. P2-Na 2/3 [Fe 1/2 Mn 1/2 ]O 2 is a promising high energy density cathode material for rechargeable sodium-ion batteries, but its poor long-term stability in the operating voltage window of 1.5–4.25 V vs Na + /Na hinders its commercial application. Here, the authors use a combination of electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and DFT calculations to investigate the origin of the capacity fading, which is attributed to an increase in bulk electronic resistance at high voltage that, among other factors, is nested in a structural phase transition.

Classical electrodes for Li-ion technology operate by either single-phase or two-phase Li insertion/de-insertion processes, with single-phase mechanisms presenting some intrinsic advantages with respect to various storage applications. We report the feasibility to drive the well-established two-phase room-temperature insertion process in LiFePO 4 electrodes into a single-phase one by modifying the material’s particle size and ion ordering. Electrodes made of LiFePO 4 nanoparticles (40 nm) formed by a low-temperature precipitation process exhibit sloping voltage charge/discharge curves, characteristic of a single-phase behaviour. The presence of defects and cation vacancies, as deduced by chemical/physical analytical techniques, is crucial in accounting for our results. Whereas the interdependency of particle size, composition and structure complicate the theorists’ attempts to model phase stability in nanoscale materials, it provides new opportunities for chemists and electrochemists because numerous electrode materials could exhibit a similar behaviour at the nanoscale once their syntheses have been correctly worked out. Electrodes exhibiting single-phase lithium insertion processes can be advantageous for storage applications such as lithium-ion batteries. By modifying the particle size and ion ordering of LiFeFO 4 electrodes an unprecedented single-phase room-temperature process is observed.

The program FAULTS has been used to simulate the X-ray powder diffraction (XRD), neutron powder diffraction (NPD), and electron diffraction (ED) patterns of several structural models for LiNi1/3Mn1/3Co1/3O2, including different types of ordering of the transition metal (TM) cations in the TM slabs, different amounts of Li+/NiII+ cation mixing and different amounts of stacking faults. The results demonstrate the relevance of the structural information provided by NPD and ED data as compared with XRD to characterize the microstructure of NMC (LiNi1−y-z Mn y Co z O2) compounds.

Breakthroughs in battery research are imperative to provide society with batteries that are safe and sustainable, have a high energy density, and have a long cycle life at low cost. Recent advances in research methodologies, the emergence of new market opportunities, and strategic funding schemes have allowed not only large, but also small companies, universities, and public research organizations to play an increasingly significant role in the advancement of battery technology. Challenges in battery technology development are multifaceted; therefore, a collaborative approach is crucial to bring together various stakeholders and ensure access to the full range of technical and scientific expertise. To grasp the core properties of electrode materials, electrolytes, and interfaces and to identify the mechanisms of battery degradation and failure, a multidisciplinary analytical approach is crucial. This strategy relies on the unique and complementary potential of advanced characterization techniques available at synchrotron and x-ray free electron laser facilities. Science-to-industry interactions are expected to increase the development of new standardized setups to approach realistic operando conditions. Therefore, rapid access to instruments, including high-throughput ex-situ , in-situ and operando capabilities, is key to accelerating the development of safe and sustainable batteries. The purpose of this paper is to discuss how the characterization needs of the battery community can be met by establishing a collaboration network based on a meta-infrastructure model, where the emphasis will be on collaboration and the sharing of experience and data. The proposed methodology considers the urgency in the battery community and the necessary technical developments to reach the scope of collaboration and focuses in particular on the needs for standardization, big data challenges, and open data approaches.

High‐voltage cathodes such as LiMn 1.5 Ni 0.5 O 4 (LNMO) offer promising energy density but suffer from interfacial degradation accelerated at elevated voltages and temperatures. Here, we present a comprehensive comparative study of three Li 3 PO 4 coating methods (precipitation, sol–gel, and dry sol–gel routes) applied to commercial LNMO powders. Coating quality and intimacy are systematically assessed using a correlative, multitechnique approach including 7 Li and 31 P solid‐state NMR, X‐ray diffraction, and electrochemical testing. A key insight from this study is the use of ssNMR relaxation behavior as a sensitive probe of coating intimacy to the active phase. The methodology is validated on commercial LNMO and reproduced in a lab‐synthesized LNMO to demonstrate reproducibility across particle morphologies. Among all methods, the sol–gel route produced a uniform ∼20 nm coating with optimal surface contact, translating to improved rate capability and outstanding high‐temperature cycling stability (87% retention after 100 cycles at 50 °C compared to 29% for the non‐coated LNMO), while retaining rate capability. These findings establish a practical framework for designing robust interfacial coatings in high‐voltage lithium‐ion battery materials.

Responsible disposal and recycling are essential for the sustainability of the battery market, which has been exponentially growing in the past few years. Under such a scenario, the recycling of materials of less economic value, but environmentally much more sustainable like LiFePO4, represents an economic challenge. In this paper an approach to recover used FePO4 electrodes from calendar aged Lithium-ion (Li-ion) batteries and their reuse in Sodium-ion (Na-ion) cells is proposed. The electrochemical performances of the Na-ion cell are shown to be comparable with previously reported values and, since the electrode can retain the original microstructure and distribution, electrode processing can be avoided. A proof of concept of a NaFePO4//hard carbon full cell using a very high positive electrode loading optimized for Li-ion batteries (≈14 mg cm−2) is shown.

Responsible disposal and recycling are essential for the sustainability of the battery market, which has been exponentially growing in the past few years. Under such a scenario, the recycling of materials of less economic value, but environmentally much more sustainable like LiFePO 4 , represents an economic challenge. In this paper an approach to recover used FePO 4 electrodes from calendar aged Lithium-ion (Li-ion) batteries and their reuse in Sodium-ion (Na-ion) cells is proposed. The electrochemical performances of the Na-ion cell are shown to be comparable with previously reported values and, since the electrode can retain the original microstructure and distribution, electrode processing can be avoided. A proof of concept of a NaFePO 4 //hard carbon full cell using a very high positive electrode loading optimized for Li-ion batteries (≈14 mg cm −2 ) is shown.