Rechargeable lithium-carbon dioxide (Li-CO2) batteries offer great potential for greenhouse gas use and high-energy-density storage. However, their practical application is hindered by the formation of a thermodynamically stable Li2CO3 (lithium carbonate) product that is hard to decompose during charging. Highly crystalline and conductive reticular material iron polyphthalocyanine (pFeIIPc) as a solid-state redox mediator into Li-CO2 batteries tailors the cathode reaction pathway, enabling stable Li2C2O4 (lithium oxalate) generation and an extraordinary discharge plateau of 3.2 V beyond the theoretical limit. Beyond delivering an ultrahigh discharge capacity of 28,790 milliampere-hours per gram and reversible cyclability over 1400 hours (cutoff capacity of 1000 milliampere-hours per gram) at 100 milliamperes per gram, the Li-CO2 batteries exhibit excellent temperature adaptability (-40 to 80°C). The Li-CO2 pouch cells using pFeIIPc as the solid-state redox mediator achieve a high energy density of 678 watt-hours per kilogram on the basis of total device mass and maintain reversible cycling for 251 hours. Our work pioneers a promising pathway toward practical high-efficiency Li-CO2 batteries.

The advancement of ultrahigh-voltage lithium metal batteries (LMBs) is hindered by the lack of efficient guidelines for electrolyte material development, with current approaches still largely relying on inefficient trial-and-error methods. Herein, we report a high-performance additive design and screening strategy. A library of phosphorus-centered candidates (containing 15,200 molecules) is constructed by simultaneously introducing electron-withdrawing and electron-donating groups to induce intramolecular charge redistribution and tune the electrochemical properties of the molecules. Through unsupervised machine learning-assisted screening, lithium diperfluoropinacolatophosphate (LiDPFP) is identified as the optimal candidate. LiDPFP features localized electron-deficient and electron-rich regions, which tune interfacial reactivity and enhance lithium ion (Li+) coordination to promote contact ion pairs. This unique structure leads to the formation of a phosphorus-oxygen polymer-rich cathode electrolyte interphase and a Li2O (lithium oxide)-rich solid electrolyte interphase, effectively suppressing cathode degradation and lithium dendrite growth. Consequently, the as-assembled NCM811||Li cells exhibit stable cycling at 4.8 volts over a wide temperature range from -40° to 80°C. A practical 4.7-volt pouch cell with the energy density of 628 Wh kg-1 (watt-hours per kilogram) exhibits an 80% capacity retention rate after 112 cycles. This work combines machine learning with molecular design, exhibiting a paradigm for practical ultrahigh-energy-density LMBs.

In this work, we propose a group II/IIIA-based Janus MBene, MgAlB2, and investigate its electrochemical properties using first-principles calculations. The substitution of one Mg layer in Mg2B2 MBene by an Al layer breaks the structural symmetry and generates a permanent out-of-plane polarization, giving rise to a distinct electronic environment compared with the parent Mg2B2 and Al2B2 monolayers. Electronic-structure analysis reveals enhanced orbital hybridization among B, Mg, and Al states near the Fermi level, resulting in improved electronic delocalization across the monolayer. The Janus MgAlB2 monolayer is found to possess excellent dynamical, mechanical, and thermal stability. Owing to its polarization-modified energy landscape, Li ions migrate with an exceptionally low diffusion barrier of 17.1 meV, corresponding to a room-temperature diffusion coefficient of 1.28 × 10[-3] cm[2] s[-1]. Unlike the pristine Mg2B2 and Al2B2 monolayers, which support only a single stable adsorption layer, MgAlB2 accommodates two complete Li layers. Detailed analysis shows that the residual polarization retained after first-layer lithiation continues to promote Li adsorption, whereas increasing Li-Li electrostatic interactions eventually limit further storage. As a result, the Janus monolayer delivers a high theoretical specific capacity of 1470.24 mAh g[-1] together with a small volume expansion of only 3.7% during maximum lithiation. The calculated open-circuit voltage exhibits an average value of approximately 1.20 V, indicating a favorable operating voltage for an anode material. These results demonstrate that Janus-induced dipole-engineering can simultaneously regulate the thermodynamics and kinetics of Li storage, providing an atomistic strategy for designing high-capacity, fast-charging, and structurally favorable two-dimensional anode materials for lithium-ion batteries.

Si-based all-solid-state batteries with sulfide solid electrolytes are strong contenders for next-generation high-safety, high-energy-density batteries. However, Si-based anodes inevitably suffer from irreversible delamination and side reactions at the rigid Si/solid electrolyte interface during cycling, making it challenging to achieve long cycle life. Here, we develop an elastic ion-conducting layer on the Si surface that transforms the rigid interface into a conformal and recoverable elastic contact, achieving highly stable Si anode. The layer comprises a lithium bis(fluorosulfonyl)imide-containing block copolymer, whose hydrogen-bond-rich hard domains provide mechanical robustness and elasticity. Ion-conductive soft segments, together with an in situ-formed inorganic-rich solid electrolyte interphase on the Si surface, construct a three-dimensional ion transport network. This interfacial architecture simultaneously mitigates interfacial stress and accelerates lithium-ion transport within the Si anode. Consequently, the full-cell exhibits stable cycling over 10,000 cycles at a high rate of 5C (8.7 mA cm[-2]), and the 0.6 Ah pouch cell retains 91% capacity after 650 cycles. Such interfacial layer holds great promise for accelerating the commercialization of Si-based all-solid-state batteries.

Managing bipolar disorder in the perinatal period relies on psychopharmacologic treatment due to high rates of postpartum recurrence in the absence of mood-stabilizing medications. Lithium is classically recommended for postpartum bipolar episodes, yet lithium management during pregnancy, labor, and postpartum is complex and clinical practice varies even among reproductive psychiatrists. This case report details a 37-year-old woman with bipolar I disorder whose unexpectedly elevated lithium levels during pregnancy heralded preeclampsia. This case highlights the treatment challenges that arise when complicated psychiatric histories interact with complicated obstetric histories. We address conceptual questions about balancing psychiatric and obstetric risk when developing a medication regimen and illustrate continued dialogue regarding optimal lithium monitoring in the peripartum period.

Observation of battery interfaces is critical, as they govern electron and ion transport and influence electrochemical processes in energy storage. Despite this importance, they are challenging to characterize due to their nanometer-scale thickness and extreme sensitivity to electron beam damage. This paper presents a dose-controlled cryogenic scanning electron nanobeam diffraction (cryo-SEND) protocol that enables structural analysis of beam-sensitive battery interfaces while preserving their native state. The central advance of this workflow is the integration of ice-free cryogenic handling with diffraction-based analysis that decouples structural sensitivity from high-dose image formation. The workflow begins with air-free sample preparation inside an inert-atmosphere glovebox, followed by cryogenic focused ion beam/scanning electron microscopy (cryo-FIB/SEM) milling to produce electron-transparent lamellae. We describe optimized cryogenic transfer procedures from the FIB to the transmission electron microscope, emphasizing the use of a cryo-shuttle equipped with a protective lid to suppress ice contamination during transport. Within the TEM, SEND is performed at cryogenic temperatures to probe interfacial structures at vitrified electrolyte-lithium metal interfaces. SEND enables crystallographic and structural analysis while significantly reducing total accumulated electron dose compared to conventional imaging. Overall, this protocol provides an approach for studying battery interfaces and is broadly applicable to cryogenic electron microscopy investigations of beam-sensitive materials.

Solvate ionic liquids (SILs) are characterised by high thermal and electrochemical stability but suffer from high viscosities and limited ionic conductivities, restricting their application as battery electrolytes. Recently, we introduced water-in-solvate-ionic-liquid (WISIL) electrolytes [Philipp et al., ChemPhysChem, 2026, 27, e70353], demonstrating that the addition of one equivalent of water per [Li][+] substantially improves transport properties while preserving the characteristic chelate structure and broad electrochemical stability window of the parent SIL. Here, we investigate how further addition of water affects the local lithium solvation environment, the stability of the cationic chelate complexes and the resulting transport properties of ternary lithium bis(trifluoromethanesulfonyl)imide:triglyme:water ([Li][NTf2]:G3:H2O) mixtures containing up to eight water equivalents per [Li][NTf2]. Combining molecular dynamics simulations with PFG-NMR, eNMR, viscosity, conductivity and cyclic voltammetry measurements, we show that water gradually replaces G3 within the first lithium coordination sphere, thereby increasingly destabilising and eventually disintegrating the characteristic chelate complexes. These structural changes are directly reflected in the transport properties, leading to higher self-diffusion coefficients and ionic conductivities together with a pronounced decrease in viscosity. While the characteristic SIL coordination motif and concerted [Li][+]-G3 transport persist up to approximately two water equivalents per lithium ion, further dilution leads to increasingly hydrated lithium species and a gradual transition towards a concentrated aqueous electrolyte. These results establish a direct link between microscopic lithium solvation, coordination dynamics and macroscopic transport behaviour, providing valuable design guides for future electrolytes.

Cathode materials hold a crucial position in enhancing the energy density and capacity of lithium-ion batteries (LIBs). Notably, lithium-rich manganese oxide (LRMO) cathode materials boast high density and high capacity (exceeding 250 mAh g[-1]), thus serving as a key element for the further commercialization of LIBs. Nevertheless, LRMO is prone to potential decay and poor cycling performance due to uncontrollable phase transition, so it is urgent to explore the corresponding modification approaches. Compared to LIBs based on liquid organic ester/ether electrolytes, all-solid-state lithium-ion batteries (ASSLIBs) have emerged as promising contenders due to their superior safety, compliance with modern requirements, and longer service life. This review systematically summarizes the challenges and modification strategies of LRMO for ASSLIBs, covering surface coating, interface engineering, lattice doping, and synergistic approaches. The structure-activity mechanisms underlying the improved electrochemical performance are thoroughly analyzed, and the intrinsic correlations between different modification strategies and structural stability as well as interfacial compatibility of LRMO are systematically clarified. Therefore, this review can serve as a reference for promoting the commercialization of high-performance LRMO cathode materials in ASSLIBs.

The structural and dynamical properties of simulation systems consisting of metal organic frameworks (MOFs), particularly MOF-5, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, and two well-known polymers, poly(vinylidene fluoride) (PVDF) and poly(ethylene oxide) (PEO), in different compositions were investigated using classical molecular dynamics (cMD) and well-tempered metadynamics (WT-MD) simulations. The cMD simulations revealed that the PEO-based hybrid electrolyte system containing LiTFSI salt and MOF-5 (System D) exhibits the highest diffusion coefficient for Li[+] ions and comparatively weaker interactions between Li[+] ions and the surrounding TFSI[-] anions than the other investigated systems. The enhanced ionic mobility is attributed to the favorable local environment generated by the incorporation of MOF-5, which facilitates efficient Li[+] ion transport while reducing ion-trapping effects, as evidenced by structural properties in terms of radial distribution functions, structure factors, spatial distribution functions, three-dimensional density distributions, ion pairing, and contact number analysis obtained from cMD. In addition, consistent with the structural properties, the dynamical and thermodynamic properties, evaluated through mean squared displacement and potential of mean force analysis, also indicate a high diffusion coefficient for Li[+] ions and favorable free-energy of Li[+]-PEO interactions in System D. Furthermore, WT-MD simulations demonstrated that System D possesses a relatively lower free-energy barrier for Li[+] ion mobility, indicating energetically favorable ion transport pathways. The combined findings from cMD and WT-MD simulations highlight the critical role of MOF-5 in regulating the dynamics and transport behavior of Li[+] ions. Therefore, this study provides valuable design guidelines for engineering hybrid MOF-polymer electrolytes with optimized ion transport properties for solid-state battery applications.

A new family of carbon-based materials named "Organically synthesised porous carbon" (OSPC) have proven to have exceptional properties as anode materials in lithium-ion batteries. Experimental X-ray photoelectron spectroscopy characterization has confirmed that the framework of OSPC-1 synthesized via two different synthetic routes, OSPC-1a and OSPC-1b, is based upon sp and sp [3] carbon. Strangely, however, the solid-state NMR spectra for both OSPC-1a and OSPC-1b do not appear consistent with this model. Here, we show that a dense highly interpenetrated morphology based on sp and sp [3] carbon can fully rationalize the solid-state NMR spectra of both OSPC-1a and OSPC-1b. We suggest that this structure is dominant, but that the porosity arises from a newly uncovered morphology with an open noninterpenetrated highly porous OSPC-1 framework structure best approximated by the topological features present in the dia, pts-c, and unc-c topologies. This impacts the conductivity and ion storage, properties of OSPC materials and so it is imperative that this is considered when designing new OSPC materials with targeted properties for potential applications.

Metal-sulfur (M-S) batteries are emerging as promising solutions for future energy storage, thanks to their high theoretical energy density and the plentiful supply of sulfur. Among these, sodium-sulfur (Na-S) batteries are gaining popularity as affordable alternatives to lithium-sulfur (Li-S) systems because sodium is widely available and low-cost. However, developing effective room-temperature Na-S batteries for practical use remains challenging because sluggish reaction kinetics, sodium polysulfide dissolution, and shuttle effects together drive rapid capacity degradation. This comprehensive review examines the electrochemical mechanisms governing room-temperature Na-S batteries, with particular emphasis on the solubility and dissolution kinetics of sulfur species across diverse electrolyte systems. It points to the need to synergistically optimise electrolyte chemistry and calls for high-energy (high-concentration liquid, solid/quasi-solid and high-entropy) electrolytes, separator design, and solid-electrolyte interlayer architectures to prevent polysulfide migration and improve electrochemical stability, as well as for advanced experimental approaches (in situ and operando characterisation) and theoretical simulations and machine learning techniques. The review also highlights recent advances in Na-S battery prototypes to evaluate their practical performance and potential for technological adoption. Concluding with a perspective on Na-S batteries within the broader context of metal-sulfur energy storage systems, the review outlines critical directions for future research essential to realising their full practical potential.

Three-dimensional (3D) current collectors are widely explored to suppress lithium dendrite growth in Li metal anodes, particularly under high-current-density operation. Nevertheless, a fundamental mechanistic understanding of Li electrodeposition within such complex 3D architectures remains markedly incomplete. Herein, using a 3D Cu mesh as a model system, we demonstrate that intrinsic heterogeneity in Li[+] transport within 3D architectures promotes localized ion-flux amplification, triggering preferential deposition and dendritic nucleation. Guided by this insight, a gradient-descending electrodeposition is proposed to regulate ion flux distribution, enabling dense, uniform, and strongly adherent bulk-like Li deposition. To mitigate the gravimetric penalty associated with conventional metallic scaffolds, an ultralight PET@Cu 3D current collector is further engineered via polymer metallization, achieving an areal mass reduction of 59.2% relative to the Cu mesh while retaining sufficient electrical conductivity and mechanical robustness. When integrated with the gradient deposition strategy, the resulting PET@Cu@G-Li anodes paired with NMC811 cathodes exhibit high-rate capability and exceptional cycling stability, retaining 90.82% of their initial capacity after 600 cycles at 3C. This work elucidates the critical role of mass-transport heterogeneity in Li electrodeposition within 3D frameworks and offers a practical anode design paradigm that reconciles high power density with high gravimetric energy density in Li metal batteries.

Uniform ionomer distribution and controlled sulfonate adsorption are critical for low-Pt-loading proton exchange membrane fuel-cell membrane electrode assemblies (MEAs), especially at high current density. In conventional Pt/C catalysts, differences between Pt and carbon surfaces promote sulfonate adsorption on Pt and ionomer aggregation on carbon, thereby limiting proton and oxygen transport. Here we show that a single Co atom dipole layer covering Pt/C (SCDC-Pt) regulates the catalyst-ionomer interface through electrostatic attraction between positively charged Co sites and sulfonate groups. The resulting MEA delivers a peak power density of 1.4 W cm[-2] and only 26 mV loss at 0.8 A cm[-2] after 30,000 square-wave cycles, compared with 0.86 W cm[-2] and 75 mV loss for commercial Pt/C under identical conditions. Operando characterization and simulations indicate that surface dipoles promote a more uniform ionomer distribution, suppress sulfonate poisoning of Pt, and stabilize the Pt structure. Electrochemical diagnostics show lower apparent sulfonate coverage (~ 8%) and local O2 transport resistance (38.6 S m[-1]) than those of commercial Pt/C (~ 20% and 48.1 S m[-1]).

Direct recycling of spent lithium-ion battery (LIB) cathodes holds great promise for sustainable materials recovery. However, residual fluorinated impurities, including inorganic fluoride species and polyvinylidene fluoride (PVDF), remain a persistent challenge due to their chemical persistence and heterogeneous distribution. Here, we report an electrochemically driven self-cleaning strategy that enables fluoride-free adaptive direct recycling of spent cathodes. Using LiNi0.5Co0.2Mn0.3O2 (NMC532) as a model system, anodic polarization activates oxygen-evolution-driven surface reconstruction, generating hydroxylated transition metal (TM) interfaces that trigger the cooperative elimination of fluorinated contaminants. Specifically, the reconstruction promotes proton-assisted dissolution of LiF and related inorganic fluoride species, while simultaneously inducing a hydrophobic-to-hydrophilic interfacial transition that weakens PVDF adhesion and facilitates its removal. These coupled redox-hydrolysis-interfacial processes synergistically eradicate fluorinated residues while preserving the bulk composition and structural integrity of the cathode. The regenerated NMC532 delivers a high discharge capacity of 145.1 mAh·g[-1], comparable to commercial material. When implemented in pouch cells, this strategy achieves an inter‑batch capacity variation of less than 1.3%, dramatically outperforming the ∼24.1% variation typical of conventional recycling and meeting commercial consistency standards (± 3%-5%). This reconstruction-enabled self-cleaning strategy is broadly applicable across diverse cathode chemistries, providing a scalable and chemically selective pathway toward impurity‑free, high‑performance battery material regeneration.