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

By connecting CoTPyP blocks with transition metal nodes, a class of bimetallic 2D MOFs are designed and synthesized. The prepared CoTPyP-M MOFs enhanced the utilization of sulfur and smoothed the lithium deposition/stripping process. The central Co sites display strong interactions with sulfur species through Co−S and Li−N bonds, facilitating the cleavage of S−S bond from both ends and promoting their conversion kinetics in Li−S batteries.

Developing the highly efficient catalysts is a great challenge for accelerating the redox reactions in Li−S batteries. Inspired by the single-atom catalysts and metalloproteins, it makes full use of the advantages of metal–organic frameworks (MOFs) as electrocatalysts. Herein, a series of 2D metal-bonded metalloporphyrin MOFs are prepared with 5,10,15,20-tetrakis(4-pyridyl) cobalt porphyrin (CoTPyP) as building blocks and transition metals (M═Mn, Fe, Co, Ni, and Cu) as nodes, respectively. The crystalline structures of the bimetallic 2D MOFs are confirmed by UV–vis spectra and X-ray diffraction analyses. According to DFT calculation, the peripheral metal nodes optimize the electronic state of Co in porphyrin core. Especially, CoTPyP-Mn facilitates the cleavage of S−S bond from both ends and promotes their conversion kinetics through Co−S and Li−N bonds. The Li−S cells with CoTPyP-Mn show the initial specific capacity of 1339 mA h g−1 at 0.2 C. The capacity decay rate is only 0.0442% per cycle after 1000 cycles at 2 C. This work achieves the rational control of the central Co d electron state through the peripheral regulation and enriches the application of MOFs in accelerating the redox kinetics in Li−S batteries.

Chemically bonded conductive metal-organic framework/polyoxometalate composites are synthesized as a high-performance bifunctional electrocatalyst through a conserved ligand replacement strategy. Excellent performances with a H2O2 production rate of 9.51 mol gcat −1 h−1 and 2, 5-furandicarboxylic acid yield of 96.8% are achieved in an integrated electrolysis system of two-electron oxygen reduction reaction coupling with 5-hydroxymethylfurfural oxidation reaction.

The design of bifunctional and high-performance electrocatalysts that can be used as both cathodes and anodes for the two-electron oxygen reduction reaction (2e− ORR) and biomass valorization is attracting increasing attention. Herein, a conserved ligand replacement strategy is developed for the synthesis of highly ordered conductive metal-organic frameworks (Ni-HITP, HITP = 2, 3, 6, 7, 10, 11-hexaiminotriphenylene) with chemically confined phosphotungstic acid (PW12) nanoclusters in the nanopores. The newly formed Ni−O−W bonds in the resultant Ni-HITP/PW12 electrocatalysts modulate the electronic structures of both Ni and W sites, which are favorable for cathodic 2e− ORR to H2O2 production and anodic 5-hydroxymethylfurfural oxidation reaction (HMFOR) to 2, 5-furandicarboxylic acid (FDCA), respectively. In combination with the deliberately retained conductive frameworks and ordered pores, the dual-functional Ni-HITP/PW12 composites enable a H2O2 production rate of 9.51 mol gcat −1 h−1 and an FDCA yield of 96.8% at a current density of 100 mA cm−2/cell voltage of 1.38 V in an integrated 2e− ORR/HMFOR system, significantly improved than the traditional 2e− ORR/oxygen evolution reaction system. This work has provided new insights into the rational design of advanced electrocatalysts and electrocatalytic systems for the green synthesis of valuable chemicals.

This is a quasi-dry transfer technique assisted by water vapor intercalation (WVI), which can be effectively used to fabricate high-quality twisted heterostructures, including monolayer/few-layer graphene and 2D quasicrystal-like heterostructure. It also enables the fabrication of suspended 2DMs and high-performance devices. This technique features excellent scalability, advancing fundamental research on 2DMs, and the fabrication of quantum devices with outstanding performance.

Transfer technique has become an indispensable process in the development of two-dimensional materials (2DMs) and their heterostructures, as it determines the quality of the interface and the performance of the resulting devices. However, how to flexibly and conveniently fabricate two-dimensional (2D) twisted heterostructures with high-quality interfaces has always been a formidable challenge. Here, a quasi-dry transfer technique assisted by water vapor intercalation (WVI) is developed, which can be flexibly used to fabricate twisted heterostructures. This method leverages a charged hydrophilic surface to facilitate WVI at the interface, enabling the clean and uniform detachment of 2DMs from the substrate. Using this method, the twisted monolayer/few-layer graphene and 2D quasicrystal-like WS2/MoS2, highlighting the surface/interface cleanness and angle-controlled transfer method is successfully fabricated. Besides, suspended structures of these 2DMs and heterostructures are fabricated, which offers substantial convenience for studying their intrinsic physical properties. Further, a high-performance hBN/graphene/hBN superlattice device with the mobility of ≈199,000 cm2 V−1 s−1 at room temperature is fabricated. This transfer technique ingeniously combines the advantages of dry transfer and wet transfer. Moreover, it features excellent scalability, providing crucial technical support for future research on the fundamental physical properties of 2DMs and the fabrication of quantum devices with outstanding performance.

A fluorinated olefin-linked triazine covalent organic framework photocatalyst is developed. The adjacent fluorine atom-olefinic bond forms p–π conjugation and expedites triplet excitons for activating O2 to 1O2 while accelerating charge separation, thus leading to high-efficiency photocatalytic O2 reduction to H2O2 and 5-hydroxymethylfurfural photo-oxidation upgrading.

High-efficiency production of triplet states in covalent organic framework photocatalysts is crucial for high-selectivity oxygen (O2) reduction to hydrogen peroxide (H2O2). Herein, fluorine and partial fluorine atoms are incorporated into an olefin-linked triazine covalent organic framework (F-ol-COF and HF-ol-COF), in which the adjacent fluorine (F) atoms-olefinic bond forms p-π conjugation that induces spin-polarization under irradiation, thus expediting triplet excitons for activating O2 to singlet oxygen (1O2) and contributing to a high H2O2 selectivity (91%). Additionally, the feasibility of coupling H2O2 production with the valorization of 5-hydroxymethylfurfural (HMF) is exhibited. The F-ol-COF demonstrates a highly stable H2O2 yield rate of 12558 µmol g−1 h−1 with the HMF-to-functionalized furan conversion yield of 95%, much higher than the partially fluorinated COF (HF-ol-COF) and the non-fluorinated COF (H-ol-COF). Mechanistic studies reveal that F-incorporation promotes charge separation, intensifies the Lewis acidity of the carbon atoms on the olefinic bond as active sites for O2 adsorption, and provides highly concentrated holes at the triazine unit for HMF oxidation upgrading. This study suggests the attractive potential of rational design of porous-crystalline photocatalysts for high-efficiency photocatalytic O2 reduction to H2O2 and biomass upgrading.

α-Tocopherylquinone (α-TQ), the oxidation product of α-tocopherol (α-TOH), catalyzes the oxidative polymerization of 3,7-dihydrobenzo[1,2-b:4,5-b′]difuran-2,6-dione (HBFDO). The saturated aliphatic chiral side chain of α-TQ suppresses its crystallization, enabling high-conductivity polymer ink without needing post-polymerization dialysis. This scalable method, tested in a 20 L reactor, yields ready-to-use poly(benzodifurandione) (PBFDO) ink.

Conductive polymers have become crucial in advancing various electronic applications. While p-type materials like poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) are widely used and produced at scale, the development of high-performance n-type polymers has lagged due to challenges in synthesis and scalability. In this work, a novel method is introduced to synthesize the highly conductive n-type polymer poly(benzodifurandione) (PBFDO) using α-tocopherylquinone (α-TQ) as a catalyst. This approach eliminates the need for post-reaction dialysis, a major obstacle to large-scale PBFDO production. By preventing catalyst aggregation, high electrical conductivity (>1320 S cm−1) is achieved, which remains stable in air for over 180 d, significantly simplifying the process. The α-TQ-synthesized PBFDO also exhibits excellent thermoelectric properties, with a power factor exceeding 100 µW m−1 K−2, placing it among the highest-performing n-type thermoelectric polymers. Additionally, residual α-TQ acts as a plasticizer, reducing the elastic modulus by over tenfold while maintaining high conductivity, making this material suitable for mechanically compliant electronics. Similarly, residual α-TQ lowers the thermal conductivity of PBFDO by more than an order of magnitude. The process is scalable, as demonstrated by producing high-conductivity ink in a 20 L reactor. This work presents an efficient and sustainable approach for large-scale n-type polymer production.

A simple solution-based method that can achieve pristine (without residual 2D precursors) and phase-pure 2D/3D perovskite heterostructure without the need for synthesizing a single crystal is developed. Perovskite solar cells with this treatment demonstrate a notable improvement in both power conversion efficiency and long-term stability, with negligible hysteresis, compared to the conventional process.

Interface engineering plays a critical role in advancing the performance of perovskite solar cells. As such, 2D/3D perovskite heterostructures are of particular interest due to their optoelectrical properties and their further potential improvements. However, for conventional solution-processed 2D perovskites grown on an underlying 3D perovskite, the reaction stoichiometry is normally unbalanced with excess precursors. Moreover, the formed 2D perovskite is impure, leading to unfavorable energy band alignment at the interface. Here a simple method is presented that solves both issues simultaneously. The 2D formation reaction is taken first to completion, fully consuming excess PbI2. Then, isopropanol is utilized to remove excess organic ligands, control the 2D perovskite thickness, and obtain a phase-pure, n = 2, 2D perovskite. The outcome is a pristine (without residual 2D precursors) and phase-pure 2D perovskite heterostructure with improved surface passivation and charge carrier extraction compared to the conventional solution process. PSCs incorporating this treatment demonstrate a notable improvement in both stability and power conversion efficiency, with negligible hysteresis, compared to the conventional process.

This work reports an OPECT-based chemical MSI with multisensory perception, multimodal synaptic plasticity, and typical MSI features in electrolytes. The advanced MSI device is then used to mimic the associative learning and reflex activities of visual and gustatory stimuli with the associated feedback loops. This work may provide new insight into the development of highly biomimetic MSI in biological fluids for seamless neuro-robotic systems.

Neuromorphic perception capable of multisensory integration (MSI) in electrolytes is important but remains challenging. Here, the aqueous implementation of artificial MSI is reported based on the newly emerged organic photoelectrochemical transistor (OPECT) by representative visual (light)-gustatory (sour) perception. Under the co-modulation of light and H+/OH−, multisensory synaptic plasticity and several typical MSI characteristics are mimicked, including “super-additive response,” “inverse effectiveness effect” and “temporal congruency.” To demonstrate its potential usage, different types of multisensory associative learning and corresponding reflex activities are further emulated. The chemical MSI system is also utilized to control artificial salivation by a closed loop of real-time perception, processing, integration, and actuation to emulate the biological responses toward external stimuli. In contrast to previous solid-state operations, this work offers a new strategy for developing neuromorphic MSI in aqueous environments that are analogous to those in biology.

High-quality single crystals of the noncollinear antiferromagnet Mn3Sn are synthesized, and a non-saturating magnetostriction exceeding 400 ppm under 57 T is observed, surpassing the giant magnetostriction materials such as FeGa. The theoretical analyses indicate that this pronounced non-saturating magnetostriction stems from an exotic exchange striction mechanism, which facilitates a linear relationship between strain output and applied magnetic field.

Magnetostriction, discovered by Joule in 1842, refers to the mechanical strain that a material undergoes in the presence of a magnetic field. Conventionally, it originates from the spin-orbit coupling and has been predominantly explored in ferromagnets. In this work, a giant magnetostriction effect is reported in the high-quality single crystal of a noncollinear antiferromagnet Mn3Sn. Non-saturating magnetostriction exceeding 400 ppm is obtained, which is even larger than the saturation values of the well-known Fe-based giant magnetostriction ferromagnetic materials such as FeGa. Theoretical calculations reveal that the large non-saturating magnetostriction results from a sophisticated exchange striction effect of the noncollinear antiferromagnetic spin structure, leading to a nearly linear dependence of the strain output on the applied magnetic field. This work provides an unprecedented strategy to design next-generation magnetoelastic materials with noncollinear compensated spin structures.

This research introduces an innovative octahedron-like cobalt structure embedded in hierarchical porous nanofibers, significantly optimizing hydrogen peroxide production in acidic environments. Achieving 80% faradaic efficiency at 400 mA cm−2 and maintaining stable operation over 120 h at 100 mA cm−2, this approach provides a scalable and sustainable pathway to enhance industrial hydrogen peroxide generation.

Electrochemically generating hydrogen peroxide (H2O2) from oxygen offers a more sustainable and cost-effective alternative to conventional anthraquinone process. In alkaline conditions, H2O2 is unstable as HO2 −, and in neutral electrolytes, alkali cation crossover causes system instability. Producing H2O2 in acidic electrolytes ensures enhanced stability and efficiency. However, in acidic conditions, the oxygen reduction reaction mechanism is dominated by the inner-sphere electron transfer pathway, requiring careful consideration of both reaction and mass transfer kinetics. These stringent requirements limit H2O2 production efficiency, typically below 10–20% at industrial-relevant current densities (>300 mA cm−2). Using a multiscale approach that combines active site tuning with macrostructure tuning, this work presents an octahedron-like cobalt structure on interconnected hierarchical porous nanofibers, achieving a faradaic efficiency exceeding 80% at 400 mA cm−2 and stable operation for over 120 h at 100 mA cm−2. At 300 mA cm−2, the optimized catalyst demonstrates a cell potential of 2.14 V, resulting in an energy efficiency of 26%.

High-aspect-ratio cationic nanocellulose self-assembles into mechanically robust nanomesh architectures at oil-water interfaces through charge-directed assembly. The resulting structures feature uniform “breathing holes” (≈34 nm) enabling efficient mass transfer. When applied to oxidative desulfurization, the system achieves >90% thiophene removal under ambient conditions with exceptional catalyst stability through multiple cycles.

Liquid–liquid interfaces present unique opportunities for sustainable biphasic catalysis, yet concurrent amplification of molecular transport and reactivity at these boundaries remains challenging. Here it is demonstrated that high-aspect-ratio cationic nanocellulose (HNC+) spontaneously self-assembles into mechanically robust nanomesh architectures at oil-water interfaces through charge-directed assembly. This assembly is driven by electrostatic attraction between the cationic nanofibers and the intrinsic negative charge at hydrophobic-aqueous interfaces (σ ≈−0.3 C m−2), generating sufficient excess attractive force (ΔU ≈−1,200 kBT) to overcome image charge repulsion. The resulting nanomesh exhibits uniform “breathing holes” (≈34 nm) and exceptional stability under extreme conditions (pH 2–13, 1.8 m NaCl, and 90 °C). When applied to oxidative desulfurization, the system achieves >90% thiophene removal under ambient conditions with exceptional atom economy (E-factor < 1.1) and catalyst stability through multiple cycles. This breakthrough strategy for interfacial engineering using renewable materials opens new possibilities for green chemical manufacturing while providing fundamental insights into charge-mediated assembly at liquid interfaces. These findings establish a viable pathway for sustainable heterogeneous catalysis that aligns with circular economy principles.

This review comprehensively elaborates on functional groups-regulated OSCs that enhance photocatalytic H2O2 production performance, such as cyano, imine, hydroxyl, carboxyl, anthraquinone, sulfonic acid, halogen, etc. Functional groups containing O, N, and S elements contribute to increased charge separation and lower energy barriers for intermediate formation, ultimately enhancing the rate of photocatalytic H2O2 production.

Hydrogen peroxide (H2O2) is an environmentally friendly reagent, and organic semiconductors (OSCs) are ideal photocatalysts for the synthesis of H2O2 due to their well-defined molecular structure, strong donor-acceptor interactions, and efficient charge separation. This review discusses the regulatory mechanisms of functional group modifications in tuning the photocatalytic performance of OSCs, highlighting the relationship between functional group structure and catalytic performance. For example, electron-regulating groups, such as cyano and halogen, induce molecular dipoles, facilitating the migration of photogenerated electrons. Fluorine groups optimize the band structure and prolong carrier lifetime due to their high electronegativity. π-Conjugated extension groups, like anthraquinone and thiophene, expand conjugation, improve visible light capture, and stabilize intermediates through redox cycles. Hydroxyl groups enhance surface hydrophilicity and promote H2O activation, while imine bond protonation adjusts charge distribution and improves selectivity and cycle stability. Multi-active site functional groups, such as sulfonic acid and amide, accelerate reaction kinetics and inhibit H2O2 decomposition. Functional groups enhance light absorption, charge separation, and surface reactions through electronic structure regulation, intermediate adsorption optimization, and proton-electron transfer. Future work should integrate machine learning to identify optimal functional group combinations and develop green functionalization strategies for efficient H2O2 photocatalyst synthesis.

Comprehensive analysis of the existing and prospective sodium-ion battery (SIB) systems unveils that a wider application of SIBs should primarily focus on i) regulating the composition, morphology, surface chemistry, safety performance, and production feasibility of mainstream cathodes, ii) enhancing the high-voltage stability, film formation ability, and cost effectiveness of electrolytes, and iii) reducing irreversible capacity loss and interphase growth of hard carbon anodes based on well-understood sodium-ion storage mechanisms.

Lithium-ion batteries (LIBs) have been widely adopted in the automotive industry, with an annual global production exceeding 1000 GWh. Despite their success, the escalating demand for LIBs has created concerns on supply chain issues related to key elements, such as lithium, cobalt, and nickel. Sodium-ion batteries (SIBs) are emerging as a promising alternative due to the high abundance and low cost of sodium and other raw materials. Nevertheless, the commercialization of SIBs, particularly for grid storage and automotive applications, faces significant hurdles. This perspective article aims to identify the critical challenges in making SIBs viable from both chemical and techno-economic perspectives. First, a brief comparison of the materials chemistry, working mechanisms, and cost between mainstream LIB systems and prospective SIB systems is provided. The intrinsic challenges of SIBs regarding storage stability, capacity utilization, cycle stability, calendar life, and safe operation of cathode, electrolyte, and anode materials are discussed. Furthermore, issues related to the scalability of material production, materials engineering feasibility, and energy-dense electrode design and fabrication are illustrated. Finally, promising pathways are listed and discussed toward achieving high-energy-density, stable, cost-effective SIBs.

Muscles represent one of the toughest anisotropic soft matters. The appealing features originate from their unique aligned fiber-based structures, which form via a combining process involving two major essentials: absorbing nutrients for matrix growth and mechanical training to strengthen the matrix. In this work, a mechanical training-associated growing strategy is proposed to mimic this process for preparing tough anisotropic hydrogels with tunable sizes and enhanced mechanical properties.

Muscles are highly anisotropic, force-bearing issues. They form via a process involving nutrient absorption for matrix growth and mechanical training for matrix toughening, in which cyclic disassembly-reconstruction of muscle fibers plays a critical role in generating strong anisotropic structures. Inspired by this process, a mechanical training-associated growing strategy is developed for preparing tough anisotropic hydrogels. Using anisotropic hydrogels made from polyvinyl alcohol (PVA)/tannic acid (TA) as an example, it is demonstrated that the hydrogels can absorb poly(ethylene glycol) diacrylate (PEGDA) via disassembling their aligned nanofibrillar structures. Incorporation of PEGDA within the hydrogels induces PVA to form crystal domains while subsequent mechanical training can restore the aligned fibrillar structures. Such a combining process results in expansion in materials’ size (≈2 times) and significant enhancement in their mechanical properties (Young's modulus: from 2.4 to 2.85 MPa; ultimate tensile strength: from 8.2 to 14.1 MPa; toughness: from 335 to 465 MJ m−3). With a high energy dissipation efficiency (≈0%), potential applications for these tough and adaptable hydrogels are envisioned in impact-protective materials, surgical sutures, etc.

The charge transfer mechanism and hydrogen evolution reaction photocatalytic reaction mechanism are determined by using transient absorption spectrum, electromagnetic simulation, in situ Raman, and density functional theory theoretical calculation.

Plasmonic metal–semiconductor nanocomposites are promising candidates for considerably enhancing the solar-to-hydrogen conversion efficiency of semiconductor-based photocatalysts across the entire solar spectrum. However, the underlying enhancement mechanism remains unclear, and the overall efficiency is still low. Herein, a hollow C@MoS2-Au@CdS nanocomposite photocatalyst is developed to achieve improved photocatalytic hydrogen evolution reaction (HER) across a broad spectral range. Transient absorption spectroscopy experiments and electromagnetic field simulations demonstrate that compared to the treated sample, the untreated sample exhibits a high density of sulfur vacancies. Consequently, under near-field enhancement, photogenerated electrons from CdS and hot electrons generated by intra-band or inter-band transitions of Au nanoparticles are efficiently transferred to the CdS surface, thus significantly improving the HER activity of CdS. Additionally, in situ, Raman spectroscopy provided spectral evidence of S─H intermediate species on the CdS surface during the HER process, which is verified through isotope experiments. Density functional theory simulations identify sulfur atoms in CdS as the catalytic active sites for HER. These findings enhance the understanding of charge transfer mechanisms and HER pathways, offering valuable insights for the design of plasmonic photocatalysts with enhanced efficiency.

Unbalanced charge carrier injections and high densities of non-radiative recombination channels are still major obstacles to advancing high-efficiency blue perovskite light-emitting diodes (LEDs). Here, a deep-HOMO level p-type small molecule, (2-(3,6-dibromo-9H-carbazol-9-yl)ethyl)phosphonic acid, constructs a better-balanced carrier injection due to improved hole and retarded electron injection by spontaneously centered at the bottom and top surfaces of perovskites films, along with modulation of all defects in bulk and at surface of doped films due to the formation of covalent bonds. With this approach a series of blue perovskite LEDs with external quantum efficiencies of up to 24.03% (485 nm), 16.61% (476 nm), and 8.55% (467 nm) is designed.

Unbalanced charge carrier injections and high densities of non-radiative recombination channels are still major obstacles to advancing high-efficiency blue perovskite light-emitting diodes (LEDs). Here, a deep-HOMO level p-type small molecule, (2-(3,6-dibromo-9H-carbazol-9-yl)ethyl)phosphonic acid, doped in blue perovskites for building a better-balanced injection and controlling over defects is demonstrated. During the perovskite film deposition process, most small molecules are extruded from the precursor solution to the bottom and top surfaces of the perovskite films. This unique distribution of molecules can construct a better-balanced carrier injection due to improved hole and retarded electron injection by its suitable energy-level structure, along with modulation of all defects in bulk and at the surface of doped films due to the formation of covalent bonds by its functional moiety. With this approach, a series of blue perovskite LEDs is designed with external quantum efficiencies (EQEs) of up to 24.03% (at a luminance of 113 cd m−2 and emission peak of 485 nm), 16.61% (at a luminance of 51 cd m−2 and emission peak of 476 nm) and 8.55% (at a luminance of 30 cd m−2 and emission perk of 467 nm), and encouraging operational stability.

a) Schematic of all-silicon photodetectors with in-plane photon trapping structures (IPTS). b) Comparison of peak specific detectivity in IPTS photodetectors with previously reported very long-wavelength infrared photodetectors.

Silicon (Si) photonics has been widely explored for many various applications, including optical communication, optoelectronic computing, spectroscopy, and image sensing. As a key component for optoelectronic signal conversion in these applications, Si-based infrared photodetectors have attracted extensive attention. However, achieving all-Si on-chip photodetection in the very long-wavelength infrared (VLWIR) range remains challenging, with broadband enhancement and improved operating temperature being pressing issues that need to be addressed. An all-Si photodetector design is presented using in-plane photon trapping structures (IPTS) to enhance detection efficiency and improve the operating temperature of the photodetector at the VLWIR range. The photodetector achieves a broadband enhancement of 285–575% (across 12–19 µm) and a 31% reduction in dark current. Additionally, it exhibits an impressive peak specific detectivity of 1.9 × 1010 cm Hz1/2 W−1 at 15 µm, operating at a temperature of 40 K. This study introduces a novel all-Si optoelectronic device architecture that offers a promising solution for improving the operating temperature and sensitivity of broadband VLWIR devices, making the whole system more compact and cost-effective.

An in-liquid superspreading space-confined epitaxy approach is proposed to fabricate Pt (II) complexes crystalline films on superamphiphilic surface. By regulation of the diffusion process, precise control over the nucleation and crystal growth is achieved, resulting in the formation of planar crystalline films. These films exhibit multi-signal sensing ability, making them suitable for reaffirmed sensing detector in complex and unstable conditions.

Solution-based method is regarded as a promising approach to fabricate large-area, high-quality crystalline films, owing to its low-cost manufacturing and facile features. However, traditional solution-based methods still suffer from random simultaneous nucleation and uncontrollable crystal growth which result in polycrystalline films and coffee-ring effect. Herein, it is proposed that an in-liquid superspreading space-confined epitaxy approach on a superamphiphilic surface to fabricate crystalline films with controllable initial nucleation and crystal morphology. With delicate control of the liquid environment, concentration, and superspreading space-confined solvent film thickness, planar crystalline films with high crystallinity and smooth morphology are obtained. A controllable dewetting crystallization mechanism is proposed, indicating that the diffusion coefficient, regulated by liquid environment, can control the dewetting process during crystallization. With the balance of solvent diffusion and solute precipitation in crystallization, the ordered in-plane and out-of-plane molecular stacking is achieved. And the as-prepared planar Pt(II) complex crystalline film exhibits multi-signal sensing ability, which can be further used to fabricate the reaffirmed sensing detector for precise gas sensing in complex and unstable conditions. This study demonstrates a facile approach for crystalline film fabrication with controllable nucleation and morphology in a liquid environment, which holds promising applications in the construction of oxygen or water-sensitive organic/inorganic devices.

This study employs multi-objective kernel-based Bayesian optimization to efficiently screen ionic polymer electrolytes (IPEs) for high-voltage, fast-charging lithium metal batteries (LMBs). By examining just 2.8% of the complex chemical space, it achieves multi-objective optimization for ionic conductivity, electrochemical stability, and capacity in IPEs. These findings highlight the pivotal role of machine learning in expediting material discovery for advanced batteries.

Designing ionic polymer electrolytes (IPEs) for high-voltage and fast-charging lithium batteries involves searching in a highly complex and discrete chemical space. Traditional material discovery processes struggle with this complexity due to high costs and long evaluation time. A kernel-based Bayesian optimization is described to complete the multi-objective optimization by considering ionic conductivity, electrochemical stability, and discharge capacity simultaneously. According to a recommender based on a union set of acquisition functions, promising IPEs through three iterations with only 2.8% of the chemical space is targeted. The achieved lithium metal batteries exhibit promising performance with ultrahigh cutoff voltage with NCM811 (LiNi0.8Co0.1Mn0.1O2, 4.8 V) and LNMO (LiNi0.5Mn1.5O4, 4.92 V). To further extend the versatility of IPEs and diminish the high cost associated with the glove-box environment, an aqueous and high-voltage lithium-ion battery is developed by introducing water molecules in IPEs coupled with Li4Ti5O12||LiMn2O4, a strong hydrogen bonding network formed between the rigid-rod polyelectrolyte and the embedded water molecules, which effectively suppresses the water reactivity, meanwhile boosting the ionic conductivity. This work reveals an innovative multi-objective optimization that effectively handles multi-targets and discontinuous parameter space, offering critical insights to address complex challenges in material discovery and property optimization for advanced and versatile lithium batteries.

POctS is an innovative, simple to prepare mRNA delivery carrier that has both high mRNA delivery efficiency and stimulator of interferon genes (STING)-stimulating function. More importantly, the unique site-specific delivery ability of POctS achieves mRNA expression in specific sites and the exertion of STING-stimulating function in specific sites, resulting in minimization of formulation toxicity and maximization of mRNA vaccine efficacy.

The development of mRNA delivery carriers with innate immune stimulation functions has emerged as a focal point in the field of mRNA vaccines. Nonetheless, the expression of mRNA in specific sites and innate immune stimulation at specific sites are prerequisites for ensuring the safety of mRNA vaccines. Based on the synthetic PEIRs carriers library, this study identifies an innovative mRNA delivery carrier named POctS with the following characteristics: 1) simultaneously possessing high mRNA delivery efficiency and stimulator of interferon genes (STING) stimulation function. 2) Leveraging the distinctive site-specific delivery capabilities of POctS, the expression of mRNA at specific sites and the activation of innate immune responses at designated sites are achieved, minimizing formulation toxicity and maximizing the vaccine performance. 3) Tailoring two types of mRNA vaccines based on POctS according to the immune infiltration status of different types of tumors. Briefly, POctS-loading ovalbumin (OVA) mRNA as a tumor antigen vaccine achieves the prevention and treatment of melanoma in mice. Further, POctS-loading mixed lineage kinase domain-like protein (MLKL) mRNA as an in situ tumor vaccine effectively treats orthotopic pancreatic cancer in mice. This delivery carrier offers a feasible mRNA vaccine-based immunotherapy strategy for various types of tumors.

Orbital angular momentum (OAM) generated via interfacial orbital Rashba–Edelstein effect is demonstrated to significantly enhance the SOT efficiency in metallic antiferromagnet IrMn-based heterostructures. The SOT efficiency variation with IrMn thickness reveals the orbital current transportation and conversion process in IrMn. The OAM contribution is verified by the critical current density decreasing of SOT-driven magnetization switching.

Current-induced spin-orbit torque (SOT) allows efficient electrical manipulation on magnetization in spintronic devices. Maximizing the SOT efficiency is a key goal that is pursued via increasing the net spin generation and accumulation. However, spin transport in antiferromagnets is seriously restricted due to the strong antiferromagnetic coupling, which blocks the development of antiferromagnetic-based devices. Here, a significant enhancement of SOT efficiency in Ir20Mn80 (IrMn)-based heterostructure associated with the orbital effect of naturally oxidized Cu (Cu*) bottom layer is reported. Considering the weak spin–orbit coupling of Cu*, the enhancement results from an orbital current generated from charge current at the Cu*/IrMn interface that contributes to spin current in the IrMn layer due to the strong spin–orbit coupling. The SOT efficiency variation with IrMn thickness reveals the process of orbital angular momentum (OAM) transportation and conversion. Moreover, the contribution of orbital current is verified by the critical current density decreasing of SOT-driven magnetization switching in Cu*/IrMn/[Co/Pt]3 heterostructure. This study opens a path to design high-efficient SOT-based spintronic devices combining the advantages of OAM and metallic antiferromagnets.