http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

This study investigates the high-field breakdown and energy dissipation of multilayer PdSe2 FETs, with a focus on the interfacial thermal transport at the PdSe2/SiO2 interface. The research proposes optimization strategies to enhance device performance and improve the thermal management, paving the way for the more efficient next-generation electronic and optoelectronic devices.

The continuous miniaturization of 2D electronic circuits results in increased power density during device operation, leading to heat localization and placing higher demands on their performance thresholds. The risk to thermal breakdown and subsequent damage, due to the energy dissipation in the 2D semiconductor field-effect transistors (FETs) supported on the bulk substrates, represents a significant challenge in maintaining their optimal performance. Herein, this study investigates energy dissipation behavior in multilayer PdSe2 FETs for the first time. The high-field breakdown behavior is firstly studied in multilayer PdSe2 FETs on SiO2/Si substrates, where a maximum current density of ≈2.74 MA cm−2 is observed, which is comparable to that of multilayer black phosphorus FET and significantly higher—by about five times—than that of multilayer MoS2 FET. Additionally, the thermal boundary conductance (TBC) of PdSe2/SiO2 interface is measured at room temperature using Raman thermometry. The TBC is found to be ≈12–13 MW m−2 K−1, which is relatively low compared to the other known solid–solid interfaces, indicating that enhancing the performance of PdSe2 FETs can be possible by optimizing the TBC at the PdSe2/SiO2 interface. These findings provide valuable insights for design of high-quality and high-performance PdSe2 electronic and optoelectronic devices.

An in situ multifunctional polymer interface layer with high-efficiency Zn2+ transport is prepared through the pre-established ion transport pathways of an innovative electrolyte initiator. This layer promotes rapid Zn2+ desolvation and uniform Zn2+ deposition, effectively suppressing interfacial side reactions and dendrite growths, thereby significantly extending the cycle life of aqueous zinc-metal batteries.

Achieving stable zinc-metal anodes is pivotal to realizing high-performance aqueous zinc-metal batteries (AZMBs). The construction of a functional polymer interface layer on the zinc-metal anode surface is confirmed as an effective strategy for mitigating dendrite growth and side reactions, thereby significantly enhancing the stability of zinc-metal anode. However, polymers capable of withstanding electrolyte environments over the long term typically suffer from elevated interfacial impedance, which hinders Zn2+ transport. Here, a pioneering zinc-metal anode enabled by a functional polymer interface layer with high-efficiency ion transport is introduced. This polymer layer is polymerized in situ on the zinc-metal anode surface through an innovative redox initiation system, where zinc trifluoromethanesulfonate (Zn(OTf)2) salts function as both reductant and ion transport pre-pathways, ensuring high-efficiency ion transport. The resultant interface layer achieves an ideal balance of ionic conductivity, water resistance, adhesion, and mechanical properties, effectively suppressing dendrite growth and side reactions. Symmetric cells assembled with this interface layer deliver an impressive lifespan of 8800 and 1600 h under 1 and 5 mA cm−2, respectively. This interface layer further demonstrates exceptional feasibility and versatility in Zn-NVO and Zn-PANI batteries. This work provides groundbreaking insights into the strategic design of high-performance polymer interface layers for AZMBs.

Multiple resonances thermally activated delayed fluorescence emitter is developed by synergizing multiple charge-transfer excited states, exhibiting excellent photoluminescence properties with a narrowband emission of 21 nm, rapid reverse intersystem crossing rate of 7.8 × 105 s−1 and suppressed concentration quenching, and electroluminescence performances with high maximum external quantum efficiencies and low-efficiency roll-offs in wide doping concentrations ranges of 3–50 wt.%.

The development of multiple resonances thermally activated delayed fluorescence (MR-TADF) emitters exhibiting high efficiency, narrowband emission, rapid reverse intersystem crossing rate (k RISC), and suppressed concentration quenching simultaneously is of great significance yet a formidable challenge. Herein, an effective strategy is presented to realize the above target by synergizing multiple charge-transfer excited states, including short-range charge transfer (SRCT), through-bond charge transfer (TBCT), and through-space charge transfer (TSCT). The proof-of-concept emitter 4tCz2B exhibits a bright green emission with a narrow full width at half maximum (FWHM) of 21 nm (0.10 eV) in solution, high photoluminescence quantum yield of 97%, fast k RISC of 7.8 × 105 s−1 and significantly suppressed concentration quenching in film state. As a result, the sensitizer-free organic light-emitting diodes (OLEDs) achieve maximum external quantum efficiencies (EQEmaxS) of over 34.5% together with an unaltered emission peak at 508 nm and FWHM of 26 nm at doping concentrations ranging from 3 to 20 wt.%. Even at a doping ratio of 50 wt.%, EQEmax is still as high as 25.5%. More importantly, the non-sensitized devices exhibit significantly reduced efficiency roll-offs, with a minimum value of 13.4% at a brightness of 1000 cd m−2.

An alcogel-based vertical thermal diode smart wall with interfacial evaporation for ambient thermal energy harvesting and spontaneous cooling/heating supply to the built environment. Owing to the vertical thermal diode structure design, the evaporation-condensation-based smart wall (ECSW) features flexible climate-adaptative heat transfer characteristics with a heat transfer coefficient from 3.33 to ≈30 W m−2 K−1 and building energy savings at 66.47% in Kunming.

Traditional building envelopes with constant thermophysical properties constrain their capabilities in temperature regulation. Whether it is possible to achieve single-direction heat transfer along building envelopes with climate-adaptative thermophysical properties to enhance passive heat gain in winter and thermal dissipation in summer? In this work, through the capillary effect in interfacial evaporation and thermal diode structure, single-direction heat transfer with passively adjustable thermal properties in a vertical building envelope is practically achieved. An evaporation-condensation-based smart wall (ECSW) is manufactured for spontaneous and continuous cooling/heating supply to the built environment. The ECSW features climate-adaptative heat transfer characteristics with heat transfer coefficient transiting from 3.33 to ≈30 W m−2 K−1. Additionally, coupling with radiant cooling and photothermal capabilities, ECSW shows excellent thermal performances, i.e., a heat transfer at 5.44 W m−2 by radiant cooling with a 5 °C cooler surface, and a heat transfer at 387.68 W m−2 under solar illumination at 1000 W m−2. Simulation results show that the ECSW enables building energy savings at 66.47% in Kunming. This study first reports vertical thermal diode building envelopes utilizing natural heating/cooling sources through interfacial evaporation for passive temperature regulation with low costs, performance stability and energy-saving potentials for smart and sustainable buildings.

A mixed ionic-electronic conducting 3D host is employed in solid-state batteries to modulate lithium plating and stripping behaviors, which can occur away from the interface to tackle dendrite and void formation issues. In situ electron microscopies and molecular dynamics simulations reveal the Li transport pathways in carbon-based Li metal anodes, which enable faster Li diffusion and high stripping capacity.

Solid-state lithium metal batteries (SSLMBs) are now under intensive research for their high energy density and excellent safety. However, the Li transport limitation in Li metal anode (LMA) leads to mass/stress accumulation, dendrite initiation and void formation at the interface, which seriously hinders the development of SSLMBs. Herein, it is demonstrated through in situ electron microscopies that a mixed ionic-electronic conducting (MIEC) 3D host can promote the Li transport in LMA by increasing the diffusion pathways along the carbonaceous framework, carbon/Li interface and Li metal surface, enabling a fast and long-distance (nearly 100 µm) diffusion of Li atoms in LMA. Consequently, the spatio-temporal sequence of Li plating/stripping can be fundamentally changed. Specifically, both deposition and dissolution can occur far away from the interface, thereby mitigating the dendrite and void issues. Impressively, the resulting cells with carbonaceous hosts can achieve excellent cyclability and the highest capacity (28.8 mAh cm−2) so far. This work provides valuable insight for understanding Li transport and deposition/dissolution mechanisms in MIEC host-based LMAs, and a feasible solution for tackling the interface issues without involving stack pressure in SSLMBs.

Biological processes rely on the concerted action of channels with different functionalities embedded in the same membrane. Inspired by nature, heterogeneous nanopore arrays are prepared where two nanopores are connected in parallel and function as two different elements of an ionic circuit: a diode and a resistor. The results provide the basis to design ionic circuits that mimic physiological processes and communication.

Much effort in the field of nanopore research has been directed toward reproducing the efficient transport phenomena of biological ion channels. For synthetic nanopores to replicate channel function on the scale of a cellular membrane, it is necessary to consider the modes of crosstalk between channels as well as to develop approaches to prepare nanopore arrays consisting of pores with different transport properties, akin to a membrane in an axon. In this manuscript, first ion concentration polarization (ICP) is identified as the primary means of the crosstalk, and subsequently, the extent and degree of ICP is tuned via targeted chemical modification of the pore walls’ functional groups. Next, two fabrication methods of a model two-nanopore array are presented in a silicon nitride membrane in which one nanopore contains a bipolar ionic junction and functions as an ionic diode, while the other one is a homogeneously charged ionic resistor. The targeted chemical modification of a thin gold layer at the opening of one pore in an array that leaves the other pore located a few tens of nm away, unmodified, is utilized. These results provide an important framework for designing abiotic ionic circuits that can mimic physiological multichannel ion transport and communication.

2D PtSe2 has been demonstrated as high-performance catalyst for electrocatalytic ethanol oxidation. Plasma treatment engineers the surface of single-crystalline PtSe2 by removing Se atoms, resulting in the exposure of PtSe2 (101) facet. Excellent EOR activity and poison-resistance are demonstrated, which is rationalized by in situ electrical transport measurement and theoretical calculations.

The development of efficient electrocatalysts for ethanol oxidation reaction (EOR) is crucial for the potential commercialization of direct ethanol fuel cells, yet it faces significant challenges between catalytic performance and cost-effectiveness. 2D materials have recently emerged as a promising group of electrocatalysts due to their large surface area, efficient charge transport, tunable band structures, and excellent catalytic activity. In this study, the novel 2D layered noble-metal dichalcogenide, PtSe2, is explored for efficient ethanol oxidation electrocatalysis from a microscopic perspective based on an on-chip microelectrochemical platform. While pristine PtSe2 demonstrates similar EOR activities to Pt, argon plasma treatment significantly enhances the performance on EOR activity, If/Ib ratio, onset and peak potentials, and durability. Detail investigations reveal that plasma treatment results in the exposure of PtSe2 surface, which is responsible for significantly enhanced EOR activity and poison-resistance as also confirmed by theoretical calculations. In situ electrical transport measurements for monitoring the catalyst surface intermediates, elucidate that both optimized OHads coverage and appropriate ethanol molecular adsorption on PtSe2 are the key for the high performance. This work demonstrates noble-metal dichalcogenides as promising EOR electrocatalysts, and establishes on-chip electrocatalytic microdevice as a promising probing platform for diverse electrocatalytic measurements.

The catalytic cage with carboxyl groups in PEH-COF stabilized the [K(H2O)n]+ ions, which enhanced the PCET kinetics of the conversion for intermediates to methanol, and ultimately allows the PEH-COF to exhibit stable operation at a jCH3OH$\mathrm{j}_{{CH}_3OH}$ of ≈100 mA cm−2.

Developing catalysts for electrocatalytic CO2 to CH3OH still faces great challenge due to the involvement of multiple proton-coupled electron transfer (PCET) processes. Molecular phthalocyanine electrocatalysts on carbon nanotubes have achieved production of methanol as the sole liquid-phase product but with the activity and stability far from meeting industrial demands. Herein, phthalocyaninato cobalt is fabricated into covalent organic frameworks PE-COF via polymerization with ellagic acid. Subsequent hydrolyzation of the ester groups in this framework affords COOH/OH-containing PEH-COF, resulting in the successful modulation over the local microenvironment of Co as electrochemical active center and in turn rendering the production of CH3OH with high yield and durability. Experimental and theoretical investigations reveal that construction of the COOH group and H2O participated catalytic cages in PEH-COF can effectively fix hydrated potassium ions, which efficiently enhances the PCET kinetics and lowers the energy barriers for the conversion of CO2 to CH3OH. The partial current density (j) and Faraday efficiency of methanol for PEH-COF could reach 100.9 mA cm−2 and 38.5%, respectively. Moreover, the jCH3OH$\mathrm{j}_{{CH}_3OH}$ of PEH-COF can be maintained at 100.4 mA cm−2 after 9 h of electrocatalysis, superior to the thus far reported catalysts.

Disorder in a crystal is rarely randomly distributed but instead can involve extra chemical order. This could offer a new degree of freedom that is essential to designing materials with emergent properties. This research achieves the continuous regulation of vacancy order from long-range order to short-range order in cation-deficient half-Heusler crystals. Engagingly, various functionalities present significant changes accompanying the evolution of vacancy order.

Extra chemical order within periodic crystalline lattices offers a promising approach for designing materials with emergent functionalities. However, achieving tunable extra chemical order in crystalline materials remains challenging. Here, it is found that the vacancy order in cation-deficient half-Heusler crystals V1- δ CoSb can be tuned from long-range order (LRO) to short-range order (SRO), or vice versa. The vacancy LRO and SRO configurations are uncovered by scanning transmission electron microscopy analysis and Monte Carlo simulations. Remarkably, the evolution of vacancy order induces profound changes in electrical, magnetic, and thermal properties, as well as hydrogen storage characteristics. In particular, the electronic density of state effective mass exhibits a nearly threefold increase, while ferromagnetism emerges from infancy when tuning the vacancy order from LRO to SRO. These results elucidate the local chemical order-property relationship and highlight the great potential of achieving desirable functionalities by designing extra chemical order in crystalline solids.

High-efficiency narrowband emissive themally activated delayed flurescence (TADF) polymers are realized by incorporating silicon─carbon σ-bond saturated spacers between multiresonance TADF units and polycarbazole backbone. The polymers exhibit a high photoluminescence quantum yield of 97% and external quantum efficiency of up to 30.2% with a narrow full width at half maximum of 42 nm in organic light-emitting diodes.

Achieving both high-efficiency and narrowband emission in thermally activated delayed fluorescence (TADF) polymers remains a formidable challenge. In this work, a proof of concept for narrowband-emissive TADF polymers with a partially conjugated structure is proposed by embedding a silicon─carbon σ-bond saturated spacer between the multiresonance (MR) TADF unit and the polycarbazole backbone. A series of TADF polymers PSix (x = 1, 3, and 6) is then prepared and characterized. All the polymers show narrowband emission with full width at half maximum (FWHM) values of 28–30 nm in a toluene solution. Impressively, polymer PSi3 has the highest photoluminescence quantum yield, reaching 97%, in the doped films due to the efficient reverse intersystem crossing process. The solution-processed devices based on PSi3 exhibit the best performance with a maximum external quantum efficiency (EQE max) of 28.8% and an FWHM of 42 nm. By employing the TADF molecule 5Cz-TRZ as the sensitizer, enhanced device performance with an EQE max of 30.2% is achieved, which is in the first tier among the MR-TADF polymers reported to date. This work provides an effective strategy for achieving highly efficient and narrowband-emissive TADF polymers by controlling the σ-bond saturated spacer between the MR-TADF chromophore and the polymer backbone.

A noninvasive second near-infrared long-wavelength nanosensor (C8R-DSNP) for real-time monitoring of immune cell-tumor interactions in vivo is reported. The sensor detects caspase-8 activation during natural killer cells-induced apoptosis in tumor cells, providing dynamic, early-stage imaging within 4.5 h of treatment. This approach offers valuable insights for optimizing immunocytotherapy strategies with rapid, in vivo feedback.

Immunocytotherapy holds significant promise as a novel cancer treatment, but its effectiveness is often hindered by delayed responses, requiring evaluations every 2–3 weeks based on current diagnostic methods. Early assessment of immune cell-tumor cell interactions could provide more timely insights into therapeutic efficacy, enabling adjustments to treatment plans. In this study, a noninvasive nanosensor (C8R-DSNP) for real-time monitoring of in vivo immune cell activities in the second near-infrared long-wavelength (NIR-II-L) window (1500–1900 nm), which offers deep tissue transparency, is reported. The C8R-DSNP responds rapidly to caspase-8, a key apoptotic signaling molecule generated during interactions between natural killer (NK-92) cells and tumor cells. Using ratiometric NIR-II-L fluorescence imaging, dynamic in vivo observations of NK-92 cells' engagement with tumor cells in a mouse model are captured. These results demonstrate tumor cells apoptosis that happens as early as 4.5 h after NK-92 cells infusion. Additionally, in vitro urine imaging confirmed the initiation of apoptosis via cleaved fluorescent small molecules, while single-cell tracking within blood vessels and tumors further elucidated immune cell dynamics. This real-time NIR-II-L monitoring approach offers valuable insights for optimizing immunocytotherapy strategies.

This study presents a novel composite solid-state polymer electrolyte incorporated dielectric BaTiO3 nanofillers (PDB) for advanced high-voltage all-solid-state lithium batteries. The design achieves a tailored coordination structure, diminished space charge layer, improved ion transport, and enhanced oxidative stability, making this approach a promising strategy for practical long-cycling all-solid-state lithium batteries.

The poor structural stability of polymer electrolytes and sluggish ion transport kinetics of interfaces with cathode limit the fundamental performance improvements of polymer all-solid-state lithium metal batteries under high voltages. Herein, it is revealed that by introducing dielectric BaTiO3 in an in-situ polymerized composite solid-state electrolyte, the generated interaction between the ether group of polymer electrolyte and dielectric material could effectively regulate the lithium-ion (Li+) coordination structure to achieve an oxidative potential higher than 5.2 V. The dielectric BaTiO3 with spontaneous polarization also weakens the space charge layer effect between the cathode and electrolyte, facilitating fast Li+ transport kinetics across the cathode/electrolyte interfaces. The all-solid-state LiNi0.8Co0.1Mn0.1O2/Li batteries with the dielectric composite solid-state electrolyte exhibit an ultra-long cycling life of 1800 and 1300 cycles at room temperature under high cut-off voltages of 4.6 and 4.7 V, respectively. This work highlights the critical role of dielectric materials in high-performance solid-state electrolytes and provides a promising strategy to realize high-voltage long-life all-solid-state lithium metal batteries.

A Li plating regulation strategy that transforms dead Li plating into reversible active Li plating is proposed by using a lithium dendrite inhibitor to realize safe and long-lifespan LIBs. Remarkably, only 1 wt.% single-atom manganese (SAMn) in the Gr anode (Gr-SAMn) is sufficient to achieve a significant improvement, and the amount of dead Li on the Gr anode can be reduced by 90%.

Under harsh conditions, such as high-rate and low-temperature charging, part of Li ions cannot intercalate into the graphite (Gr) particles and will form dendrite-like Li plating, causing capacity fading and serious safety hazards in commercial lithium-ion batteries (LIBs). Herein, instead of eliminating the Li plating, a Li plating regulation strategy that transforms dead Li plating into reversible active Li plating is proposed by using a lithium dendrite inhibitor to realize safe and long-lifespan LIBs. Remarkably, only 1 wt.% single-atom manganese (SAMn) in the Gr anode (Gr-SAMn) is sufficient to achieve a significant improvement, thus both the volumetric and mass-energy density remain roughly unaffected. The amount of dead Li on the Gr anode can be reduced by 90%, thereby enabling much-improved pouch cell performance at high rates and low temperatures. The capacity retention of the Gr-SAMn||NCM811 pouch cell is 86.2% (23.0% higher than that of the pristine Gr||NCM811 pouch) for 1500 cycles at 2 C, and the cell can even be cycled at 5C charge. Even cycling at −20 °C, the average coulombic efficiency (CE) can be improved from 97.95% to 99.94% by using SAMn additive. Hence, this promising strategy provides a novel alternative to solve the Li plating issue.

The carrier transport behavior is regulated rather than the previously oversimplified limitation strategy to reduce losses and enhance energy storage efficiency. It is expected to offer a novel and effective theoretical basis for the design and fabrication of advanced polymer dielectrics with high capacitive energy storage level at harsh environments.

Polymer dielectrics with high capacitive energy-storage levels in harsh environments have become key components in electrostatic capacitors. However, excessive losses in polymer dielectrics caused by high carrier densities at high temperatures and strong electric fields often result in low energy storage efficiency, which is the most challenging problem that urgently needs to be solved. In existing studies, the losses are mainly suppressed by limiting carrier formation; however, it is very challenging to completely limit carrier formation, especially at high temperatures and strong electric fields. Therefore, this perspective proposes to regulate the carrier transport behavior through “guiding/constraining/blocking” forms rather than the previously oversimplified carrier limitation strategy, which further clarifies dominant structure factors that inhibit carrier transport to reduce losses and enhance energy storage efficiency. Meanwhile, the influence of different structural designs on carrier transport behavior, individually or collaboratively, must be systematically studied to determine the specific mode of carrier transport behavior, thereby establishing a relationship between carrier transport behavior and energy storage efficiency. The presented perspective is expected to offer a novel and effective theoretical basis for the design and fabrication of advanced polymer dielectrics with high capacitive energy storage levels in harsh environments.

The degradable additive couple is developed to enable pure and preferential-oriented α-FAPbI3 perovskite with a bandgap of 1.489 eV and robustness against light, heat, and moisture over 1000 h, without the additive residue. The resultant perovskite solar cells achieve a power conversion efficiency of 25.20% with a short current density of 26.40 mA cm−2 and long-term operational stability of over 1000 h.

Pure black-phase FAPbI3 has always been pursued because of its ideal bandgap (E g) and high thermal stability. Here, a pair of sacrificial agents containing diethylamine hydrochloride (DEACl) and formamide (Fo) is reported, which can induce the oriented growth of black-phase FAPbI3 along (111) and will disappear by the aminolysis reaction during perovskite annealing, retaining the E g of FAPbI3 as 1.49 eV. In addition, the tensile strain of the target FAPbI3 is found to be mitigated with a stabilized black phase due to the tilt of FA+. The devices based on the pure and stable black-phase (111)-FAPbI3 achieved a power conversion efficiency of 25.2% and 24.2% (certified 23.51%) with an aperture area of 0.09 and 1.04 cm2, respectively. After 1080 h of operation at the maximum power point under 1-sun illumination (100 mW cm−2), the devices maintained 91.68 ± 0.72% of the initial efficiencies.

A versatile assembly method is developed to uniformly assemble 2D single-crystal copper nanosheets (Cu NS) onto substrates with complex shapes via ultrasonication process. This technique leverages cavitation effects to deposit monolayer Cu NS films with minimal overlap. The assembly is optimized by tuning solvent polarity and substrate surface energy. Demonstrated applications include a resistive heater, highlighting the potential in flexible electronics.

Scalable and cost-effective fabrication of conductive films on substrates with complex geometries is crucial for industrial applications in electronics. Herein, an ultrasonic-driven omni-directional and selective assembly technique is introduced for the uniform deposition of 2D single-crystalline copper nanosheets (Cu NS) onto various substrates. This method leverages cavitation-induced forces to propel Cu NS onto hydrophilic surfaces, enabling the formation of monolayer films with largely monolayer films with some degree of nanosheet overlap. The assembly process is influenced by solvent polarity, nanosheet concentration, and ultrasonic parameters, with non-polar solvents significantly enhancing Cu NS adsorption onto hydrophilic substrates. Furthermore, selective assembly is achieved by patterning hydrophobic and hydrophilic regions on the substrate, ensuring precise localization of Cu NS films. The practical potential of this approach is demonstrated by fabricating a Cu NS-coated capillary tube heater, which exhibits excellent heating performance at low operating voltages. This ultrasonic-driven and selective assembly method offers a scalable and versatile solution for producing conductive films with tailored geometries, unlocking new possibilities for applications in flexible electronics, energy storage, and wearable devices with complex structural requirements.

This study introduce a novel approach to enhancing cathode-SPE compatibility by utilizing the same poly(ionic liquid) (PolyIL)-based material in both the SPE and the cathode binder. A modified biomass-based PolyIL substrate, enriched with highly negatively charged C═O and ─OH groups, is incorporated into the SPE to improve Li+ migration and strengthen its mechanical properties. The Li||LiFePO₄ cell, assembled via in situ photopolymerization, demonstrate stable cycling for over 1100 cycles, while the Li||NCM811 cell operated reliably at a high cut-off voltage of 4.8 V for 100 cycles.

Lithium metal batteries (LMBs) with solid polymer electrolytes (SPEs) offer higher energy density and enhance safety compared to the Li-ion batteries that use a graphite anode and organic electrolytes. However, achieving long cycle life for LMBs while enabling the use of high-voltage cathodes required the compatibility between cathode-SPE, rather than focusing solely on the individual components. This study presente a dual-functional poly(ionic liquid) (PolyIL)-based material that simultaneously serves as an SPE matrix and a cathode binder, constructing a cathode-SPE interface with exceptional (electro)chemical compatibility owing to the high ionic conductivity and wide electrochemical stability window. Additionally, a modified cellulose acetate (CA)-based PolyIL substrate, enriched with C═O and ─OH groups, is designed rationally and incorporated to assist the Li+ migration, leveraging their highly negative charge, and enhancing the mechanical strength of the SPE. Furthermore, an in situ polymerization approach is employed to assemble the cells, improving the physical compatibility at the cathode-SPE interface. As a result, the Li||LFP cell demonstrate stable cycling beyond 1100 cycles, and the Li||NCM811 cell reliably operates at a high cut-off voltage of up to 4.8 V.

Synthesis of topological semimetal TaAs2 nanowires in situ encapsulated with a thin SiO2 shell unravel a richness of intertwined topological phases manifested by their magnetotransport features: A near-room-temperature metal-to-insulator transition, strong expressions of topologically nontrivial surface transport, giant magnetoresistance with direction-dependent sign reversal, chiral anomaly, and a unique double pattern of Aharonov–Bohm oscillations.

Nanowires (NWs) of topological materials are emerging as an exciting platform to probe and engineer new quantum phenomena that are hard to access in bulk phase. Their quasi-1D geometry and large surface-to-bulk ratio unlock new expressions of topology and highlight surface states. TaAs2, a compensated semimetal, is a topologically rich material harboring nodal-line, weak topological insulator (WTI), C2-protected topological crystalline insulator, and Zeeman field-induced Weyl semimetal phases. We report the synthesis of TaAs2 NWs in situ encapsulated in a dielectric SiO2 shell, which enable to probe rich magnetotransport phenomena, including metal-to-insulator transition and strong signatures of topologically nontrivial transport at remarkably high temperatures, direction-dependent giant positive, and negative magnetoresistance, and a double pattern of Aharonov–Bohm oscillations, demonstrating coherent surface transport consistent with the two Dirac cones of a WTI surface. The SiO2-encapsulated TaAs2 NWs show room-temperature conductivity up to 15 times higher than bulk TaAs2. The coexistence and susceptibility of topological phases to external stimuli have potential applications in spintronics and nanoscale quantum technology.

A thermo-electrochemically compatible polymer electrolyte is proposed with a locally conjugated structure through self-regulation of paired tertiary anilines coupled with in situ polymerization, which significantly reconstructs an improved Li+ solvation and enhances electrode/electrolyte interfacial stability of LMBs. This concept provides an important theoretical basis and technical means for achieving practical high energy/power density LMBs.

Pursuing high energy/power density lithium metal batteries (LMBs) with good safety and lifespan is essential for developing next-generation energy-storage devices. Nevertheless, the uncontrollable degradation of the electrolyte and the subsequent formation of inferior electrolyte/electrode interfaces present formidable challenges to this endeavor, especially when paring with transition metal oxide cathode. Herein, a fireproof polymeric matrix with a local conjugated structure is constructed by 4,4′-methylenebis (N, N-diglycidylaniline) (NDA) monomer via in situ polymerization, which promotes the use of ester-based liquid electrolyte for highly stable LMBs. The conjugated tertiary anilines in this PNDA electrolyte effectively tune the Li+ solvation sheath and generate conformal protective layers on the electrode surfaces, resulting in excellent compatibility with both high-voltage cathodes and Li-metal anodes. Moreover, the accumulated electron density endows PNDA with a powerful capability to seize and eliminate the corrosive hydrofluoric acid, which strikingly mitigates the irreversible structure transformation of LiNi0.8Mn0.1Co0.1O2 (NMC) particles. As a result, the PNDA-based Li||LiFePO4 and Li||NMC cells reach excellent electrochemical and safety performance. This study provides a promising strategy for the macromolecular design of electrolytes and emphasizes the importance of “local conjugation” within the polymers for LMBs.

An efficient and safe circular-RNA delivery system circSCMH1@LNP1 is developed for direct nose-to-brain delivery of circRNA SCMH1 to ischemic lesions. Experiments demonstrate that intranasally administrated circSCMH1@LNP1 significantly accumulates in the peri-infarct region of PT stroke mice, thereby improving functional recovery by enhancing synaptic plasticity, vascular repair, neuroinflammation relief, and myelin sheath formation.

Ischemic stroke represents one of the leading cerebrovascular diseases with a high rate of mortality and disability globally. To date, there are no effective clinical drugs available to improve long-term outcomes for post-stroke patients. A novel nucleic acid agent circSCMH1 which can promote sensorimotor function recovery in rodent and nonhuman primate animal stroke models has been found. However, there are still delivery challenges to overcome for its clinical implementation. Besides, its effects on post-stroke cognitive functions remain unexplored. Herein, lipid nanoparticle circSCMH1@LNP1 is established to deliver circSCMH1 and explore its therapeutic efficacy comprehensively. Distribution experiments demonstrate that intranasal administration of circSCMH1@LNP1 significantly increases circSCMH1 distribution in the peri-infarct region and reduces its non-specific accumulation in other organs compared to intravenous injection. Therapeutic results indicate that circSCMH1@LNP1 promotes synaptic plasticity, vascular repair, neuroinflammation relief, and myelin sheath formation, thereby achieving enhanced sensorimotor and cognitive function recovery in post-stroke mice. In conclusion, this research presents a simple and effective LNP system for efficient delivery of circSCMH1 via intranasal administration to repair post-stroke brain injury. It is envisioned that this study may bridge a crucial gap between basic research and translational application, paving the way for clinical implementation of novel circSCMH1 in post-stroke patient management.