Self-assembling, nanophase-separated multi-block copoly(arylene sulfone)s, selectively swelled with ethylene carbonate, provide excellent single-ion conductivity and cycling stability for high-energy lithium/Li[Ni1/3Co1/3Mn1/3]O2 batteries.

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The aqueous processing of lithium-ion battery (LIB) electrodes has the potential to notably decrease the battery processing costs and paves the way for a sustainable and environmentally benign production (and recycling) of electrochemical energy storage devices. Although this concept has already been adopted for the industrial production of LIB graphite anodes, the performance decay of cathode electrodes based on transition metal oxides processed in aqueous environments is still an open issue. In this study, we show that the addition of small quantities of phosphoric acid into the cathodic slurry yields Li[Ni0.33 Mn0.33 Co0.33 ]O2 electrodes that have an outstanding electrochemical performance in lithium-ion cells.

stability, power density, and safety. [1,3,4] Among the alternative electrode materials, transition metal sulfides (TMSs) are quite appealing due to their improved safety and high theoretical capacity (e.g., CuS: 560 mAh g −1 ; CoS 2 : 870 mAh g −1 ; and FeS 2 : 894 mAh g −1 , as calculated for the full conversion reaction). [4] Important, compared to other conversion materials, e.g., oxides, TMSs usually show improved electronic conductivity as well as faster reaction kinetics due to the weaker metal-sulfur bond (compared to the metal-oxygen bond), making the conversion reaction easier. [4] In addition, the voltage hysteresis of sulfides (≈0.7 V) is distinctly lower than that of oxides (≈0.9 V), thus promising better energy efficiencies. [5] Manganese sulfide (α-MnS) is particularly appealing as anode material for LIBs, as it possesses a large theoretical capacity (616 mAh g −1 ) and a lower redox potential compared to other TMSs, such as copper, cobalt, and iron sulfides-besides being highly abundant, ecofriendly, and less expensive. [3,6,7] Despite these advantages, the application of α-MnS as anode material in LIBs has been hampered due to common problems of TMSs such as: (i) serious volume variation during repeated (dis)charge processes leading to poor cycling stability, and (ii) low rate capability arising from low electronic conductivity and Li-ion mobility. [3,7] In order to improve the lithium-ion storage performance of TMSs, many approaches have been proposed. One of the most efficient strategies, so far, is to fabricate nano/microstructured composite materials, Herein, a Mn-based metal-organic framework is used as a precursor to obtain well-defined α-MnS/S-doped C microrod composites. Ultrasmall α-MnS nanoparticles (3-5 nm) uniformly embedded in S-doped carbonaceous mesoporous frameworks (α-MnS/SCMFs) are obtained in a simple sulfidation reaction. As-obtained α-MnS/SCMFsshows outstanding lithium storage performance, with a specific capacity of 1383 mAh g −1 in the 300th cycle or 1500 mAh g −1 in the 120th cycle (at 200 mA g −1 ) using copper or nickel foil as the current collector, respectively. The significant (pseudo)capacitive contribution and the stable composite structure of the electrodes result in impressive rate capabilities and outstanding long-term cycling stability. Importantly, in situ X-ray diffraction measurements studies on electrodes employing various metal foils/disks as current collector reveal the occurrence of the conversion reaction of CuS at (de)lithiation process when using copper foil as the current collector. This constitutes the first report of the reaction mechanism for α-MnS, eventually forming metallic Mn and Li 2 S. In situ dilatometry measurements demonstrate that the peculiar structure of α-MnS/SCMFs effectively restrains the electrode volume variation upon repeated (dis)charge processes. Finally, α-MnS/SCMFs electrodes present an impressive performance when coupled in a full cell with commercial LiMn 1/3 Co 1/3 Ni 1/3 O 2 cathodes.

Li‐garnets are promising inorganic ceramic solid electrolytes for lithium metal batteries, showing good electrochemical stability with Li anode. However, their brittle and stiff nature restricts their intimate contact with both the electrodes, hence presenting high interfacial resistance to the ionic mobility. To address this issue, a strategy employing ionic liquid electrolyte (ILE) thin interlayers at the electrodes/electrolyte interfaces is adopted, which helps overcome the barrier for ion transport. The chemically stable ILE improves the electrodes‐solid electrolyte contact, significantly reducing the interfacial resistance at both the positive and negative electrodes interfaces. This results in the more homogeneous deposition of metallic lithium at the negative electrode, suppressing the dendrite growth across the solid electrolyte even at high current densities of 0.3 mA cm−2. Further, the improved interface Li/electrolyte interface results in decreasing the overpotential of symmetric Li/Li cells from 1.35 to 0.35 V. The ILE modified Li/LLZO/LFP cells stacked either in monopolar or bipolar configurations show excellent electrochemical performance. In particular, the bipolar cell operates at a high voltage (≈8 V) and delivers specific capacity as high as 145 mAh g−1 with a coulombic efficiency greater than 99%.