Yonggang Min

Composite polymer electrolytes (CPEs) are promising for all‐solid‐state lithium metal batteries (LMBs), yet their practical implementation is still hindered by sluggish Li ⁺ transport kinetics. This limitation is associated with heterointerfacial mass‐transfer barriers between inorganic fillers and polymer matrices. Herein, a gear‐meshing composite polymer electrolyte (GMCPE) is developed to reduce these barriers and enhance Li ⁺ transport kinetics in CPEs. In this design, the hydroxyl‐ and amino‐rich polydopamine (PDA) coating functions as a molecular gear‐like interfacial coupler, which meshes polymer chains to improve filler/polymer compatibility and anchors anions to promote Li‐salt dissociation, thereby liberating more mobile Li ⁺ . Meanwhile, the Al ₂ O ₃ with a low Li ⁺ diffusion barrier and the three‐dimensional (3D) polyacrylonitrile (PAN) framework synergistically construct continuous Li ⁺ transport pathways while reinforcing mechanical robustness. Consequently, GMCPE achieves an enhanced Li ⁺ transference number of 0.52 and an ionic conductivity of 0.5 mS cm ⁻¹ at 60 °C. Moreover, Li|GMCPE|Li symmetric cells exhibit stable dendrite‐free Li plating/stripping for over 4200 h. All‐solid‐state Li|GMCPE|LiFePO ₄ cells maintain 84.7% capacity retention after 500 cycles at 1 C. This work provides a novel gear‐meshing interfacial design paradigm for advancing accelerated Li ⁺ transport in CPEs toward high‐performance all‐solid‐state LMBs.

Three‐dimensional (3D) architectures can stabilize lithium (Li) metal anodes (LMAs) by mitigating localized charge accumulation and volume fluctuation, but the enlarged anode/electrolyte interfaces aggravate parasitic reactions and unstable solid electrolyte interphase (SEI) evolution. In this study, we constructed a mass‐charge regulatory microdomain‐functionalized LMA (MCRM‐Li) by mechanically integrating a hierarchically structured NiS _x framework with Li foil to address this structure‐interface dilemma. The embedded conductive matrix partitions bulk Li into ordered microdomains and establishes an interconnected electron transport network to dissipate localized current density. Simultaneously, the in situ formed Li ₂ S‐rich interphase suppresses solvent attack and induces Li ₂ S/LiF‐enriched SEI formation during cycling, thereby homogenizing Li ⁺ flux and facilitating interfacial Li ⁺ diffusion. Consequently, the symmetric cell based on MCRM‐Li delivers an ultralong lifespan of over 5380 h with dendrite‐free Li deposition. Moreover, LiFePO ₄ full cells retain 94.1% capacity after 1000 cycles at 2 C. This work provides a coupled structural‐interfacial design paradigm for durable lithium metal batteries through regional control of electric‐field distribution and interfacial mass transfer in operating 3D LMAs.

The cubic Ni0.96S/Co3S4 bimetallic sulfide heterostructure attached on MXene nanosheets and coated with carbon layer was successfully synthesized (shorten as Ni0.96S/Co3S4@MXene-C). The main Ni0.96S and Co3S4 phase are identified by XRD . And the cubic Ni0.96S/Co3S4 bimetallic sulfide heterostructure is measured to be ~600 nm in SEM , which is firmly adhered on the MXene nanosheets. The surface chemical state is further charactered by XPS, which demonstrates the presence of Niv in Ni0.96S/Co3S4@MXene-C and according with XRD result. The existence of Niv can enhance the conductivity, provide more active sites and thereby significantly improve electrochemical performances for Ni0.96S/Co3S4@MXene-C anode in lithium-ion batteries (LIBs). Through the synergistic combination of bimetallic sulfide heterostructure, the carbon layer and MXene, Ni0.96S/Co3S4@MXene-C maintains ~594mAh/g (90% retention) after 350 cycles (at 0.5 A/g). Ni0.96S/Co3S4@MXene-C delivers a practical capacity close to 490 mAh/g (at 4 A/g), which is higher than that of Ni0.96S@MXene-C (~285 mAh/g) and Co3S4@MXene-C (~288 mAh/g) . Furthermore, Ni0.96S/Co3S4@MXene-C also exhibits 76% pseudo-capacitance at 1.0 mV/s, indicating that the charge storage process is mainly dominated by the surface pseudo-capacitive behavior. According to the GITT (Galvanostatic Interlaced Titration Technique) testing, the Li+ discharge diffusion coefficient of Ni0.96S/Co3S4@MXene-C is within the range of 4.35×10-12 to 2.44×10-10. In the Ni0.96S/Co3S4@MXene-C anode, the synergistic effect of the highly conductive MXene and the cubic bimetallic sulfide heterostructure can effectively provide an efficient channel for charge transfer and ion diffusion. This work may also provide a way for the development of other new bi-/multi-metal sulfide composite electrodes for advanced LIBs.

Helium extraction from natural gas demands ultra‐high He/CH ₄ selectivity (>1000), yet this benchmark remains largely unmet by polymeric membranes due to the permeability‐selectivity trade‐off and the challenge of constructing sub‐4 Å sieving channels. Here, we report an orthogonal light–heat dual‐crosslinking strategy to program the free‐volume topology of polyimide membranes. A photoreactive precursor (6FCC‐X) was synthesized via a click reaction by incorporating photosensitive units (C═C─S) and varying amounts of thermally labile─COOH groups into the backbone. UV irradiation first triggers [2+2] cycloaddition to construct a dense and uniform super‐crosslinked network, which defines the primary molecular‐sieving framework. Subsequent thermal decarboxylation generated rigid biphenyl linkages that are proposed to function as molecular‐strut‐like structural motifs, enhancing chain rigidity, improving micropore connectivity, and refining sub‐4 Å sieving constrictions. This sequential topology programming decouples helium transport from methane exclusion, which enables the optimized 6FCC‐3‐CR membrane to achieve a He permeability of 33.9 Barrer and an exceptional He/CH ₄ selectivity of 3767, outperforming most reported polymer‐based membranes and rivaling advanced carbon molecular sieve membranes. This work establishes a molecular‐strut‐mediated topology‐programming principle for polymer molecular sieves, offering a general route to reconcile fast transport with precise molecular exclusion.

Ternary blends represent an effective strategy to improve power conversion efficiency (PCE) of organic solar cells (OSCs). However, most reported third components are fused-ring acceptors with complicated synthesis and high cost, which limits their commercialization. Herein, we introduce an asymmetric, easily synthesized non-fused ring electron acceptor (NFREA) HBTZ as the third component into the PM6:Y6 system to fabricate efficient and low-cost ternary OSCs. The incorporation of HBTZ optimizes the active layer morphology, enhances molecular stacking, suppresses charge recombination, and particularly reduces energy loss. Consequently, the ternary OSCs achieve a superior PCE of 18.02% and enhanced stability, with simultaneously improved open-circuit voltage, short-circuit current density, and fill factor, outperforming the PM6:Y6-based binary device (16.43%). Moreover, quantitative evaluation of synthetic complexity reveals that this ternary strategy reduces the average figure-of-merit by 10.37%, demonstrating enhanced cost-effectiveness of the OSCs. This work highlights that asymmetric NFREAs are promising third components for achieving high-performance and low-cost ternary OSCs, providing guidance for the design of cost-efficient organic photovoltaic systems.