Photobreeding Heterojunction on Semiconductor Materials for Enhanced Photocatalysis

Construction of heterojunctions to photocatalysts is one of the most promising approaches to improve charge separation efficiency; however, the established constructing processes usually require high-temperature conditions and/or the adding of highly concentrated or expensive exotic species, and the improvement of effective contact and charge exchange between heterojunction components remains a problem. This work proposes an unprecedented “photobreeding” method and realizes the direct growth of Zn nanowires and Mott–Schottky heterojunctions from ZnS or viologen-coated ZnS microspheres through a photochemical reaction at room temperature without external species, while demonstrating the hypothesis proposed 140 years ago on the formation of Zn in the photochromic process of ZnS. After photobreeding of the heterojunctions, the hydrogen production efficiency of the photocatalysts increases by 2 orders of magnitude. This inexpensive, facile and efficient synthetic method will find applications in H₂ production, organic synthesis, CO₂ reduction, nitrogen fixation, and so on.     

Ultrahigh Energy Storage Capacitors Based on Freestanding Single-Crystalline Antiferroelectric Membrane/PVDF Composites

Inorganic/organic dielectric composites are very attractive for high energy density electrostatic capacitors. Usually, linear dielectric and ferroelectric materials are chosen as inorganic fillers to improve energy storage performance. Antiferroelectric (AFE) materials, especially single-crystalline AFE oxides, have relatively high efficiency and higher density than linear dielectrics or ferroelectrics. However, adding single-crystalline AFE oxides into polymers to construct composite with improved energy storage performance remains elusive. In this study, high-quality freestanding single-crystalline PbZrO₃ membranes are obtained by a water-soluble sacrificial layer method. They exhibit classic AFE behavior and then 2D–2D type PbZrO₃/PVDF composites with the different film thicknesses of PbZrO₃ (0.1-0.4 µm) is constructed. Their dielectric properties and polarization response improve significantly as compared to pure PVDF and are optimized in the PbZrO₃(0.3 µm)/PVDF composite. Consequently, a record-high energy density of 43.3 J cm⁻³ is achieved at a large breakdown strength of 750 MV m⁻¹. Phase-field simulation indicates that inserting PbZrO₃ membranes effectively reduces the breakdown path. Single-crystalline AFE oxide membranes will be useful fillers for composite-based high-power capacitors.     

Polyether-b-Amide Based Solid Electrolytes with Well-Adhered Interface and Fast Kinetics for Ultralow Temperature Solid-State Lithium Metal Batteries

Solid-state lithium metal batteries (SSLMBs) are highly desirable for energy storage because of the urgent need for higher energy density and safer batteries. However, it remains a critical challenge for stable cycling of SSLMBs at low temperature. Here, a highly viscoelastic polyether-b-amide (PEO-b-PA) based composite solid-state electrolyte is proposed through a one-pot melt processing without solvent to address this key process. By adjusting the molar ratio of PEO-b-PA to lithium bis(trifluoromethanesulphonyl)imide (ethylene oxide:Li = 6:1) and adding 20 wt.% succinonitrile, fast Li⁺ transport channel is conducted within the homogeneous polymer electrolyte, which enables its application at ultra-low temperature (−20 to 25 °C). The composite solid-state electrolyte utilizes dynamic hydrogen-bonding domains and ion-conducting domains to achieve a low interfacial charge transfer resistance (<600 Ω) at −20 °C and high ionic conductivity (25 °C, 3.7 × 10⁻⁴ S cm⁻¹). As a result, the LiFePO₄|Li battery based on composite electrolyte exhibits outstanding electrochemical performance with 81.5% capacity retention after 1200 cycles at −20 °C and high discharge specific capacities of 141.1 mAh g⁻¹ with high loading (16.1 mg cm⁻²) at 25 °C. Moreover, the solid-state SNCM811|Li cell achieves excellent safety performance under nail penetration test, showing great promise for practical application.     

Soft Robotic-Adapted Multimodal Sensors Derived from Entirely Intrinsic Self-Healing and Stretchable Cross-Linked Networks

Flexible sensing technologies that play a pivotal role in endowing robots with detection capabilities and monitoring their motions are impulsively desired for intelligent robotics systems. However, integrating and constructing reliable and sustainable flexible sensors with multifunctionality for robots remains an everlasting challenge. Herein, an entirely intrinsic self-healing, stretchable, and attachable multimodal sensor is developed that can be conformally integrated with soft robots to identify diverse signals. The dynamic bonds cross-linked networks including the insulating polymer and conductive hydrogel with good comprehensive performances are designed to fabricate the sensor with prolonged lifespan and improved reliability. Benefiting from the self-adhesiveness of the hydrogel, strong interfacial bonding can be formed on various surfaces, which promotes the conformable integration of the sensor with robots. Due to the ionic transportation mechanism, the sensor can detect strain and temperature based on piezoresistive and thermoresistive effect, respectively. Moreover, the sensor can work in triboelectric mode to achieve self-powered sensing. Various information can be identified from the electrical signals generated by the sensor, including hand gestures, soft robot crawling motions, a message of code, the temperature of objects, and the type of materials, holding great promise in the fields of environmental detection, wearable devices, human-machine interfacing, and robotics.     

Optoelectronic Synapses and Photodetectors Based on Organic Semiconductor/Halide Perovskite Heterojunctions: Materials,Devices, and Applications

Both photodetectors (PDs) and optoelectronic synaptic devices (OSDs) are optoelectronic devices converting light signals into electrical responses. Optoelectronic devices based on organic semiconductors and halide perovskites have aroused tremendous research interest owing to their exceptional optical/electrical characteristics and low-cost processability. The heterojunction formed between organic semiconductors and halide perovskites can modify the exciton dissociation/recombination efficiency and modulate the charge-trapping effect. Consequently, organic semiconductor/halide perovskite heterojunctions can endow PDs and OSDs with high photo responsivity and the ability to simulate synaptic functions respectively, making them appropriate for the development of energy-efficient artificial visual systems with sensory and recognition functions. This article summarizes the recent advances in this research field. The physical/chemical properties and preparation methods of organic semiconductor/halide perovskite heterojunctions are briefly introduced. Then the development of PDs and OSDs based on organic semiconductor/halide perovskite heterojunctions, as well as their innovative applications, are systematically presented. Finally, some prospective challenges and probable strategies for the future development of optoelectronic devices based on organic semiconductor/halide perovskite heterojunctions are discussed.     

Challenges and Opportunities of Implantable Neural Interfaces: From Material,Electrochemical and Biological Perspectives

The desirable implantable neural interfaces can accurately record bioelectrical signals from neurons and regulate neural activities with high spatial/time resolution, facilitating the understanding of neuronal functions and dynamics. However, the electrochemical performance (impedance, charge storage/injection capacity) is limited with the miniaturization and integration of neural electrodes. The “crosstalk” caused by the uneven distribution of elctric field leads to lower electrical stimulation/recording efficiency. The mismatch between stiff electrodes and soft tissues exacerbates the inflammatory responses, thus weakening the transmission of signals. Though remarkable breakthroughs have been made through the incorporation of optimizing electrode design and functionalized nanomaterials, the chronic stability, and long-term activity in vivo of the neural electrodes still need further development. In this review, the neural interface challenges mainly on electrochemistry and biology are discussed, followed by summarizing typical electrode optimization technologies and exploring recent advances in the application of nanomaterials, based on traditional metallic materials, emerging 2D materials, conducting polymer hydrogels, etc., for enhancing neural interfaces. The strategies for improving the durability including enhanced adhesion and minimized inflammatory response, are also summarized. The promising directions are finally presented to provide enlightenment for high-performance neural interfaces in future, which will promote profound progress in neuroscience research.     

Poly(pentahydropyrimidine)-Based Hybrid Hydrogel with Synergistic Antibacterial and Pro-Angiogenic Ability for the Therapy of Diabetic Foot Ulcers

Bacterial infection and impaired angiogenesis make the treatment of diabetic foot ulcers (DFU) extremely challenging. Cationic polymers are expected to treat infected wounds due to their excellent antibacterial properties, but still, it is difficult to meet the therapeutic needs of pro-angiogenesis and anti-infections due to their simple construction units and outmoded synthesis methods. Herein, a cationic poly(pentahydropyrimidine) (PPHP) library with strong modifiability is synthesized to construct a hybrid hydrogel with synergistic therapeutic effects for the treatment of infected DFUs. It is found that the as-synthesized hybrid hydrogel can up-regulate angiogenesis-related gene (HIF-1, VEGF, and bFGFR/bFGF) expression and targeted disruption of bacterial cell membranes, which finally promotes the healing of infected DFU (wound healing rate: 92%) within 10 days. This hydrogel, thus, holds great promise in developing new strategies to significantly enhance the treatment of DFU and other bacterial-infected pathological diagnoses.     

Hyperelastic,Robust, Fire-Safe Multifunctional MXene Aerogels with Unprecedented Electromagnetic Interference Shielding Efficiency

MXene aerogels have shown great potential for many important functional applications, in particular electromagnetic interference (EMI) shielding. However, it has been a grand challenge to create mechanically hyperelastic, air-stable, and durable MXene aerogels for enabling effective EMI protection at low concentrations due to the difficulties in achieving tailorable porous structures, excellent mechanical elasticity, and desired antioxidation capabilities of MXene in air. Here, a facile strategy for fabricating MXene composite aerogels by co-assembling MXene and cellulose nanofibers during freeze-drying followed by surface encapsulation with fire-retardant thermoplastic polyurethane (TPU) is reported. Because of the maximum utilization of pore structures of MXene, and conductive loss enhanced by multiple internal reflections, as-prepared aerogel with 3.14 wt% of MXene exhibits an exceptionally high EMI shielding effectiveness of 93.5 dB, and an ultra-high MXene utilization efficiency of 2977.71 dB g g⁻¹, tripling the values in previous works. Owing to the presence of multiple hydrogen bonding and the TPU elastomer, the aerogel exhibits a hyperelastic feature with additional strength, excellent stability, superior durability, and high fire safety. This study provides a facile strategy for creating multifunctional aerogels with great potential for applications in EMI protection, wearable devices, thermal management, pressure sensing, and intelligent fire monitoring.     

A Self-Assembled Vertical-Gradient and Well-Dispersed MXene Structure for Flexible Large-Area Perovskite Modules

Advancing hole transport layers (HTL) to realize large-area, flexible, and high-performance perovskite solar cells (PSCs) is one of the most challenging issues for its commercialization. Here, a self-assembled gradient Ti₃C₂T_x MXene incorporated PEDOT:PSS HTL is demonstrated to achieve high-performance large-area PSCs by establishing half-caramelization-based glucose-induced MXene redistribution. Through this process, the Ti₃C₂T_x MXene nanosheets are spontaneously dispersed and redistributed at the top region of HTL to form the unique gradient distribution structure composed of MXene:Glucose:PEDOT:PSS (MG-PEDOT). These results show that the MG-PEDOT HTL not only offers favorable energy level alignment and efficient charge extraction, but also improves the film quality of perovskite layer featuring enlarged grain size, lower trap density, and longer carrier lifetime. Consequently, the power conversion efficiency (PCE) of the flexible device based on MG-PEDOT HTL is increased by 36% compared to that of pristine PEDOT:PSS HTL. Meanwhile, the flexible perovskite solar minimodule (15 cm² area) using MG-PEDOT HTL achieve a PCE of 17.06%. The encapsulated modules show remarkable long-term storage stability at 85 °C in ambient air (≈90% efficiency retention after 1200 h) and enhanced operational lifetime (≈90% efficiency retention after 200 h). This new approach shows a promising future of the self-assembled HTLs for developing optoelectronic devices.