A series of intensely blue-emissive ortho-linked donor-acceptor conjugates comprising triarylamine donors and cyanopyridine or benzonitrile acceptors was readily synthesized via the bromine-lithium exchange-borylation-Suzuki (BLEBS) sequence in moderate to good yields. The modular synthetic approach enables systematic variation of conformational constraint as a molecular design element for tailoring excited-state properties. Cyclic voltammetry reveals irreversible dimerization of triarylamine derivatives lacking para-substituents. Photophysical studies in the solid state, solution, and polymethylmethacrylate (PMMA) matrix reveal photoluminescence quantum yields (PLQY) of up to 70%, emission bandwidths as narrow as 2480 cm-1 (47 nm), and CIE 1931 coordinates approaching the standard blue point. Phenylene extension increases conformational constraint around the acceptor, inducing hypsochromically shifted emission and providing an additional structural handle for tuning the optical properties. Pronounced positive emission solvatochromism, aggregation-induced emission enhancement (AIEE), temperature-dependent spectroscopy, and quantum-chemical calculations consistently indicate that conformational modulation governs charge-transfer interactions, excited-state relaxation, and triplet-state accessibility. Together, the experimental and theoretical results establish structure-property relationships that provide design principles for the rational engineering of future blue-emissive organic chromophores.

Aqueous zinc-iodine batteries (ZIBs) and lithium-sulfur batteries (LSBs) are promising energy-storage systems because of their high theoretical energy density and relatively abundant active materials. However, both systems suffer from severe shuttle effects and sluggish redox kinetics, which considerably hinder their practical applications. Here, an imidazolium-containing cationic covalent triazine framework (iCTF-BCIM) is rationally designed as a bifunctional host and catalyst to address common challenges of both ZIBs and LSBs. Specifically, the resulting iodine-loaded iCTF-BCIM cathode (I2@iCTF-BCIM) delivers an ultra-long cycling life of more than 100 000 cycles at 5 A g-1, with a capacity retention of 97.2% and a Coulombic efficiency approaching 100%. In situ and ex situ spectroscopic analyses demonstrate that the I2@iCTF-BCIM electrode undergoes a highly reversible iodine redox process. Furthermore, LSBs assembled with sulfur-loaded iCTF-BCIM cathode, denoted as S@iCTF-BCIM, deliver a high specific capacity of 1275 mAh g-1 at 0.2 C (1 C = 1675 mA g-1), along with remarkable cycling stability. More importantly, theoretical calculations combined with experimental results reveal that imidazolium-derived cationic environments contribute to regulating the adsorption and conversion behavior of electrochemical intermediates in both ZIBs and LSBs. This work demonstrates the applicability of iCTF-BCIM as a common host catalyst for both ZIBs and LSBs.

Ideal solid-state electrolytes (SSEs) should simultaneously possess excellent ionic conductivity, mechanical strength, electrochemical stability, and cathode compatibility. Here, inspired by the hierarchical architecture of organisms like the lotus leaf, a micro-nano hierarchical composite electrolyte was fabricated via in situ growth of a bifunctional metal-organic framework (F&OH-ZIF-8) on a cellulose acetate (CA) substrate. The micro- and nano-sized F&OH-ZIF-8 crystals have the same composition but exhibit different size-dependent advantages. The micro-sized crystals provide greater structural continuity and mechanical support, whereas the nano-sized crystals offer more accessible polar sites and interfacial regions for Li+ coordination and transport. Their cooperative integration suppresses dendrite penetration and stabilizes the electrode/electrolyte interphases while facilitating Li+ transport. An outstanding SSE with a room-temperature ionic conductivity of 2.9 × 10-3 S cm-1, a lithium-ion transference number of 0.61, and a wide electrochemical stability window extending to 5.5 V was obtained by this strategy, resulting in Li||NCM811 full cells achieving a high-capacity retention of 80.9% after 300 cycles at 1C under a high cut-off voltage of 4.6 V. This strategy of transforming existing commercialized ordinary membrane materials into more valuable electrolyte membranes has extremely high practical significance.

Solid electrolyte interphase (SEI) instability and dead Li accumulation remain persistent challenges for lithium metal batteries. Although considerable efforts have been devoted to optimizing the SEI composition, the issue of dead lithium accumulation remains largely neglected. Herein, we design a covalent organic framework (COF)-based dual-functional separator to regulate the chemical composition of the solid electrolyte interphase to form a LiF/LiBr-rich SEI, while simultaneously introducing Br-/Br3- redox couple in-situ at the interface for dead lithium reactivation. Both theoretical and experimental evidence demonstrate that the introduction of TPPA-Br triggers cleavage of the C-Br bond, leading to the in-situ formation of an ionically conductive LiF/LiBr-rich SEI. The LiF can promote uniform lithium deposition and prevent dead Li formation. Meanwhile, the LiBr can result in Br-/Br3- redox couple, which further chemically reactivates Li2O and electrically isolates Li0, mitigating capacity decay associated with dead Li accumulation. Consequently, Li||LiFePO4 cells employing TPPA-Br functional separators display good cycling stability over 1200 cycles with 90.1% capacity retention at 1 C (1 C=170 mA g-1), confirming the practical potential of this interphase-regulation strategy.

Electrochemical lithium (Li) extraction from low-grade brines is challenged by maintaining high Li selectivity at practically relevant extraction rates while enabling off-grid, round-the-clock operation in remote, infrastructure-deficient regions. Here we propose a solar-powered redox adsorption method (SRAM), in which dissolved, regenerable electron carriers (ECs) deliver electrons to dispersed olivine iron phosphate (o-FePO4) adsorbents. In SRAM, EC-mediated electron transfer enables electrochemically effective use of dispersed o-FePO4 adsorbents, while interfacial charge accumulation and electric double layer (EDL) formation may hinder further access of ECs to the adsorbent surface, thereby moderating local electron flux and suppressing competing-ion intercalation. As a result, SRAM achieves a high extraction rate of 40 mA mmol-1 o-FePO4 while maintaining high selectivity (separation factors of 700 for Li+/Na+ and 2400 for Li+/Mg2+) from low-grade brines (70 ppm Li+). Meanwhile, ECs function as integrated chemical energy-storage media that can buffer intermittent photovoltaic input and temporally decouple charging from Li extraction, enabling solar-buffered day-night operation without an external electrical storage unit. Field demonstrations support stable operation (∼9 mg Li g-1 h-1) and provide a lab-scale validation through 50-L raw brine processing. Our work establishes EC-mediated electron transfer as a promising strategy for sustainable Li recovery from previously untapped low-grade brines.

To address the demand for safe, high-energy-density lithium-metal batteries, we developed a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based composite electrolyte via an "interfacial molecular bridge" strategy. γ-aminopropyltriethoxysilane (APTES) molecules are covalently anchored onto Aluminum oxide (Al2O3) fillers, where the terminal NH2 groups act as Lewis base sites to immobilize bis(trifluoromethanesulfonyl)imide anion(TFSI-) anions, releasing free Li+ and boosting the transference number from 0.42 to 0.66. Concurrently, the uniformly dispersed fillers suppress PVDF-HFP crystallization, creating continuous amorphous pathways that deliver a high ionic conductivity of 7.02 × 10-4 S cm-1 with a low activation energy of 0.11 eV. A "more is less" effect of grafting density is revealed: insufficient grafting fails to inhibit agglomeration, while excessive silane forms an insulating polysiloxane barrier that degrades performance. The optimized electrolyte exhibits a wide electrochemical window (∼5.0 V), robust Li plating/stripping for over 1000 h at 0.1 mA cm-2, and stable cycling in LFP||Li full cells with 86.6% capacity retention over 500 cycles at 0.5C. This work establishes a surface-engineering paradigm for designing high-performance composite solid-state electrolytes.

Among emerging energy storage technologies, lithium (Li) metal anode-based solid-state batteries (SSBs) have drawn considerable attention, as they promise greater energy density alongside improved safety relative to traditional Li-ion cells. Despite this promise, the performance of such systems remains constrained by intrinsic obstacles tied to the nucleation and growth of voids at the Li-solid electrolyte (SE) interface as stripping proceeds. Void morphology and contact distribution jointly dictate the coupled reaction-diffusion behavior at the interface, thereby affecting the interfacial resistance. In the present study, we track the detailed evolution of a single void as Li stripping progresses, characterizing how its shape, size, and overall morphology evolve under the action of the distinct modes of surface diffusion, i.e., terrace, step, and interlayer diffusion. The depth and size attained by the void are strongly governed by coupling between reaction kinetics and the surface diffusion modes, which together dictate the dominant diffusion pathways. In addition, the role of operating temperature in mitigating void growth under high-reaction-rate conditions is examined. Extending the single-void analysis to the collective voids regime, we resolve the progression toward a multi-clustered morphology and determine the critical void fraction value the onset of percolation, beyond which dispersed voids coalesce into a connected network. Understanding these interactions between voids helps identify the mechanisms that control the final interfacial structure and provides guidance for designing stable, low-resistance interfaces in SSBs.

Anode-free sodium metal batteries (AFSMBs) offer a lithium-independent route to high-energy, low-cost storage, but their deployment is constrained by limited sodium inventory and interfacial instability. Without excess sodium, small inefficiencies in nucleation, interphase formation, and cross-electrode reactions accumulate into irreversible capacity loss, and advances in materials design frequently fail to survive practical conditions. Here we establish a mechanism-informed framework that resolves the sodium inventory into reversible, dead, and chemically bound fractions, each tied to a measurable quantity, and apply it across current collectors, electrolytes, cathodes, separators, and solid-state architectures. Because Coulombic efficiency reports only the sum of two loss channels that scale differently, we derive the efficiency required for practical operation rather than assuming it: 500 cycles at N/P = 0 demands an average above 99.95%. Screened against lean-electrolyte and high-areal-capacity criteria, few reported systems approach this threshold, and most omit the electrolyte loading at which their efficiency is obtained. We identify operando diagnostics and quantitative morphological descriptors as the missing tools for predictive design. AFSMBs are therefore integration-limited rather than materials-limited, and progress depends on translating interfacial control into manufacturable cell architectures.

Silicon-based all-solid-state batteries (ASSBs) promise high energy density for next-generation energy storage systems. However, the poor solid-solid contact between silicon (Si) and the solid-state electrolyte (SSE), coupled with interfacial instability during cycling, leads to lithium trapping and parasitic reactions, resulting in a low initial coulombic efficiency (ICE). Herein, we report a solution-assisted in situ polymerization and prelithiation strategy to construct a highly ion-conductive interphase via reductive passivation for Si anodes. Lithium biphenyl replenishes active lithium while inducing the in situ formation of a highly stable hybrid interphase composed of polybiphenyl, lithium bis(trifluoromethanesulfonimide) (LiTFSI), and reductively passivated lithium fluoride. The electrochemically stable and ion-conductive interphase minimizes interfacial ion-transport resistance while suppressing SSE decomposition. The engineered anode delivers an ICE of 100.6% with a high electrode-level reversible capacity of 3215 mAh g-1 at the electrode level, enabling an ICE of 96.4% in LiCoO2 full cells (6.2 mAh cm-2) with 96.6% capacity retention after 300 cycles at 1 C. The all-solid-state pouch cell demonstrates a high energy density of 313 Wh kg-1 with 92.7% capacity retention after 100 cycles. This work underscores the critical role of stable ion-conductive interphase design at Si anodes and provides a viable strategy toward practical high-energy-density ASSBs.

Lithium-rich cathode materials offer significantly higher energy densities than conventional cathode materials, due to their ability to store charge beyond the formal transition-metal redox limit, via so-called "oxygen redox". In lithium-rich oxides, oxygen redox is accompanied by molecular O2 formation and transition-metal migration, associated with irreversible structural change and poor cycling stability. Lithium-rich silicates provide an alternative lithium-rich chemistry, and have been proposed to be resilient to O2 formation at the top of charge, due to their covalently bonded [SiO4]4- framework. We report a computational study of the top-of-charge behavior of the prototypical silicate cathode Li2FeSiO4. Using density functional theory, we predict that fully delithiated FeSiO4 is thermodynamically unstable with respect to oxidation of oxide ions to form molecular O2 within the bulk material. Ab initio molecular dynamics shows this decomposition occurs spontaneously, via a multistep mechanism involving FeIV migration and disproportionation to FeIII and FeV, and subsequent FeV reduction alongside molecular O2 formation. Our findings demonstrate that polyanionic frameworks do not inherently prevent O2 formation in lithium-rich cathodes, and illustrate how different previously proposed oxygen redox mechanisms can function as steps within a compound process.

Bat-origin swine acute diarrhea syndrome coronavirus (SADS-CoV) causes diarrhea and death in piglets and also poses a cross-species transmission risk due to its broad host cell tropism. In the absence of commercial vaccines or therapeutics, identifying the host factors exploited by SADS-CoV may provide potential targets for antiviral therapies. Inhibition of glycogen synthase kinase 3 (GSK3) restricts diverse coronavirus replication by targeting the N protein and disrupting its phosphorylation. Here, we identified GSK3 as a crucial host factor for SADS-CoV RNA synthesis. Both GSK3 deficiency and treatment with a classical GSK3 inhibitor, lithium chloride (LiCl), strongly impaired SADS-CoV dsRNA synthesis. LiCl treatment did not alter electrophoretic mobility or expression of SADS-CoV N protein in N-transfected Huh7 cells but significantly reduced NSP12 protein levels. The absence of GSK3 led to the proteasomal degradation of NSP12 to reduce viral RNA synthesis. However, GSK3 interacted with ubiquitin-specific peptidase 27X (USP27X) and promoted the USP27X-mediated deubiquitination of NSP12, thereby enhancing NSP12 stabilization and facilitating viral RNA synthesis. LiCl not only protected neonatal mice from lethal SADS-CoV challenge but also exhibited a notable broad-spectrum antiviral effect against PEDV and TGEV. Our findings demonstrate that GSK3-mediated NSP12 stabilization is essential for SADS-CoV RNA synthesis, underscoring the potential of GSK3 as a broad-spectrum antiviral target for emerging and re-emerging swine coronaviruses.IMPORTANCEZoonotic transmission of coronaviruses continues to pose a significant threat to human populations. Swine acute diarrhea syndrome coronavirus (SADS-CoV) has been identified as a potentially high-risk emerging coronavirus pathogen that could adversely affect the global economy and human health. However, the replication mechanisms of SADS-CoV remain largely unexplored. Our study demonstrates that GSK3 stabilizes NSP12 by interacting with USP27X, thereby enhancing the synthesis of SADS-CoV dsRNA. LiCl, a GSK3 inhibitor, exhibits broad-spectrum antiviral activity against swine enteric alphacoronaviruses. Our work is distinguished for the first time by the GSK3-USP27X regulatory axis that controls the stability of NSP12 and indicates that GSK3 is a promising therapeutic target for the development of broad-spectrum antiviral drugs against emerging or re-emerging swine coronaviruses.

The aim of this study was to evaluate the hardness and elastic properties of various computer-aided design (CAD)/computer-aided manufacturing lithium disilicate ceramics, including IPS e.max CAD, GC Initial LiSi Block and CEREC Tessera and to assess the impact of repeated firings on these characteristics. Sixty fully crystallized square-plate specimens were generated, 20 for each evaluated material (n = 20), and were subjected to two additional firings. Initially and after each additional firing, hardness and modulus values were measured with a nanoindentation tester. Changes in microstructure and elemental composition were analyzed by field emission scanning electron microscopy and energy-dispersive x-ray spectroscopy. Statistical analysis was conducted in RStudio using linear mixed-effects models, with significance set at α = 0.05. Across all firing cycle protocols, CEREC Tessera specimens exhibited higher Martens hardness values than those of IPS e.max CAD and GC Initial LiSi Block. Firing had the greatest effect on hardness and indentation modulus, with all parameters showing a consistent peak after the first additional firing.