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

In this work, a 3D superionic transport skeleton Na3P is in situ constructed within the sodium anode, which successfully enhances the ion diffusion coefficient of the anode from 2.54 × 10‒8 to 1.33 × 10‒7 cm2 s‒1. Thanks to the ultrafast ion transport and excellent interfacial stability, the solid-state sodium-metal battery can be stably cycled for more than 15 000-cycle at 3C.

Solid-state sodium-metal batteries (SSSMBs) have emerged as a promising candidate for next-generation energy storage systems due to their natural abundance, cost-effectiveness, and high safety. However, the intrinsically low ionic conductivity of sodium anode (SA) and poor wettability to solid-state electrolyte (SSE) severely hinder the development of SSSMBs. In this study, a 3D superionic transport skeleton Na3P is in situ constructed within the sodium anode by simply melting inexpensive and low-density red phosphorus with sodium, which successfully enhances the ion diffusion rate from 2.54 × 10‒8 to 1.33 × 10‒7 cm2 s‒1. Moreover, Na3P in the composite sodium anode (CSA) effectively induces the uniform deposition of Na on the surface of SSE, significantly reducing the interface impedance of symmetric cells from the initial value of 749.15 to 14.97 Ω cm2. Enabled by the integrated 3D superionic transport skeleton, the symmetric cell achieves exceptional cycle stability of over 7000 h at 0.1 mA cm‒2 and 4000 h at 0.3 mA cm‒2. Furthermore, SSSMBs incorporating CSA demonstrate an ultralong lifespan of over 15 000 cycles at 3C while maintaining a high-loading operation capability, significantly outperforming previously reported studies. This study highlights the crucial role of cost-effective CSA design with enhanced ion transport in advancing high-performance SSSMBs.

The interface in printable mesoscopic perovskite solar cells is regulated via the flexible molecule of dodecaethylene glycol (DEG) with abundant polar oxygen atoms. The regulation modulated the wetting sequence of the scaffold, promoted perovskite crystallization in the scaffold, and relaxed interface stress. The device with interface regulation successfully achieved an improved power conversion efficiency of 20.27% and demonstrated good stability.

Perovskite solar cells have achieved remarkable progress in photovoltaic performance, driven by advancements in interface engineering. The buried interface between the electron transport layer and the perovskite layer is particularly critical, as it governs both perovskite crystallization and the formation of residual strain. In this study, the buried interface in printable mesoscopic perovskite solar cells (p-MPSCs) based on a triple-mesoporous scaffold of TiO2/ZrO2/carbon is reconstructed by employing dodecaethylene glycol (DEG), a long chain molecule rich in polar oxygen atoms, to enhance device performance. Treating the scaffold with DEG optimizes the wettability sequence across the three layers by improving the TiO2 surface's wettability, facilitating the preferential crystallization of perovskite in the underlying TiO2 layer. Moreover, the DEG layer effectively buffers residual strain and suppresses detrimental defects at the interface. As a result, p-MPSCs with the optimized interface achieve a power conversion efficiency (PCE) of 20.27% and retain over 92% of their initial PCE after 500 h of continuous operation under maximum power point tracking.

This study reports an effective strategy, OSPLIT (optothermal-stimulated persistent luminescence imaging and therapy), which enables high-contrast imaging and the thermal ablation of lymph node metastases. The rational design of these nanomaterials is detailed and mechanistic insights are provided, demonstrating the advantages of optothermal-stimulated NIR-II persistent luminescence in lanthanide-doped nanoparticles over conventional NIR-II fluorescence imaging.

Persistent luminescent nanomaterials have significantly advanced in vivo bioimaging and biosensing by emitting photons after excitation ceases, effectively minimizing tissue autofluorescence. However, their application in biomedical fields such as tumor theranostics is limited by low brightness and rapid signal decay. To address these issues, OSPLIT (optothermal-stimulated persistent luminescence imaging therapy), a dual-function strategy for imaging and treatment is introduced. The OSPLIT approach enhances the release of charge carriers from deep traps in lanthanide-doped nanoparticles, resulting in a 73 fold increase in persistent luminescence within the second near-infrared (NIR-II) window. In living mice, it enables high-contrast imaging of lymph node metastases, with a signal-to-background ratio 11.8 times greater than conventional NIR-II fluorescence. Optothermal-boosted nanoparticles are effective in ablating lymph node metastasis and preventing tumor spread. These findings highlight the potential of optothermal stimulation to enhance persistent luminescence for both imaging and therapeutic applications.

A novel method for detecting cancer cells and monitoring apoptosis employs electron-sink-enhanced surface-enhanced Raman scattering (SERS). Gold (Au) shells coated with electroactive liposome membranes amplify the SERS signal through active electron transfer. This technique enables real-time and highly sensitive detection of cancer cells by measuring apoptosis-associated electron flow, offering a powerful approach for distinguishing cancerous from normal cells.

A novel method is presented for detecting cancer cells and assessing apoptosis using electron-sink-enhanced surface-enhanced Raman scattering (SERS) via active electron transfer. By coating gold (Au) shells with electroactive liposome membranes (ELMs) derived from Shewanella oneidensis MR-1, the SERS signal is enhanced through chemical mechanism (CM) enhancement driven by electron transfer. The ELMs first donate electrons to the Au shells, which, upon laser excitation, amplify the local electromagnetic field, resulting in stronger Raman signals from the attached probing molecules. Additionally, the electron flow from cancer cells into the Au shells correlates with apoptosis, producing a strong SERS signal, while normal cells exhibit weaker signals. This method enables real-time monitoring of cancer cell apoptosis, distinguishing cancer cells from normal cells based on the enhanced Raman signal linked to electron flow. This approach marks a breakthrough in CM-based SERS applications, offering a sensitive method for cancer detection through the measurement of electron flow.

Isomeric graphdiyne frameworks with ThSi2 topology are synthesized from 2,2′-binaphthalene and 6,6′-biazulene-based isomeric monomers. The biazulene-based graphdiyne framework shows narrow bandgap of down to 1.15 eV and can act as new platform for loading single metal atoms for high-performance electrocatalysis.

Graphdiynes (GDYs), synthesized via direct coupling of arylacetylenes, have attracted great attention due to their unique electronic properties and structural diversity, typically forming 2D layered frameworks. However, crystalline GDY-like frameworks with 3D topology remain challenging to synthesize. Here, the study reports two highly crystalline, isomeric GDY-like frameworks with ThSi2 topology, constructed from 2,2′-binaphthalene and 6,6′-biazulene-based monomers. The azulene-based framework, due to its large dipole moment, exhibits a narrow bandgap of 1.15 eV, significantly lower than its naphthalene counterpart (2.33 eV). As ruthenium (Ru) single-atom supports, these frameworks enable strong Ru-diyne interactions, achieving an ammonia yield rate of 188.7 ± 1.6 µg h−1 mgcat −1 and a Faradaic efficiency of 37.4 ± 0.6%. Such bicontinuous channels and tunable electronic structures offer electrocatalysis field new opportunities. Moreover, the azulene-based framework, featuring a higher highest occupied molecular orbital  and lower lowest unoccupied molecular orbital  energy level, ensures superior electron mobility. These 3D crystalline frameworks introduce a new covalent organic framework (COF) family with diyne linkages and pure carbon skeletons, broadening the scope of COF materials. Their well-defined structures provide an ideal platform for tuning optoelectronic properties, enabling fundamental studies on structure-property relationships and opening new opportunities for catalytic and electronic applications.

Diabetic wound repair remains hindered by persistent inflammation, infection risks, and microenvironment dysregulation. Electromagnetic biomaterials offer transformative solutions for intelligent wound monitoring and pathological microenvironment modulation. This review summarizes the advantages, biological mechanisms, and application strategies of electromagnetic biomaterials in diabetic tissue repair, focusing on skin and bone regeneration, and highlighting their potential to enhance clinical outcomes.

The diabetic tissue repair process is frequently hindered by persistent inflammation, infection risks, and a compromised tissue microenvironment, which lead to delayed wound healing and significantly impact the quality of life for diabetic patients. Electromagnetic biomaterials offer a promising solution by enabling the intelligent detection of diabetic wounds through electric and magnetic effects, while simultaneously improving the pathological microenvironment by reducing oxidative stress, modulating immune responses, and exhibiting antibacterial action. Additionally, these materials inherently promote tissue regeneration by regulating cellular behavior and facilitating vascular and neural repair. Compared to traditional biomaterials, electromagnetic biomaterials provide advantages such as noninvasiveness, deep tissue penetration, intelligent responsiveness, and multi-stimuli synergy, demonstrating significant potential to overcome the challenges of diabetic tissue repair. This review comprehensively examines the superiority of electromagnetic biomaterials in diabetic tissue repair, elucidates the underlying biological mechanisms, and discusses specific design strategies and applications tailored to the pathological characteristics of diabetic wounds, with a focus on skin wound healing and bone defect repair. By addressing current limitations and pursuing multi-faceted strategies, electromagnetic biomaterials hold significant potential to improve clinical outcomes and enhance the quality of life for diabetic patients.

In this study, AGEs derived is found from glycated ECM significantly promote tumor growth and VM formation through the RAGE-HMGB1-SNAI2 axis. However, carbon dots (egCDs) derived from glycated ECM can competitively bind to RAGE, promoting its lysosomal degradation and inhibiting this process. This finding reveals the transformation of pathogenic substances into therapeutic targeting carriers after carbonization, reversing disease-driving factors.

This study investigates the role of advanced glycation end-products (AGEs) in tumor vasculogenic mimicry (VM). Using high-sugar diet animal models and glycated extracellular matrix (ECM) ex vivo models, AGEs derived is demonstrated from glycated ECM significantly enhanced tumor growth and VM formation. However, carbon dots (egCDs) derived from glycated ECM effectively inhibit tumor growth and VM formation in this glycated microenvironment. Mechanistic studies show that AGEs from glycated ECM bind to the Receptor of Advanced Glycation Endproducts (RAGE) receptors on tumor cells, promoting RAGE nuclear translocation and binding with high mobility group box 1 (HMGB1), which increases the transcription of Snail family transcriptional repressor 2 (SNAI2), thereby driving VM formation. However, egCDs competitively bind to RAGE, promoting its lysosomal degradation and blocking VM formation induced by the RAGE-HMGB1-SNAI2 axis. In conclusion, this study demonstrates that egCDs can target RAGE and promote its lysosomal degradation to block VM formation induced by glycated ECM. This finding not only reveals the transformation of glycated ECM from a pro-VM factor to an anti-VM therapeutic agent after carbonization, but also provides a theoretical basis for the innovative strategy of “reconstructing pathogenic substances into carbon dots to reverse disease-driving factors into therapeutic targeting carriers”.

A nacre-mimetic ceramic-polymer structural material is developed by a dual-oxide interface design strategy, achieving high mechanical properties, tunable colors and superior EM wave-transparent performance. These characteristics make it hold great potential as a protective material for radar and communication equipment.

Ceramic materials are widely used in various protective equipment owing to their excellent mechanical properties and chemical stability, while their applications are limited by monotonous color and poor toughness. Inspired by the colorful and tough natural shells, nacre-mimetic alumina (Al2O3)-based (NMA) composites are fabricated by proposing a dual-oxide interface design strategy inspired by the hierarchical structure of natural nacre. The NMA composites achieve color regulation, providing possibilities for their application in camouflage protective armor. The fracture toughness of the optimal NMA composite is more than three times that of commercial Al2O3 ceramic. Simultaneously, the NMA composites have obvious advantages in terms of impact resistance compared with Al2O3 ceramic and polymer polymethyl methacrylate (PMMA). Additionally, the hierarchical structure of the NMA composites provides favorable structural conditions for transmission of electromagnetic (EM) waves at the frequency band of 18–26.5 GHz. These characteristics make the NMA composites potential protective materials for radar and communication equipment.

A modified chemical vapor transport method incorporating a feedback-regulated strategy provides closed-loop control of the growth temperature of MnBi2nTe3n+1 family within ± 0.1 °C, which reveals rich magnetic tunability, such as varying antiferromagnetic coupling in MnBi2Te4 and inducing magnetic ground state transitions from antiferromagnetism to ferromagnetism in MnBi4Te7 and MnBi6Te10.

MnBi2nTe3n+1 is a representative family of intrinsic magnetic topological insulators, in which numerous exotic phenomena such as the quantum anomalous Hall effect are expected. The high-quality crystal growth and magnetism manipulation are the most essential processes. Here a modified chemical vapor transport method using a feedback-regulated strategy is developed, which provides the closed-loop control of growth temperature within ± 0.1 °C. Single crystals of MnBi2Te4, MnBi4Te7, and MnBi6Te10 are obtained under different temperature intervals respectively, and show variable tunability on magnetism by finely tuning the growth temperatures. Specifically, the cold-end temperatures not only vary the strength of antiferromagnetic coupling in MnBi2Te4, but also induce magnetic ground state transitions from antiferromagnetism to ferromagnetism in MnBi4Te7 and MnBi6Te10. In MnBi2Te4 with optimized magnetism, quantized transport with Chern insulator state can be easily replicated. These results provide a systematic picture for the crystal growth and the rich magnetic tunability of MnBi2nTe3n+1 family, providing richer platforms for the related researches combining magnetism and topological physics.

Robust 2D Ruddlesden–Popper lead-tin perovskites demonstrate exceptional resistive switching memory performance after cesium carbonate deposition, achieving a high accuracy of 90.1% in MNIST pattern recognition. Additionally, a novel energy-efficient content-addressable memory architecture, based on perovskite memristive devices, is proposed for neuromorphic applications, demonstrating ultralow energy consumption of ≈0.025 fJ bit−1 per cell.

Metal halide perovskites have drawn great attention for neuromorphic electronic devices in recent years, however, the toxicity of lead as well as the variability and energy consumption of operational devices still pose great challenges for further consideration of this material in neuromorphic computing applications. Here, a 2D Ruddlesden-Popper (RP) metal halides system of formulation BA2Pb0.5Sn0.5I4 (BA = n-butylammonium) is prepared that exhibits outstanding resistive switching memory performance after cesium carbonate (Cs2CO3) deposition. In particular, the device exhibits excellent switching characteristics (endurance of 5 × 105 cycles, ON/OFF ratio ≈105) and achieves 90.1% accuracy on the MNIST dataset. More importantly, a novel energy-efficient content addressable memory (CAM) architecture building on perovskite memristive devices for neuromorphic applications, called nCAM, is proposed, which has a minimum energy consumption of ≈0.025 fJ bit/cell. A mechanism involving the manipulation of trapping states through Cs2CO3 deposition is proposed to explain the resistive switching behavior of the memristive device.

Post-synthesis surface engineering and doping control significantly improve the performance of Ag₂Te CQD photodiodes, achieving a low dark current of 450 nA cm− 2 at −0.5 V, an LDR exceeding 150 dB, and a rapid response speed of ≈25 ns. A proof-of-concept LiDAR demonstration in the SWIR using a nanosecond diode laser, achieves decimetre-level resolution at a distance exceeding 10 m, paving the way in advancing SWIR CQDs toward consumer electronics and automotive markets.

Shortwave infrared (SWIR) light, characterized as the “eye-safe” window, is considered extremely promising in various technological fields and particularly valuable for imaging and light detection and ranging (LiDAR) applications. Silver telluride (Ag2Te) colloidal quantum dots (CQDs), featuring RoHS-compliance, solution-processability, and CMOS compatibility, emerge as a potential contender for SWIR optoelectronics. Yet, further improvements in dark current, response speed, and linear dynamic range (LDR) are essential for meeting the rigorous demands of sensing and LiDAR applications. Here, it is shown that post-synthesis surface engineering and doping control significantly improve the dark current, response speed, and LDR of Ag₂Te CQD photodiodes, achieving a low dark current of 450 nA cm− 2 at −0.5 V, an LDR exceeding 150 dB, and a rapid response speed of ≈25 ns. A proof-of-concept LiDAR demonstration in the SWIR using a practical nanosecond diode laser achieves decimetre-level resolution at a distance exceeding 10 m. This work represents a key step in advancing SWIR CQDs toward consumer electronics and automotive markets.

The incorporation of hydroxyl groups (─OH) as a proton reservoir into the covalent organic framework (COF) can compensate oxygen reduction reaction (ORR), and achieve a 3.3 times higher H2O2 photosynthetic activity than that of COF without ─OH, which elucidates the favorability mechanisms of regulating the internal proton transfer of COF with proton reservoir in the accelerated ORR progress.

The water oxidation reaction (WOR) with sluggish kinetics usually fails to adequately furnish protons to oxygen reduction reaction (ORR), which ultimately constrains the overall efficiency of photocatalytic synthesis of H2O2, particularly in the absence of sacrificial agents. Herein, a class of hydroxyl groups (─OH) functionalized covalent organic framework (COF) is reported as a proton reservoir to compensate ORR for greatly improving the efficiency of H2O2 photosynthesis. It has been demonstrated that the incorporation of ─OH into the TFBP-DHBD (TFBP: 1,2,4,5-tetrakis-(4-formylphenyl)benzene, DHBD: 3,3′-dihydroxybenzidine) COF can achieve a 3.3 times higher H2O2 photosynthetic activity than that of TFBP-BD (BD: benzidine) COF without ─OH groups. Isotope labeling experiments and in situ infrared spectroscopy analysis demonstrate that the proton reservoir can donate protons for ORR and subsequently regain the released protons from WOR. Theoretical calculations further confirm that the ─OH functionalized COF provides the protons for the formation of *OOH intermediate and reduces its energy barrier, thereby facilitating the photosynthesis of H2O2. A novel COF loaded with Al2O3 spheres-based streamlined microreactor is built that can simultaneously achieve production of H2O2 and elimination of bacteria over 1.3 × 104 CFU mL−1, superior to the reported continuous flow photocatalytic reactors.

In this work, a novel design strategy is proposed by strengthening the van der Waals forces in the nanostructure of DESs, which significantly enhances the reducibility of DESs components. Benefiting from this, the leaching kinetics of metals is greatly improved, resulting in an excellent leaching performance that far exceeds previous reports.

Promoting the green and efficient recycling of critical metals in spent ternary batteries represents a crucial step in driving the reduce of resource dependence in the electric vehicle industry. However, the leaching progress of metals from spent cathodes generally requires high reaction temperatures and large usage of solvents. Herein, a strategy is proposed to strengthen the van der Waals forces between solvent components by constructing affinity interactions between functional groups (e.g., -OH and -COOH), which can significantly enhance the leaching kinetics of metals at a high solid-liquid ratio and low temperature (30 °C). The results demonstrate that the strong van der Waals force between ascorbic acid with -OH group and betaine ions with -COOH group can strengthen the nucleophilicity of the carbon atoms and reduce the specific C─C bond energy, thus enhancing the redox capability of the DESs. Encouragingly, the designed solvent shows an impressive leaching performance at a super high S/L ratio (1: 3) without external heating for the actual black mass under a scaled-up experiment.

Metal–organic frameworks (MOFs) possessing coordinately unsaturated Zr4+ sites are exploited as a new material library of electrode additives for lithium-ion batteries (LIBs), which simultaneously boost lithium-ion conduction within electrodes and deliver step-change electrochemical performances. Such a cost-effectiveness MOF additive approach illuminates a new avenue toward advancing industry-relevant LIBs.

Performances of lithium-ion batteries (LIBs) are dictated by processes of electron-ion separation, transfers, and combination. While carbon additives are routinely used to ensure electronic conductivity, additives capable of simultaneously boosting ion conduction and delivering step-change performance remain elusive. Herein, metal–organic frameworks (MOFs) possessing coordinately unsaturated Zr4+ sites are exploited as a new material library of electrode additives. The MOFs imbue infused electrolytes with an expanded electrochemical stability window (0 to 5 V vs Li/Li⁺) and enhanced Li⁺ transport efficiency. Mechanistically, strong interactions between Zr4+ sites and Li+ solvation sheaths result in trimmed, anion-fixed, and solvent-separated ion pairs, mitigating electrostatic coupling and enabling efficient Li⁺ translocation in the porous nanospace. Concomitantly, these solvation structural modulations foster interfacial and electrochemical stabilities. When implemented at 1.7 wt.% in graphite and sub-Ah full cell, the MOF additives significantly improved Li+ diffusional kinetic, rate capability beyond 2C, and cycling longevity doubling lifespan. This work offers a straightforward yet effective route to remedy the bottlenecks of industrial LIBs.

A facile and scalable dual-solvent strategy is developed to fabricate dendritic ZIF-67-D with tailored preferred facet and coordination environments. The reduced Co coordination number and enhanced electron-donating capability lead to significantly improved performance in triboelectric nanogenerators (TENGs) and electrocatalysis, highlighting the multifunctional potential of ZIF-67-D.

Metal-organic frameworks (MOFs) are highly versatile materials with tunable chemical and structural properties, making them promising for triboelectric nanogenerators (TENGs) and electrocatalysis. However, achieving precise control over MOF coordination structures to optimize facet-dependent properties remains challenging. Here, a facile and scalable dual-solvent synthesis strategy is presented to fabricate dendrite Co-2-methylimidazole MOF (ZIF-67-D), enabling tailored preferred facet and coordination environments. Using density functional theory (DFT) calculations and synchrotron-based X-ray absorption spectroscopy, it is demonstrated that ZIF-67-D, enriched with (112) facets, features a reduced Co coordination number and enhanced electron-donating ability compared to the conventionally (011) facet-dominated rhombic dodecahedron ZIF-67 (ZIF-67-R). This facet engineering boosts TENG charge density by 2.4-fold, OER current density by 9.9-fold (@1.65 V), and HER current density by 1.9-fold (@-0.3 V). The (112)/(011) facet ratio can be also tuned to precisely alter TENG output. Moreover, the optimized ZIF-67-D shows excellent stability, maintaining electrolyzer performance for 72 h and enabling TENG devices even in high humidity. Consequently, ZIF-67-D-based TENG (D-TENG) devices exhibit robust energy generation and power ZIF-67-D||ZIF-67-D electrolyzers for continuous hydrogen (H2) production. These findings introduce a new paradigm for converting mechanical energy into sustainable chemical energy, offering insights into facet engineering for high-performance energy harvesting systems.

A novel 3D template-catalyzed growth (3D-TCG) method is developed for kilogram-scale production of few-layered 2D nanosheet powders with high efficiency. The template-catalyzed growth mechanism of this approach enables the high-quality and controllable lateral sizes from 100 nm to 10 µm of the products, demonstrating promising viability for large-scale practical applications.

Bulk availability of 2D material powders presents broad opportunities for various industrial applications. Particle size and morphology control are critical factors that govern their properties, and in particular, large-scale size-controlled production of 2D materials nanosheets remains extremely challenging. Herein, a novel 3D template-catalyzed growth (3D-TCG) method is demonstrated that allows the mass production of size-tunable 2D hexagonal boron nitride (h-BN) nanosheet powders, a key material in the 2D materials family. Rather than limiting the nanosheet growth on 2D substrate surfaces, this method provides large numbers of active sites distributed in 3D space, leading to the feasibility of scale-up production with excellent product homogeneity and high efficiency. Ultrathin h-BN nanosheets are synthesized with high throughput (kilogram quantities) and lateral sizes that can be tuned from 100 nm to 10 µm with thicknesses of few layers. Their practical application is demonstrated in lithium metal batteries, where the obtained nanosheet powders are processed and roll-to-roll coated on commercial separators (>10 m2). The prototype pouch cell delivers high energy density (501.8 Wh kg−1) and improved cycling stability. The template-based large-scale production strategy can be used to generically produce various types of bulk pristine 2D nanopowders with potential for many large-scale applications.

Selective C-H activation is a crucial step in organic molecule transformation. Photocatalytic radicals-driven C-H activation is considered a promising approach but suffers from simultaneously utilizing electron/hole pairs which are limited to broad-band gap semiconductors. A half-photocathodic reaction strategy is reported for the selective oxidation of toluene to benzaldehyde using a narrow-bandgap porous CuBi2O4 photocathode. The intrinsic Cu+/Cu2+ redox of porous CuBi2O4 catalyzes the photocathodic oxygen reduction, generating H2O2-derived ·OH radicals that activate the C(sp3)-H bond, followed by ·O2 --mediated oxidation to yield benzaldehyde.

Selective C-H activation is the most important step for organic molecule transformation. Photocatalytic radicals driven C-H activation is considered a promising route but suffers from simultaneously utilizing electron/hole pairs which are limited to broad-band gap semiconductors. Herein, a half-photocathodic reaction strategy is demonstrated to activate and oxygenate C(sp3)-H bonds of toluene toward selective benzaldehyde production using a narrow-bandgap CuBi2O4 (CBO) porous photocathode. The intrinsic Cu+/Cu2+ redox of porous CBO photocathode catalyzes the photocathodic oxygen reductive H2O2 to generate ·OH capable of oxidation which activates the C(sp3)-H bond that is further oxygenated via ·O2 − formed of the photocathodic oxygen reduction. As a result, the benzaldehyde selectivity is up to 90%. Impressively, the narrow-band gap of CBO enables record-high light-driven benzaldehyde yields of 111.93 mmol m−2 h−1 with stability of over 20 h. This work opens a green and efficient light-driven C(sp3)-H bond oxidation strategy by using a narrow-bandgap photocathode.

An electron-rich ɛ-Keggin cluster CuMo16 is synthesized and can act as an active material is introduced into a hydrogel system for intelligent electronics. Molecular dynamics simulations reveal that integrating CuMo16 significantly enhances the intelligent storage performance of flexible electronics, and molecular regulation of CuMo16 content provides an effective strategy for optimizing flexible electronic devices.

The fabrication of molecular cluster-based intelligent energy storage systems remains a significant challenge due to the intricacies of multifunctional integration at the molecular level. In this work, low-valent metal atoms are successfully encapsulated within ɛ-type Keggin structures, yielding a novel cluster denoted as CuMo16 . This unique structure displayed the characteristic “molybdenum red” coloration, with a high degree of reduction (76.47%), which played a pivotal role in enhancing its electrochemical properties. The specialized configuration significantly enhanced multi-proton-coupled electron transfer kinetics, enabling efficient and rapid electron storage and release, with up to thirteen electrons per molecule. To construct an intelligent energy storage device, CuMo16 is employed as a proton-coupled electron-active material and embedded within a polyvinyl alcohol (PVA) matrix, resulting in the flexible, wearable, rechargeable devices. The flexible electronics not only demonstrate real-time human motion detection but also exhibit remarkable energy storage performance, reaching a peak capacity of 194.19 mAh g−1 and maintaining 68.2% capacity retention after 2500 cycles. Molecular dynamics simulations reveal that integrating CuMo16 significantly enhances the intelligent storage performance of flexible electronics, and molecular regulation of CuMo16 content provides an effective strategy for optimizing flexible electronic devices. This study lays the foundation for the development of cluster-based intelligent energy storage systems.

This work introduces a salt-segregation strategy for solid polymer electrolytes, which decouples surface and bulk salt distribution to form an ion-enriched surface layer. The design dramatically enhances the lithium deposition kinetics and suppresses parasitic reactions, empowering Li||LiFePO4 solid-state batteries with exceptional cycling over 20 000 cycles at high-rate of 1.12 A g−1.

Solid-polymer electrolytes (SPEs) demonstrate great potential for solid-state lithium batteries (SSLBs), however, interfacial instability and sluggish ion transport at the interface critically hinder their high-rate capability and long-term stability. Here, a novel salt-segregation methodology with spatial salt grade for SPEs is introduced. This approach leverages the differential solubility of lithium salts and PVDF matrix in a commercially available fluoroethylene carbonate during fabrication, which drives the formation of an ion-enriched surface layer. The strategy simultaneously enhances interfacial and bulk ionic conductivity while effectively mitigating parasitic reactions. These advancements optimize Li+ flux at the lithium metal interphase, promoting a spherical Li growth with minimized surface area and leading to dense lithium deposition. Consequently, the engineered SPE achieves a remarkable cycling of 500 h in Li||Li cells at 2 mA cm−2. Solid-state Li||LiFePO4 cells exhibit a record stability for 20 000 cycles at 1.12 A g−1 (2 mg cm−2 LiFePO4 cathode), and a high capacity of 147 mAh g−1 over 300 cycles at 0.84 mA cm−2 under a high-loading 2 mAh cm−2 cathode. The strategy addresses interfacial limitations in SPEs and further introduces a paradigm shift by emphasizing the critical role of spatial salt-graded engineering at the surface over uniform ion distribution for stabilizing high-rate SSLBs.

A novel dual-modification approach, ─NH₂ groups modification and Cu ions coordination, is first imposed on MIL-125, which greatly improved carrier separation due to the enhanced piezoelectricity of MOFs caused by polarity alteration, leading to exceptional high piezo-photocatalytic hydrogen production.

Metal–organic frameworks (MOFs) face significant challenges in photocatalysis due to severe carrier recombination. Here, a novel approach is presented that incorporates ─NH2 groups and Cu ions onto MOFs with a MIL-125 skeleton, forming NH2-MIL-125 and Cu-NH2-MIL-125. This modification effectively enhances the polarity of MOFs, evidenced by significantly increased d33 values (from 1.69 to 26.21 pm/V) and notable higher dipole moments (from 6.60 to 25.99 D). Notably, it's the first demonstration of boosting MOFs piezoelectricity via a dual modulation strategy. Moreover, the polarity can be further amplified by ultrasonic vibration based on the positive piezoelectric effect, which is justified by in situ Raman spectra, COMSOL simulations, and DFT calculations, by taking into account the applied pressure. The positive impact of introduced piezoelectric effect in facilitating charge separation and transfer of Cu-NH2-MIL-125, proved by enhanced current response. Consequently, through coupling piezocatalysis and photocatalysis, the H2 production rate of Cu-NH2-MIL-125 can be significantly enhanced to ≈2884.2 µmol·g−1·h−1, 2.76 and 9.92 times higher than that of NH2-MIL-125 and MIL-125, respectively, ranking first in all reported MOF-based piezo-photocatalysts. This research demonstrates the prospective opportunity for alleviating the severe carriers recombination problem for MOFs through the implantation of piezoelectric field driving force.