Nanoscience News (<front>)

An ionic diode-based drug delivery system is demonstrated, which uses electric potential for spatiotemporally controlled yet sustained drug release with minimal leakage. It provides flow-free drug delivery at scales ranging from nanogram to microgram. In a tumor-bearing mouse model, it shows superior anti-tumor efficacy and reduced off-target immune toxicity compared to intratumoral drug injection.

Drug delivery systems hold promise for delivering cytotoxic drugs by controlling the timing and location of the drug release. However, conventional delivery mechanisms often fall short of achieving spatiotemporally controlled yet sustained release, which is crucial for ensuring drug efficacy and minimizing impact on surrounding tissues. Here, an ionic diode-based drug delivery system is reported that is controlled by an electric potential and capable of releasing drugs at scales ranging from nanogram to microgram. The migrated drug is slowly but continuously diffused to the lesion through the hydrogel at the desired rate. The ionic diode provides flow-free drug delivery while minimizing unintended drug leakage over prolonged periods. Implanted in a freely moving tumor-bearing mouse model, the system filled with doxorubicin demonstrated superior anti-tumor efficacy and minimal off-target immune toxicity compared to the intratumoral injection of free doxorubicin. With its mechanically compliant and biocompatible components, the system offers a safe and readily translatable approach to patients with surgically unresectable tumors.

The non-equilibrium microwave-powered liquid metal depolymerization is proposed for converting various polyolefin wastes into high-value olefin monomers and narrowband hydrocarbon oils by introducing. By leveraging the self-separation feature of liquid metals and their exceptional chemical-bond activation ability under microwave field, an unprecedented high turnover frequency of 2.83 kgPlastic mLLiquid metal −1 is achieved.

Upcycling waste plastics is highly promising to tackle global white pollution while achieving sustainable development. However, prevailing approaches often encounter challenges in scalable engineering practices due to either insufficient plastic upcycling capability or arduousness in the separation, recovery, and purification of catalysts, which inevitably augments the cost of plastic upcycling. Here, the microwave-powered liquid metal synergetic depolymerization is presented to facilitate low-cost plastic upcycling. By leveraging the fluidity of liquid metals and their exceptional chemical-bond activation ability under microwave field, this method efficiently converts various polyolefins into narrowband hydrocarbon oil (Oil yield: 81 wt.% for polypropylene (PP), 85.9 wt.% for polyethylene (PE)) and high-value olefin monomers (C2-4  selectivity: 50% for PE, 65.3% for PP) over 30 successive cycles, resulting in a high turnover frequency of 2.83 kgPlastic mLLiquid metal −1. These captivating advantages offered by electromagnetically-powered liquid metals are also supported by their self-separation features, thereby paving the way for large-scale engineering solutions in waste plastic upcycling.

A novel acetamide-based eutectic electrolyte with enhanced solvation chemistry design, combined with a widened operation voltage range to induce hydrogen evolution reaction, forms a robust solid-electrolyte-interphase layer, mitigating electron tunneling and significantly improving the cycle stability of high-voltage aqueous Li-ion batteries.

Water is pursued as an electrolyte solvent for its non-flammable nature compared to traditional organic solvents, yet its narrow electrochemical stability window (ESW) limits its performance. Solvation chemistry design is widely adopted as the key to suppress the reactivity of water, thereby expanding the ESW. In this study, an acetamide-based ternary eutectic electrolyte achieved an ESW ranging from 1.4 to 5.1 V. The electrolyte confines water molecules within the primary solvation sheath of Li-ions, reducing the free water and breaking the hydrogen bond network. Despite this, initial capacity retention is suboptimal due to inadequate formation of solid-electrolyte-interphase (SEI) layers. To address this, additional hydrogen evolution reaction is induced by widening the operation voltage range, thereby optimizing the SEI layer to mitigate the electron tunneling effect. This approach resulted in a denser LiF-rich SEI layer, effectively preventing water decomposition and improving long-term cycle stability. The optimized SEI layer reduced the electron tunneling barrier, achieving a discharge capacity of 152 mAh g−1 at 1 C and maintaining 76% of its capacity (116 mAh g−1) after 1000 cycles. This study highlights the critical role of both solvation structure and SEI layer optimization in enhancing the performance of high-voltage aqueous Li-ion batteries.

A vascularized patient-derived tumor organoid (PDTO)-on-a-chip with a hierarchical, tumor-specific microvasculature is developed, enabling high-resolution, real-time visualization of dynamic interactions within the tumor's perivascular niche. This platform effectively models tumor-driven angiogenesis and migration, highlighting its potential as a valuable tool for assessing metastatic risk and guiding clinical strategies.

While tumor organoids have revolutionized cancer research by recapitulating the cellular architecture and behaviors of real tumors in vitro, their lack of functional vasculature hinders their attainment of full physiological capabilities. Current efforts to vascularize organoids are struggling to achieve well-defined vascular networks, mimicking the intricate hierarchy observed in vivo, which restricts the physiological relevance particularly for studying tumor progression and response to therapies targeting the tumor vasculature. An innovative vascularized patient-derived tumor organoids (PDTOs)-on-a-chip with hierarchical, tumor-specific microvasculature is presented, providing a versatile platform to explore tumor-vascular dynamics and antivascular drug efficacy. It is found that highly metastatic tumor cells induced vessel angiogenesis and simultaneously migrated toward blood vessels via the Notch pathway. The evident association between the angiogenic and migratory capacities of PDTOs and their clinical metastatic outcomes underscores the potential of the innovative platform for evaluating tumor metastasis, thus offering valuable insights for clinical decision-making. Ultimately, the system represents a promising avenue for advancing the understanding of tumor metastasis and developing personalized treatment strategies based on patient-specific tumor characteristics.

A method of electrochemical pulsing which forms a spinel-like δ phase in Mn-rich disordered rocksalt materials with Li-excess (DRX) (DRX) cathode materials is demonstrated. This concept is extended to large single-crystalline particles, greatly improving the cycling stability. X-ray diffraction, scanning electron nanodiffraction (SEND) and atomic resolution STEM-HAADF were used to reveal a nanodomain spinel structure separated by antiphase boundaries.

Mn-rich disordered rocksalt materials with Li-excess (DRX) materials have emerged as a promising class of earth-abundant and energy-dense next-generation cathode materials for lithium-ion batteries. Recently, an electrochemical transformation to a spinel-like “δ” phase has been reported in Mn-rich DRX materials, with improved capacity, rate capability, and cycling stability compared with previous DRX compositions. However, this transformation unfolds slowly over the course of cycling, complicating the development and understanding of these materials. In this work, it is reported that the transformation of Mn-rich DRX materials to the promising δ phase can be promoted to occur much more rapidly by electrochemical pulsing at elevated temperature, rate, and voltage. To extend this concept, micron-sized single-crystal DRX particles are also transformed to the δ phase by the same method, possessing greatly improved cycling stability in the first demonstration of cycling for large, single-crystal DRX particles. To shed light on the formation and specific structure of the δ phase, X-ray diffraction, scanning electron nanodiffraction (SEND) and atomic resolution STEM-HAADF are used to reveal a nanodomain spinel structure with minimal remnant disorder.

A highly stretchable 3D multielectrode array (sMEA) with protruding microelectrodes is presented, achieved through structural design of a non-stretching material and over-electrodeposition of PEDOT:PSS. sMEA enables tight contact with organoids despite exposure to buoyant force in medium, resulting in electrophysiological signals with a high signal-to-noise ratio (SNR). High SNR signals allow for non-invasive functional assessment of the organoids for drug screening.

Organoids are 3D biological models that recapitulate the complex structures and functions of human organs. Despite the rapid growth in the generation of organoids, in vitro assay tools are still limited to 2D forms. Thus, a comprehensive and continuous functional evaluation of the electrogenic organoids remains a challenge. Here, a highly stretchable 3D multielectrode array (sMEA) with protruding microelectrodes is presented for functional evaluation of electrogenic organoids. The optimized serpentine structures with bridge structures cover the surface of the organoids conformally even in immersion. The protruding microelectrodes form a stable contact with the organoids and allow electrophysiological recordings with high signal-to-noise ratio (SNR). sMEAs are fabricated in wafer-scale for repeatable, scalable, and mass production and packed into an easy-to-use, user-friendly, and robust microwell for fast dissemination of technology. The versatility of sMEA is validated by measuring electrophysiological signals from cardiac spheroids and midbrain organoids with a wide range of sizes from 500 to 1500 µm. Also, electrophysiological signals recorded with high SNR enable functional evaluation of the effects of drugs. The proposed sMEA with high SNR and user-friendly interface could be the key player in high-throughput drug screening, 3D spatiotemporal mapping of electrogenic organoids, and standardization of protocols for quality assessment.

Herein, a novel strategy is proposed that reinforces hole consumption to boost the oxidation half-reaction and ultimately the photocatalytic H2 production. This is achieved by the rational design of noble-metal-free cocatalysts as efficient oxidative sites, promoting the generation of sacrificial agents (CH3O−). Such a strategy can achieve a record apparent quantum efficiency of up to 65.8%.

Achieving efficient and sustainable hydrogen production through photocatalysis is highly promising yet remains a significant challenge, especially when replacing costly noble metals with more abundant alternatives. Conversion efficiency with noble-metal-free alternatives is frequently limited by high charge recombination rates, mainly due to the sluggish transfer and inefficient consumption of photo-generated holes. To address these challenges, a rational design of noble-metal-free cocatalysts as oxidative sites is reported to facilitate hole consumption, leading to markedly increased H2 yield rates without relying on expensive noble metals. By integrating femtosecond transient absorption spectroscopy with in situ characterizations and theoretical calculations, the rapid hole consumption is compellingly confirmed, which in turn promotes the effective separation and migration of photo-generated carriers. The optimized catalyst delivers an impressive photocatalytic H2 yield rate of 57.84 mmol gcat −1 h−1, coupled with an ultrahigh apparent quantum efficiency reaching up to 65.8%. Additionally, a flow-type quartz microreactor is assembled using the optimal catalyst thin film, which achieves a notable H2 yield efficiency of 0.102 mL min−1 and maintains high stability over 1260 min of continuous operation. The strategy of reinforcing hole consumption through noble-metal-free cocatalysts establishes a promising pathway for scalable and economically viable solar H2 production.

A novel strategy for developing self-adaptive zwitterionic polysilazane coatings with excellent mechanical robustness and broad-spectrum antiadhesion properties is proposed. The developed coatings exhibits excellent wear resistance, good flexibility, strong adhesion, and high transparency as well as anti-biofouling, anti-liquid adhesion, and anti-scaling properties. They have potential applications in marine industries, optical devices, pipeline transportation, and other fields.

Antiadhesive coatings have been extensively studied owing to their wide applications in biology, environment, and energy. However, developing a mechanically robust coating with broad-spectrum antiadhesion properties remains challenging. Herein, a novel strategy for preparing hard yet flexible and self-adaptive zwitterionic polysilazane coatings with broad-spectrum antiadhesion properties (anti-biofouling, anti-liquid adhesion, and anti-scaling) is proposed. The coatings are prepared by combining polysilazane with a telomer (FT) consisting of a low-surface-energy fluorine motif and hydrolysis-induced zwitterions. Before Si─OH generation in polysilazane, the fluorine motif drives the zwitterionic precursor to enrich on the surface, generating a zwitterionic layer following pre-hydrolysis. This unique design prevents the coatings from swelling in water, allowing them to adapt to diverse environments. The fluorine motif can orient toward the surface of air, providing anti-liquid adhesion capabilities, whereas the zwitterions orient underwater to endow anti-biofouling, anti-liquid adhesion, and anti-scaling capabilities. The highly cross-linked network toughened by FT contributes to the high hardness (up to 7H) and good flexibility of the coating. The chemical bonding between the coating and substrates ensures their strong adhesion (≈2.06–7.67 MPa). This study contributes to the design of mechanically robust broad-spectrum antiadhesive coatings applicable in marine industries, optical devices, pipeline transportation, and other fields.

Optimized electrodeposition dynamics help mitigate severe hydrodynamic fluctuations and hydrogen embrittlement issues, which not only refines the Zn deposition quality but also cultivates high-index Zn (112) texture, rendering durable Zn metal batteries.

Electrodeposition is promising to fabricate Zn electrodes affording nonepitaxial single-crystal textures. Previous research endeavors focus on achieving Zn(002) faceted deposition, nevertheless, the popularization of a high-index Zn plane with favorable electrochemical activity remains poorly explored. There also exists a deficiency in the assessment of the electrodeposited quality of Zn. Here, a straightforward strategy to address such concerns by cultivating predominant Zn(112) texture via a potentiostatic electrodeposition mode is reported. By precisely identifying the “limiting” conditions for electrodeposition, a striking balance between improved deposition quality, tailored deposition kinetics, and suppressed hydrogen evolution is found. (002) Faceted Zn electrode is shown that be indeed produced, yet the rampant hydrodynamic convection and hydrogen embrittlement issue under such “over-limiting” preparation conditions pose challenges in the electrode lifespan. In contrast, an optimized deposition minimizes hydrodynamic disturbances and mitigates the hydrogen embrittlement effect, where the thus-generated high-index (112)-textured Zn electrode manifests impressive deposition quality and demonstrates holistic cycling stability. The pouch cell by pairing a ZnxV2O5 (ZnVO) cathode manages a reversible capacity of ≈130 mAh and a capacity retention of 98.42%. This study offers guidance for the development of dendrite-free and hydrogen-embrittlement-relieved Zn anodes, unleashing the potential of high-index plane textures for advanced Zn batteries.

Precise and efficient treatment of orthotopic small-size glioblastoma is realized in this work by fully taking advantage of two-photon excitation and an aggregation-induced emission photosensitizer. The proposed photosensitizer with a large two-photon absorption cross-section, the second near-infrared excitation, the first near-infrared emission, and prominent ROS generation, contributes to remarkable tumor growth inhibition and an ultra-deep imaging depth in the brain.

The existence of residual small-size tumors after surgery is a major factor contributing to the high recurrence rate of glioblastoma (GBM). Conventional adjuvant therapeutics involving both chemotherapy and radiotherapy usually exhibit unsatisfactory efficacy and severe side effects. Recently, two-photon photodynamic therapy (TP-PDT), especially excited by the second near-infrared (NIR-II) light, offers an unprecedented opportunity to address this challenge, attributed to its combinational merits of PDT and TP excitation. However, this attempt has not been explored yet. On the other hand, the lack of high-performance photosensitizers (PSs) also hinders the progress of TP-PDT on GBM. Based on those, a robust TP-PS, termed MeTTh, is constructed intendedly through elaborately integrating multiple beneficial design strategies into a single molecule, which simultaneously achieves excellent NIR-II excitation, large absorption cross-section, aggregation-induced NIR-I emission, and prominent Type I/II reactive oxygen species generation. Aided by nanofabrication, an impressive brain structure imaging depth of 940 µm is realized. Moreover, MeTTh nanoparticles smoothly implement precise and efficient treatment of small-size GBM in vivo under a 1040 nm femtosecond laser irradiation. This study represents first-in-class using TP-PDT on GBM, offering new insights for the therapy of small-size tumors in complex and vital tissues.

The study indentifies localized excitons confined by substrate defects in the MoSe2/CrSBr heterostructure, thereby underscoring the pivotal role of intrinsic defects in modulating excitonic properties. Distinctive proximity-induced behaviors, including opposite valley polarization evolutions of MoSe2 excitons and novel in-plane anisotropic emissions, are reported. This work deepens the understanding of spectrally resolved proximity effects in magnetic van der Waals heterostructures.

Despite extensive studies on magnetic proximity effects, the fundamental excitonic properties of the 2D semiconductor-magnet heterostructures remain elusive. Here, the presence of localized excitons in MoSe2/CrSBr heterostructures is unveiled, represented by a new photoluminescence emission feature, X*. Our findings reveal that X* originates from excitons confined by intrinsic defects in the CrSBr layer. Additionally, the degrees of valley polarization of the X* and trion peaks exhibit opposite polarities under a magnetic field and closely correlate with the magnetic order of CrSBr. This is attributed to spin-dependent charge transfer across the heterointerface, supported by density functional theory calculations which reveal a type-II band alignment. Furthermore, the strong in-plane anisotropy of CrSBr induces unique polarization-dependent responses in MoSe2 emissions. This study highlights the crucial role of defects in shaping excitonic properties and offers valuable insights into spectrally resolved proximity effects in semiconductor-magnet van der Waals heterostructures.

Thin film Diamond Like Carbon (DLC) on roll-to-roll gravure printing cylinders offers superior conductive ink transfer to flexible substrates compared to chrome. It enables fine lines and intricate structures for flexible electronics and security applications. DLC supports high-volume production of flexible microelectronics and micro-scale battery components, providing a more sustainable alternative to rigid electronics and reducing the carbon footprint.

Diamond-Like Carbon (DLC), a thin-film material, is emerging as a promising alternative for durable surfaces due to its eco-friendly application process. This study evaluated the use of thin-film DLC on the wafer surface of gravure cylinders for roll-to-roll printing of fine-line electrodes and microtext patterns, specifically for applications in flexible electronics and graphics security. Results suggested that using thin film DLC on the wafer surface allows reliable reproduction of isometric grids and line structures with widths of 15, 20, and 30 µm, as well as solid electrodes. The uniform conformity of thin-film DLC on the wafer surface, featuring an engraved micron-size cell structure, demonstrates superior ink transfer onto flexible PET (polyethylene terephthalate) substrates. This results in increased electrode line width and reduced electrical resistance compared to chrome. Statistical analysis confirmed the reliability and repeatability of the findings. Visual analysis of lines and microtext also demonstrated the reliable print-reproducing capabilities of DLC-coated surfaces. Overall, these results suggest that thin-film DLC is a promising alternative for use as a protective layer on gravure wafer surfaces. It has the potential to produce high-quality, high-volume electronics, such as sensors, antennas, and batteries, for applications in the Internet of Things (IoT) and other sustainable technologies.

A combination of advanced structural characterization at local and average scales and theoretical calculations reveals that the macroscopic rhombohedral-tetragonal phase coexistence of (K,Na)NbO3-based piezoceramics is essentially an average projection of collective local disordered units exhibiting the order-disorder behavior. The field-induced polarization rotation with a change in the degree of ordering is found to play a key role in boosting the functional properties of the investigated ferroelectrics.

Phase boundary is highly recognized for its capability in engineering various physical properties of ferroelectrics. Here, field-induced polarization rotation is reported in a high-performance (K, Na)NbO3-based ferroelectric system at the rhombohedral-tetragonal phase boundary. First, the lattice structure is examined from both macroscopic and local scales, implementing Rietveld refinement and pair distribution function analysis, respectively. The macroscopic phase coexistence at the phase boundary can be interchangeably rationalized with an average projection of collective local disordered units, exhibiting the order–disorder nature. The structural evidence of field-induced polarization rotation is provided by the in situ synchrotron study. Theoretical studies including density functional theory calculation and molecular dynamics simulation also predict the polarization rotation mechanism. The simulation result reveals the variation of the degree of ordering during the polarization rotation as a key feature of the boosted electrical properties in the order–disorder ferroelectric system. The discovery provides meaningful insight into the design of ferroelectrics with enhanced physical properties.

By utilizing anthracene and metalloporphyrin as the active components for the activation of oxygen and the catalysis of intramolecular cross-oxidation coupling reaction, respectively, a series of photosensitive and stable tandem heterogeneous COF catalysts are constructed for realizing the efficient photosynthesis of 4-quinazolinones. Particularly, TAPP-Cu-An enables one-step, gram-scale photosynthesis of 4-quinazolinones in a short time and under mild conditions.

The dehydrogenative cross-coupling reaction is the premier route for synthesizing important 4-quinazolinone drugs. However, it usually requires high reaction temperature and long reaction time, and the yield of the final product is low. Here two stable and photosensitive covalent-organic frameworks (COFs), TAPP-An and TAPP-Cu-An are purposefully designed and constructed to serve as unprecedented heterogeneous tandem catalysts to complete dehydrogenative cross-coupling reactions in a short time and under mild reaction conditions (room temperature and light), leading to the high-efficient photosynthesis of 4-quinazolinones. Particularly, TAPP-Cu-An is the best heterogeneous catalyst currently available for the synthesis of 4-quinazolinones, even surpassing all the catalysts reported so far. It also enables one-step photosynthesis of 4-quinazolinones with higher conversion (>99%) and selectivity (>99%) in a shorter time, and the product can be easily prepared on a gram scale. Extensive experiments combined with theoretical calculations show that the excellent photogenerated charge separation and transport capability, as well as the synergistic An-Cu catalysis in TAPP-Cu-An are the main driving forces for this efficient reaction.

A sulfonate-based deep eutectic electrolyte (DEE) composed of prop-1-ene-1,3-sultone (PES) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) without additional additives is developed. The unique Li+−PES−TFSI− coordination structure in the DEE facilitates rapid ion transport. Meanwhile, the strengthened α−H···F coordination broadens the electrochemical stability window of the DEE, thereby enabling the cycle stability of high-capacity and high-voltage cathode materials in lithium metal batteries.

The safety and cycle stability of lithium metal batteries (LMBs) under conditions of high cut-off voltage and fast charging put forward higher requirements for electrolytes. Here, a sulfonate-based deep eutectic electrolyte (DEE) resulting from the eutectic effect between solid sultone and lithium bis(trifluoromethanesulfonyl)imide without any other additives is reported. The intermolecular coordination effect triggers this eutectic phenomenon, as evidenced with nuclear magnetic resonance, and thus the electrochemical behavior of the DEE can be controlled by jointly regulating the coordination effects of F···H and Li···O intermolecular interactions. The DEE with a properly coordinated environment of Li+ presents a low motion barrier and a high transport rate of localized Li+, leading to a 10 C fast-charging LiFePO4||Li battery with a capacity retention of 95.1% after 500 cycles. Meanwhile, the strengthened α−H···F coordination broadens the electrochemical stability window of the DEE, thus enabling the cycle stability of high-capacity and high-voltage cathode materials in LMBs, e.g., a cycle stability at 4.5 V in the LiNi0.88Co0.07Mn0.05O2||Li battery with a capacity retention of 81.0% after 500 cycles, and an excellent compatibility in 4.5 V LiCoO2||Li and 4.8 V Li1.13Mn0.517Ni0.256Co0.097O2||Li batteries. The practical applicability of the carefully designed DEE is underscored through successful implementation in pouch cells.

Customized multi-metal sites within covalent organic frameworks (COFs) offer a versatile platform for optimizing catalytic performance by precisely tuning metal composition based on their inherent properties. Specifically, the incorporation of oxophilic rare-earth La into the dual Cu COF steers CO2 electroreduction selectivity from C2H4 to CH4, which realizes the directional regulation of catalytic products.

Customizing multi-metal site catalysts for achieving controllable CO2 reduction reaction (CO2RR) product tuning holds immense promise yet poses formidable challenges. The traditional synthesis method of multi-metal sites is the pyrolysis of metal-containing precursors, which is inherently uncontrollable. Herein, a bottom-up strategy is employed to customize and synthesize multi-metal sites in covalent organic frameworks (COFs), aiming to controllably switch the CO2 reduction selectivity by regulating the electronic structure of active sites. Briefly, La element provides chances for manipulating and finetuning the electronic structure of the customized dual Cu sites, and converts the main catalytic product of CO2RR from ethylene to methane. Density functional theory calculations show that the introduction of La alters the electronic structure around Cu, enhances CO2 and H2O activation, and changes the formation of energy barriers of key intermediates. To the best of the author's knowledge, this study constructed the first example of customized multi-metal site COF catalysts and provided new ideas for controllable modulation of products.

The repaired LiNi0.5Co0.2Mn0.3O2 by direct recycling technology shows an unsatisfactory cycle life. Local lattice stress is introduced into the regenerated cathode during repair. The resulting stress gradient leads to the localization of the phonon mode and changes the phonon dispersion relation of materials, inhibits TM atoms migration and the formation of defect structures. The regenerated cathode exhibits good electrochemical performance.

Direct recycling technology can effectively solve the environmental pollution and resource waste problems caused by spent lithium-ion batteries. However, the repaired LiNi0.5Co0.2Mn0.3O2 (NCM) black mass by direct recycling technology shows an unsatisfactory cycle life, which is attributed to the formation of spinel/rock salt phases and rotational stacking faults caused by the in-plane and out-of-plane migration of transition metal (TM) atoms during charge/discharge. Herein, local lattice stress is introduced into the regenerated cathode during repair. The resulting stress gradient leads to the localization of the phonon mode and changes the phonon dispersion relation of materials, lowers the bending and stretching vibration frequencies of the TM─O covalent bond in cathode materials, and inhibits the TM atoms migration and the formation of defect structures. Beneficial from the favorable low-frequency phonon dispersion relation, the regenerated NCM represents remarkably enhanced structural stability during cycling, and exhibits good electrochemical performance. This reconstructed phonon dispersion relation approach broadens the perspective for lattice stress field engineering to suppress the defective structure raised from TM migration and paves the way for the development of regenerated cathodes with long durability.

A highly modulated interlayer spacing is observed for the first time in the epitaxial 2D spirals with electron correlations. Scalable synthesis of the epitaxial TaS2 spirals is achieved with customized CVD reactions. An intertwined CDW-Mott state appears at room-temperature in the epitaxial 1T-TaS2 spirals, offering a platform to study collective properties at high temperatures.

Tantalum disulfide (1T-TaS2), being a Mott insulator with strong electron correlation, is highlighted for diverse collective quantum states in the 2D lattice, including charge density wave (CDW), spin liquid, and unconventional superconductivity. The Mott physics embedded in the 2D triangular CDW lattice has raised debates on stacking-dependent properties because interlayer interactions are sensitive to van der Waals (vdW) spacing. However, control of interlayer distance remains a challenge. Here, spiral lattices in the epitaxial TaS2 spirals are studied to probe collective properties with tunable interlayer interactions. A scalable synthesis of epitaxial TaS2 spirals is presented. A more than 50%-increased interlayer spacing enables prototype decoupled monolayers for enhanced electronic correlation exhibiting Mott physics at room-temperature and a simplified system to explore collective properties in vdW materials.

A novel hydrogel bioadhesive taking the structural advantage of phenylalanine derivative for interfacial drainage and matrix toughening as well as various electrostatic interactions mediated by zwitterions is reported. The hydrogel adhesive can not only realize fast hemostasis and accelerated tissue/organ injuries healing in vivo but also can be assembled as bioelectronics for precise and long-term health monitoring under humid environments.

Hydrogel bioadhesives with adequate wet adhesion and swelling resistance are urgently needed in clinic. However, the presence of blood or body fluid usually weakens the interfacial bonding strength, and even leads to adhesion failure. Herein, profiting from the unique coupling structure of carboxylic and phenyl groups in one component (N-acryloyl phenylalanine) for interfacial drainage and matrix toughening as well as various electrostatic interactions mediated by zwitterions, a novel hydrogel adhesive (PAAS) is developed with superior tissue adhesion properties and matrix swelling resistance in challenging wet conditions (adhesion strength of 85 kPa, interfacial toughness of 450 J m−2, burst pressure of 514 mmHg, and swelling ratio of <4%). The PAAS hydrogel can not only realize fast hemostasis of liver, heart, artery rupture, and sealing of pulmonary air-leakage but also accelerate the recovery of stomach and liver defects in rat, rabbit, and pig models. Moreover, PAAS hydrogel can precisely and durably monitor various physiological activities (pulse, electrocardiogram, and electromyogram) even under humid environments (immersion in water for 3 days), and can be employed for the evaluation of in vivo sealing efficiency for artery rupture. The work provides a promising hydrogel adhesive for clinical hemostasis, tissue injury repair, and bioelectronics.

The reversibility and activity of anionic redox reactions in lithium-rich manganese-based oxides (LRMOs) for all-solid-state batteries (ASSBs) are significantly enhanced by the simultaneous incorporation of high-binding energy B─O bonds and high-efficiency LBO ionic networks into LRMO. This results in the formation of a robust LRMO-LBO interwoven structure, which stabilizes the layered structure and LRMO|solid electrolyte interface, thereby contributing to superior long-term cycling stability in ASSBs.

The use of lithium-rich manganese-based oxides (LRMOs) as the cathode in all-solid-state batteries (ASSBs) holds great potential for realizing high energy density over 600 Wh kg−1. However, their implementation is significantly hindered by the sluggish kinetics and inferior reversibility of anionic redox reactions of oxygen in ASSBs. In this contribution, boron ions (B3+) doping and 3D Li2B4O7 (LBO) ionic networks construction are synchronously introduced into LRMO materials (LBO-LRMO) by mechanochemical and subsequent thermally driven diffusion method. Owing to the high binding energy of B─O and high-efficiency ionic networks of nanoscale LBO complex in cathode materials, the as-prepared LBO-LRMO displays highly reversible and activated anionic redox reactions in ASSBs. The designed LBO-LRMO interwoven structure enables robust phase and LBO-LRMO|solid electrolyte interface stability during cycling (over 80% capacity retention after 2000 cycles at 1.0 C with a voltage range of 2.2–4.7 V vs Li/Li+). This contribution affords a fundamental understanding of the anionic redox reactions for LRMO in ASSBs and offers an effective strategy to realize highly activated and reversible oxygen redox reactions in LRMO-based ASSBs.