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

The dual delivery system employing extracellular vesicles to mediate the co-delivery of mRNA and nanozymes exhibits synergistic effects on endoplasmic reticulum stress, mitochondrial injury, and their functional crosstalk. This system is capable of regulating microglia function from many aspects, including inhibiting NF-κB signaling pathway, inhibiting microglia overactivation, and promoting microglia M2 polarization, and ultimately ameliorates depressive behaviors.

The development of new non-neurotransmitter drugs is an important supplement to the clinical treatment of major depressive disorder. The latest development of mRNA therapy provides the possibility for the treatment of some major diseases. The endoplasmic reticulum (ER) and mitochondria constitute a highly interconnected set of fundamental organelles within cells. The interconnection between them forms specific microdomains that play pivotal roles in calcium signaling, mitochondrial dynamics, inflammation, and autophagy. Perturbations in ER-mitochondrial connections may contribute to the progression of neurological disorders and other diseases. Herein, an extracellular vesicles-based delivery system, grounded in mRNA gene therapy and integrated with nanomedicine technology is devised. This system is engineered to traverse the blood–brain barrier and specifically target the central nervous system (CNS), facilitating the simultaneous delivery of mRNA drugs and metallic nanozymes into the brain. This dual-pronged approach, targeting ER and mitochondrial crosstalk, inhibits microglial overactivation, promotes M2 polarization of microglia, and suppresses the NF-κB signaling pathway. Consequently, it significantly alleviates Lipopolysaccharides-induced neuroinflammatory responses and ameliorates anxiety- and depression-like behaviors. This study demonstrates a novel antidepressant therapeutic strategy and establishes a new paradigm for mRNA gene therapy in CNS diseases.

Using food-safe sargassum nanocellulose as the binder framework, combined with food-grade additives, a highly biocompatible fully ingestible supercapacitor is successfully employed. This design introduces high mechanical strength and fast ion transport behavior of the nanofiber, achieving a disposable power supply and electrical stimulation antibacterial in vivo, which provides a promising alternative power source for novel medical electronic devices.

Small high-performance energy modules have significant practical value in the biomedical field, such as painless diagnosis, alleviation of gastrointestinal discomfort, and electrical stimulation therapy. However, due to performance limitations and safety concerns, it is a formidable challenge to design a small, emerging ingestible power supply. Here, a fully ingestible supercapacitor (FISC) constructed of sargassum cellulose nanofiber is presented. FISCs exhibit an electrode areal capacitance of 2.29 F cm−2 and a high energy density of 307 µWh cm−2. Furthermore, over 90% of the antibacterial activity against Escherichia coli is achieved during the self-discharge process. Therefore, following insertion into an enteric capsule, this device can enable a disposable power supply and electrostimulation for bacteriostasis in the intestine after being swallowed by a human, which offers new possibilities for scientific and simple therapy.

A microglial-biomimetic memantine-loaded polydopamine nanomedicine, PDA-Mem@M, that achieves blood-brain barrier penetration and brain inflammation site targeting for rapid and precise treatment of depression is designed. PDA-Mem@M effectively alleviate depression-like behaviors. This synergistic strategy, with satisfactory biosafety and strong anti-inflammatory and synaptic plasticity restoration effects, is conducive to advances in depression therapy.

Depression is a common psychiatric disorder, and monoamine-based antidepressants as first-line therapy remain ineffective in some patients. The synergistic modulation of neuroinflammation and neuroplasticity could be a major strategy for treating depression. In this study, an inflammation-targeted microglial biomimetic system, PDA-Mem@M, is reported for treating depression. Microglial membrane-coated nanoparticles penetrate the blood-brain barrier and facilitate microglial targeting. Subsequently, owing to the excellent free radical-scavenging capacity, PDA-Mem@M attenuate the brain inflammatory microenvironment. After on-demand release from the nanoparticles, memantine increases the expression of brain-derived neurotrophic factors and reverses the loss of synaptic dendritic spines. Further, in vivo studies demonstrate that PDA-Mem@M effectively alleviate depression-like behaviors to a greater extent than memantine or polydopamine nanoparticles (PDA) monotherapy. This synergistic strategy, with satisfactory biosafety and strong anti-inflammatory and synaptic plasticity restoration effects, is conducive to advances in depression therapy.

This review provides a comprehensive understanding of the role of flame-retardant materials in enhancing the safety and performance of TENG devices, addressing critical challenges in their design and application. It paves the way for researchers and engineers seeking to develop safer, more reliable energy-harvesting technologies.

Triboelectric nanogenerators (TENGs) have gained significant attention for ability to convert mechanical energy into electrical energy. As the applications of TENG devices expand, their safety and reliability becomes priority, particularly where there is risk of fire or spontaneous combustion. Flame-retardant materials can be employed to address these safety concerns without compromising the performance and efficiency of TENGs. The primary focus of this review is on flame-retardant materials, including polymers, biomaterials, liquid polymers, aerogels, and carbon-based materials. The fundamental properties of these materials for TENG applications are elucidated. The characteristics of each material type are described, along with their potential to boost the safety and performance of TENGs. The importance of flame retardancy in advancing TENG technology can be projected from its usage in wearable electronics, self-powered sensors, and smart textiles. Current challenges such as material compatibility, fabrication complexity, and environmental concerns are addressed, along with proposed strategies for overcoming them. This review underscores the significance of flame-retardant materials in strengthening the functionality and safety of TENG devices, paving the way for their widespread adoption across various industries.  

This study reveals the pivotal role of ferroelectric-like crystals in boosting the high-temperature capacitive energy storage of polynorbornene dielectrics. This distinctive characteristic enables the polymers to exhibit an impressive high-temperature discharge energy density of 6.76 J cm−3, even under electric fields that are far below their Weibull breakdown strength.

Achieving optimal capacitive energy storage performance necessitates the integration of high energy storage density, typical of ferroelectric dielectrics, with the low polarization loss associated with linear dielectrics. However, combining these characteristics in a single dielectric material is challenging due to the inherent contradictions between the spontaneous polarization of ferroelectric dielectrics and the adaptability of linear dielectrics to changes in the electric field. To address this issue, a linear isotactic sulfonylated polynorbornene dielectric characterized by ferroelectric-like crystals has been developed. The sulfonyl dipoles in the ferroelectric-like crystals are oriented in the same direction, thereby enabling this polymer to exhibit a considerable dielectric constant (7.5) at room temperature. Notably, when the operating temperature surpasses the polymer's glass transition temperature (T g ≈ 140 °C), its dielectric constant rises to 12 with just minor changes in the dissipation factor. At 150 °C, 90% efficiency of the discharge energy density reaches as high as 6.76 J cm−1 under a low electric field of 320 MV m−1, which is ten times that of the state-of-the-art, high-temperature, capacitor-grade polyetherimide. The enhancement of high-temperature capacitive performance, achieved by utilizing the crystallinity of isotactic polymers to form a polar structure, presents a new perspective for the design of high-temperature dielectric polymers.

This work systematically explores piezoelectric response of vitamin-based self-assemblies for power generation. Vitamin molecules can self-assemble into different supramolecular structures exhibiting tunable predicted piezoelectric coefficients. Vitamin B7 D-biotin (D-BIO) self-assemblies with high piezoelectricity are fabricated into piezoelectric devices for human motion monitoring and energy harvesting. These findings will facilitate the exploration and development of biomolecule-based piezoelectric materials.

Structural diversity of biomolecules leads to various supramolecular organizations and asymmetric architectures of self-assemblies with significant piezoelectric response. However, the piezoelectricity of biomolecular self-assemblies has not been fully explored and the relationship between supramolecular structures and piezoelectricity remains poorly understood, which hinders the development of piezoelectric biomaterials. Herein, for the first time, the piezoelectricity of vitamin-based self-assemblies for power generation is systematically explored. X-ray diffraction studies revealed that vitamin molecules can self-assemble into different supramolecular structures, which exhibited tunable piezoelectric coefficients ranging from 3.8 to 42.8 pC N−1 by density functional theory (DFT) calculations. Notably, vitamin B7 D-biotin (D-BIO) self-assemblies exhibited superior piezoelectricity due to low crystal symmetry and high polarization of supramolecular arrangements. The D-BIO assemblies-based piezoelectric nanogenerator (PENG) produced output voltages of ≈0.8 V under a mechanical force of 47 N, showing high mechanical durability after 5400 pressing-releasing cycles and high stability of at least three months. The PENG-based wearable sensor successfully detected bending motions of human limbs. Furthermore, the PENG-based insole converted biomechanical energy into stable electrical energy upon foot movement, illuminating 12 light-emitting diodes (LEDs). This work fills knowledge gaps in piezoelectricity of vitamin-based self-assemblies, providing paradigms for realizing high-performance piezoelectric biomaterials through supramolecular engineering.

Based on two kinds of biomolecule-MOFs, we construct a self-powered multi-functional wearable device by combining Zn-Car_MOF and patterned PDMS to achieve various environmental energy collection (water droplets, ocean energy, and e-bike driving) and human gait detection, when Thy loaded Cu-HHTP_MOF combined with wearable fibers are cooperated with Zn-Car_TPHG, achieving electrocatalytic ROS generation and drug releasing synergistic sterilization.

New types of metal–organic framework (MOF) materials have great potential in solving the current global dilemma on energy, environment, and medical care. Herein, based on two kinds of biomolecule-MOFs (Bio-MOFs) with favorable biocompatibility and degradation-reconstruction characteristics, we have established a self-powered muti-functional device to achieve an efficient and broad-spectrum environmental energy collection and biomedical applications. Combining Zn(II) and carnosine-based Zn-Car_MOF possessing a high piezoelectric response (d 33 = 11.17 pm V−1) with patterned polydimethylsiloxane (PDMS) film, a tribo-piezoelectric hybrid nanogenerator (TPHG) is constructed with a synergy output of triboelectric and piezoelectric effects. The Zn-Car_TPHG demonstrates a high output performance (131 V at 100 kPa) and a wide range of pressure response (1 Pa–100 kPa), possessing applications in environmental energy collection and biomedical sensors. To expand the application of the wearable device, a conductive hexagonal prism MOF (Cu3(2,3,6,7,10,11-hexahydroxytriphenylene)2 (Cu-HHTP)) is synthesized and employed to load thymol (Thy). Cooperating with Zn-Car_TPHG, the resulting Cu-HHTP/Thy can achieve an efficient self-powered ROS (singlet oxygen (1O2) and hydroxyl radical (·OH)) generation and drug synergistic broad-spectrum sterilization effect (efficiency ≥ 98%). In a word, the flexible wearable device based on the muti-functional Bio-MOFs is sustainable and environmentally friendly, possessing wide application potential in fields of environmental energy collection, biosensors, and self-powered antibacterial.

Hierarchically porous covalent organic frameworks (hCOFs) are constructed using a solvothermal template-induced synthetic strategy. Commercially available zinc oxide nanoparticles are employed as hard template enabling an increase in total pore volume in a series of COFs. The hierarchically porous nature of hCOFs significantly reduces diffusion limitations, thus leading to simultaneous enhancements in adsorption capacity, diffusivity, and catalytic performance.

The rapid advancement of covalent organic frameworks (COFs) in recent years has firmly established them as a new class of molecularly precise and highly tuneable porous materials. However, compared to other porous materials, such as zeolites and metal-organic frameworks, the successful integration of hierarchical porosity into COFs remains largely unexplored. The challenge lies in identifying appropriate synthetic methods to introduce secondary pores without compromising the intrinsic structural porosity of COFs. In this study, a template-induced synthetic methodology is realized to facilitate the construction of hierarchically porous COFs (hCOFs). This novel approach utilizes commercially available zinc oxide nanoparticles as a hard template, enabling to increase the total pore volume of a series of β-ketoenamine-linked COFs as well as an imine-based COF while preserving their surface areas. In addition to transmission electron microscopy and gas adsorption analyses, small-angle X-ray scattering and pulsed field gradient nuclear magnetic resonance techniques are employed to investigate the hierarchical porosity and diffusivity of guest molecules within hCOFs. This study demonstrates that the hierarchically porous nature of hCOFs significantly reduces diffusion limitations, thus leading to simultaneous enhancements in adsorption capacity, diffusivity, and catalytic performance.

Green and red quantum dot (QD) luminescence microspheres with simultaneous excellent color conversion performance and high photoluminescence stability are synthesized by a facile wet chemical process. They further serve as color conversion materials for the fabrication of green and red micro-LEDs, which exhibit world-record external quantum efficiencies of 40.8% and 22.1% and high brightnesses of 1.7 × 108 and 7.6 × 107 cd m−2.

Quantum dot (QD)-converted micrometer-scale light-emitting diodes (micro-LEDs) are regarded as an effective solution for achieving high-performance full-color micro-LED displays because of their narrow-band emission, simplified mass transfer, facile drive circuits, and low cost. However, these micro-LEDs suffer from significant blue light leakage and unsatisfactory electroluminescence properties due to the poor light conversion efficiency and stability of the QDs. Herein, the construction of green and red QD luminescence microspheres with the simultaneously high conversion efficiency of blue light and strong photoluminescence stability are proposed. These luminescence microspheres exhibit high external photoluminescence quantum yields exceeding 46% under 450 nm excitation, along with excellent reliability against blue light, heat, and water-oxygen degradation, owing to the waveguide and spatial confinement effects of the microspheres. The microsphere-based green and red micro-LEDs achieve world-record external quantum efficiencies of 40.8% and 22.1%, respectively, and high brightness values of 1.7 × 108 and 7.6 × 107 cd m−2, respectively. Finally, 0.6 inch red, green, and blue monochrome micro-LED displays are demonstrated by integrating microsphere-converted micro-LED arrays with thin-film transistor backplanes, which show a pixel resolution as high as 1700 PPI and brightness exceeding 10 000 cd m−2.

Mechanical information recognition technology, which integrates information acquisition, pre-processing and processing, promises to enable applications in intelligent robotics, healthcare, and virtual reality. The mechanosensory systems of organisms in nature have inspired to develop mechanical information bionic recognition technology to address the challenges of information acquisition performance and information processing efficiency. In this work, bionic strategies for information pre-processing, acquisition, and processing are summarized systematically. The potential applications, future challenges, and opportunities of MIBRT are also presented.

Mechanical information is a medium for perceptual interaction and health monitoring of organisms or intelligent mechanical equipment, including force, vibration, sound, and flow. Researchers are increasingly deploying mechanical information recognition technologies (MIRT) that integrate information acquisition, pre-processing, and processing functions and are expected to enable advanced applications. However, this also poses significant challenges to information acquisition performance and information processing efficiency. The novel and exciting mechanosensory systems of organisms in nature have inspired us to develop superior mechanical information bionic recognition technologies (MIBRT) based on novel bionic materials, structures, and devices to address these challenges. Herein, first bionic strategies for information pre-processing are presented and their importance for high-performance information acquisition is highlighted. Subsequently, design strategies and considerations for high-performance sensors inspired by mechanoreceptors of organisms are described. Then, the design concepts of the neuromorphic devices are summarized in order to replicate the information processing functions of a biological nervous system. Additionally, the ability of MIBRT is investigated to recognize basic mechanical information. Furthermore, further potential applications of MIBRT in intelligent robots, healthcare, and virtual reality are explored with a view to solve a range of complex tasks. Finally, potential future challenges and opportunities for MIBRT are identified from multiple perspectives.

A sole-solvent high-entropy electrolyte is capable of forming stable anion-derived electrode–electrolyte interphases, extending the temperature extremes of the battery. Consequently, high-voltage anode-free sodium batteries with cycling ability in a wide temperature range (−20–60 °C) are realized. Furthermore, Ah-level pouch cell delivers a leadingly high energy density (209 Wh kg−1) and a high capacity retention (83.1%) after 100 cycles at 25 °C.

Anode-free sodium batteries (AFSBs) hold great promise for high-density energy storage. However, high-voltage AFSBs, especially those can stably cycle at a wide temperature range are challenging due to the poor electrolyte compatibility toward both the cathode and anode. Herein, high-voltage AFSBs with cycling ability in a wide temperature range (−20–60 °C) are realized for the first time via a sole-solvent high-entropy electrolyte based on the diethylene glycol dibutyl ether solvent (D2) and NaPF6 salt. The sole-solvent high-entropy electrolyte with unique solvent-ions effect of strong anion interaction and weak cation solvation enables entropy-driven electrolyte salt disassociation and high-concentration contact ion pairs, thus simultaneously forming stable anion-derived electrode–electrolyte interphases on cathode and anode. Moreover, the wide liquid range of D2 further extends the temperature extremes of the battery. Consequently, ampere-hour (Ah)-level anode-free sodium pouch cells with cyclability in a wide temperature range of −20–60 °C are realized. Impressively, the pouch cell achieves a leadingly high cell-level energy density of 209 Wh kg−1 and a high capacity retention of 83.1% after 100 cycles at 25 °C. This work provides inspirations for designing advanced electrolytes for practical AFSBs.

This article presents the design and characterization of first molecular ferroelectric Mott insulator, (C7H14N)3V12O30. Accompanied by the ferroelectric phase transition, (C7H14N)3V12O30 shows a sharp change in conductivity, implying the metal–insulator transition-like behavior. This finding opened up new possibilities for the development of strongly correlated electron systems.

With the discovery of colossal magnetoresistance materials and high-temperature superconductors, Mott insulators can potentially undergo a transition from insulating state to metallic state. Here, in molecular ferroelectrics system, a Mott insulator of (C7H14N)3V12O30 has been first synthesized, which is a 2D organic–inorganic ferroelectric with composition of layered vanadium oxide and quinuclidine ring. Interestingly, accompanied by the ferroelectric phase transition, (C7H14N)3V12O30 changes sharply in conductivity. The occurrence of a Mott transition has been proven by electric transport measurements and theoretical calculations. This research has significantly expanded the applicative horizons of ferroelectric materials, and offering an ideal platform for the investigation of strongly correlated electron systems.

ZnFe2O4 nanoparticles self-assemble in situ effectively and introduce mechanical force simulating primary biomechanical into the tiny target spot of TME through wireless magnetic control, which effectively inhibits tumor migration.

Mechanical force attracts booming attention with the potential to tune the tumor cell behavior, especially in cell migration. However, the current approach for introducing mechanical input is difficult to apply in vivo. How the mechanical force affects cell behavior in situ also remains unclear. In this work, an intelligent miniaturized platform is constructed with magnetic ZnFe2O4 (ZFO) micromotors. The wireless ZFO can self-assemble in situ and rotate to generate mechanical torque of biologically relevant piconewton-scale at the target tumor site. It is observed unexpectedly that enhanced in situ mechanical rotating torque from ZFO micromotors and the active fluid inhibit the migration of highly invasive A549 tumor cells. The down-regulation of the Piezo1 channel and the suppressed signaling of ROCK1 in mechano-adaptive tumor cells is found to be related to the inhibition effect. With effectiveness confirmed with the zebrafish xenograft model, this platform provides a valuable toolkit for mechanobiology and force-associated non-invasive tumor therapy.

This review outlines advancements in untethered soft robots based on 1D and 2D nanomaterials. It covers basic locomotion forms like crawling, jumping, swimming, rolling, gripping, and multimodal, along with self-sustained motions like light tracking, self-oscillating, self-crawling, self-rolling, and flying. It also summarizes progress in integrating sensing, energy harvesting, energy storage, self-healing, and color response into soft actuators.

Biological structures exhibit autonomous and intelligent behaviors, such as movement, perception, and responses to environmental changes, through dynamic interactions with their surroundings. Inspired by natural organisms, future soft robots are also advancing toward autonomy, sustainability, and interactivity. This review summarizes the latest achievements in untethered soft robots based on 1D and 2D nanomaterials. First, the performance of soft actuators designed with different structures is compared. Then, the development of basic locomotion forms, including crawling, jumping, swimming, rolling, gripping, and multimodal, mimicking biological motion mechanisms under dynamic stimuli, is discussed. Subsequently, various self-sustained movements based on imbalance mechanisms under static stimuli are introduced, including light tracking, self-oscillating, self-crawling, self-rolling, and flying. Following that, the progress in soft actuators integrated with additional functionalities such as sensing, energy harvesting, and storage is summarized. Finally, the challenges faced in this field and the prospects for future development are discussed.

This review explores the advances in halide perovskite lasers, covering key topics such as emission properties, optical gain mechanisms, and diverse laser architectures. It also discusses challenges related to CW-pumped and electrically driven lasing and outlines future research directions aimed at improving material durability, optimizing thermal management, and developing fabrication techniques for scalable, efficient devices.

Over the past decade, semiconducting halide perovskite lasers have emerged as a transformative platform in optoelectronics, owing to unique properties such as high photoluminescence quantum yields, tunable bandgaps, and low-cost fabrication processes. This review systematically examines the advancements in halide perovskite lasers, covering diverse laser architectures, such as whispering gallery mode, Fabry–Pérot, plasmonic, bound states in the continuum (BIC), quantum dot, and polariton lasers. The mechanisms of optical gain, the role of material engineering in optimizing lasing performance, and the challenges associated with continuous-wave (CW) pumping and electrically driven lasing are discussed. Furthermore, recent progress in improving the stability and scalability of perovskite lasers, essential for their integration into practical applications in displays, optical communications, sensing, and integrated photonics is highlighted. Finally, future research directions are discussed, emphasizing the potential of perovskite lasers to revolutionize various technological domains by enabling the development of next-generation photonic devices.

A reversible switching between colored and bleached phases of three colors of inorganic perovskite smart windows is induced using dimethyl sulfoxide vapor at room temperature. Compared with normal houses in field tests, the model houses with three colors of smart windows reached a maximum indoor temperature drop of 2.6, 3.6, and 4.2 °C at noon, respectively, showing excellent energy-saving potential.

Perovskite smart windows (PSWs) are widely investigated owing to excellent thermochromic properties, while restricted by poor transition performance and cycle stability. Herein, dimethyl sulfoxide vapor is utilized as an induction reagent for rapid reversible switching at room temperature between the colored and bleached phases. To obtain PSWs with different optical properties and transition performance, red CsPbIBr2, yellow Rb0.5Cs0.5PbIBr2 and brown CsSn0.1Pb0.9IBr2 are prepared through alloying. The perovskites can exhibit reversible switching at 27.4–34.3 °C within 1.9–5.1 min. Even after 100 cycles, they exhibit remarkable stability of luminous transmittance (retention ≥97.4%) and transition time (retention ≥97.6%). Experimental characterization proves that the reversible switching occurs between colored three-dimension perovskite phase and bleached zero-dimension perovskite phase. In the field test (air temperature = 21.6–26.5 °C), model houses with PSWs exhibit a maximum indoor temperature drop of 4.2 °C. Furthermore, they exhibit considerable temperature modulation ability up to 7.9 °C under a solar simulator (temperature of the control model house = 60 °C). The decrease in the luminous transmittance of the PSWs after 20 days is 2.9%, indicating excellent long-term stability. This study offers PSWs with prominent transition performance and long cycle stability.

The in situ atomic scale transmission electron microscopy experiment reveals a non-polar phase-mediated ferroelectric-ferroelastic coupled switching pathway in fluorite oxides.

HfO2/ZrO2-based ferroelectrics present tremendous potential for next-generation non-volatile memory due to their high scalability and compatibility with silicon technology. Unlike the continuous polar layers in perovskite ferroelectrics, HfO2/ZrO2-based ferroelectrics are composed of alternating polar layers with oxygen shifts and non-polar spacers, which leads to a distinct ferroelectric switching mechanism. However, directly observing the switching process has been a big challenge due to the polymorph feature of nanoscale fluorites and the difficulty in in situ imaging on light elements. Here, the ferroelectric-ferroelastic coupled switching process in freestanding ZrO2 thin films is directly visualized by in situ imaging on oxygen motions. A multi-step 90-degree polarization switching mechanism is uncovered that challenges the conventional one-step 180-degree switching paradigms in fluorite oxides, which is highly consistent with the interlocked nature of ferroelectricity and ferroelasticity. A non-polar tetragonal (T) phase is discovered as a crucial intermediate state, lowering the energy barrier for polarization switching by 35%. More importantly, the T phase prevents irreversible transitions to the non-polar ground state and facilitates stable ferroelectric switching. These findings are fundamental to understanding nanoscale polarization switching mechanisms in fluorite ferroelectrics, paving the way for advanced high-durability devices.

This article introduces an innovative method, achieving molecular-level epitaxial growth of metal–organic frameworks (MOF) on BiVO4 photoanodes by precisely controlling the concentration of surface oxygen vacancies. The seamless interface of BiVO4/MOF optimizes electron transfer and reduces recombination losses, elevating the overall efficiency of the PEC water oxidation.

Efficient charge separation at the semiconductor/cocatalyst interface is crucial for high-performance photoelectrodes, as it directly influences the availability of surface charges for solar water oxidation. However, establishing strong molecular-level connections between these interfaces to achieve superior interfacial quality presents significant challenges. This study introduces an innovative electrochemical etching method that generates a high concentration of oxygen vacancy sites on BiVO4 surfaces (Ov-BiVO4), enabling interactions with the oxygen-rich ligands of MIL-101. This reduces the formation energy and promotes conformal growth on BiVO4. The Ov-BiVO4/MIL-101 composite exhibits an ideal semiconductor/cocatalyst interface, achieving an impressive photocurrent density of 5.91 mA cm−2 at 1.23 VRHE, along with excellent stability. This high-performing photoanode enables an unbiased tandem device with an Ov-BiVO4/MIL-101-Si solar cell system, achieving a solar-to-hydrogen efficiency of 4.33%. The molecular-level integration mitigates surface states and enhances the internal electric field, facilitating the migration of photogenerated holes into the MIL-101 overlayer. This process activates highly efficient Fe catalytic sites, which effectively adsorb water molecules, lowering the energy barrier for water oxidation and improving interfacial kinetics. Further studies confirm the broad applicability of oxygen vacancy-induced molecular epitaxial growth in various MOFs, offering valuable insights into defect engineering for optimizing interfaces and enhancing photocatalytic activity.

The dewatering difficulty of nanocellulose dispersion has long been a major challenge hindering its practical utilization. Here, through a supramolecular scale hydrophilicity regulation, the water retention value is substantially decreased and efficient dewatering of cellulose nanofibers (CNF) dispersion is realized, enabling the fabrication of highly dense, strong, fire-retardant, and moldable CNF bulk materials as sustainable plastic substitutes.

Cellulose nanofibers (CNFs) are ideal building blocks for creating lightweight and strong bulk structural materials due to their unique supramolecular structure and exceptional mechanical properties within the crystalline regions. However, assembling CNFs into dense bulk structural materials with customizable shape and functionalities remains a great challenge, hindering their practical applications. Here, the dewatering issue of aqueous CNF dispersions is addressed by regulating supramolecular scale hydrophilicity using lactic acid, combined with hot-press molding. This approach enables the fabrication of transparent CNF bulk structural materials with a density of up to 1.426 g cm−3. The mechanical properties, including isotropic in-plane tensile strength (75.5 ± 4.5 MPa), flexural strength (198 ± 20 MPa), and hardness (≈300 MPa), surpass most engineering plastics. Moreover, unlike conventional CNF based materials, the CNF bulk structural materials exhibit remarkable water stability and flame retardancy. These unique advantages open a new avenue to bottom-up assembly of CNFs into high-performance multifunctional eco-friendly structural materials, dedicating to substitution of plastics and easing the consumption of petrochemical resources.