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

Biomimetic Chlorosomes

Photocatalytic therapy suffers from inefficiencies due to its reliance on oxygen and the attendant risk of unregulated activation. In article number 2413385, Wen Sun, Chao Yang, Wen-fei Dong, and their colleagues present a Chlorosome-mimetic nanoreactor (Ru-Chlos), made by aggregating ruthenium-polypyridyl-silane monomers, showing great photocatalytic ability in acidic conditions without oxygen consumption, and its photocatalytic activity of Ru-Chlos can be impeded by the light-responsive disassembly.

3D Printing

A novel organic ink based on egg albumen and saccharides is developed to create sacrificial supports for gelatin-based hydrogel prints. The cover photo shows biogel scaffolds with tunable pore size down to 0.4 mm, enabled by selective support removal. This allows printing of complex-shaped biodegradable joint-like vacuum actuators with 60° maximum bending angle at 0.23 s response time. More details can be found in article number 2409403 by Martin Kaltenbrunner and co-workers.

Solid-State Electrolytes

In article number 2410402, Jianwen Liang, Xueliang Sun, Xiaona Li, and co-workers present a pioneering and universal strategy for the hydrate-assisted synthesis of LiAlOCl solid-state electrolytes, enabling the kilogram-scale synthesis of low-cost aluminum-based chloroxides. The oxychloride SSEs contain large amounts of amorphous [Al a O b Cl c ](2b+c−3a)− components, achieving faster local mobility of lithium ions. The technology is expected to promote the industrial application of high specific energy all-solid-state batteries.

Ultrafast Symmetry Control

In article 2414196, Burak Guzelturk and co-workers reveal an ultrafast symmetry change upon photoexcitation in PbS quantum dots using time-resolved structural techniques. The magnitude of symmetry change is tunable by quantum dot surface chemistry, opening a pathway to designed phase changes for applications in data storage, computing, and sensing in the future.

Spatiotemporal Programmable 3D Chiral Blue Phase Patterns

In article number 2411988, Wenjie Yang, Chenglin Zheng, Jingxia Wang, and co-workers propose a method for spatiotemporal control of inkjet printing 3D chiral patterns in blue phase liquid crystals (BPLCs). Spontaneous ink diffusion in dual-chiral polymer-templated BPLCs enables programmable evolution of photonic bandgaps, and spatial chiral modes. The study quantitatively links ink diffusion kinetics to 3D optical diffraction of BPLCs, offering potential applications in time-temperature indicators, multidimensional encryption, and advanced optical sensor devices.

MicroRNA Sponge

The illustration depicts a tetrahedral RNA sponge constructed using a DNA framework, capable of simultaneously carrying three microRNA inhibitors. It can adsorb target microRNA molecules and deplete reactive oxygen species. This modulation alters the inflammatory state, promoting the transition of M1 macrophages to M2 macrophages, thereby alleviating pulmonary inflammatory damage and restoring microenvironmental homeostasis. More details can be found in article number 2414336 by Taoran Tian, Yunfeng Lin, and co-workers.

Ultraflexible Vertical Organic Electrochemical Transistors

Ultra-flexible, skin-conformable vertical-structure organic electrochemical transistors adhere seamlessly to the epidermis, enabling highly sensitive monitoring of physiological signals at ultra-low voltages. Their exceptional flexibility and strong skin adherence support accurate signal detection, driving advancements in non-invasive health monitoring applications. More details can be found in article number 2410444 by Myung-Han Yoon, Sungjun Park, and co-workers.

Motion-Adaptive Tessellated Skin Patches

In article number 2412271, Jae Joon Kim, Hoon Eui Jeong, and co-workers develop a multifunctional skin adhesive patch that integrates phase change elements in a tessellated configuration. This patch simultaneously provides remarkable skin adhesion, dynamic motion adaptability, the ability to integrate bulky electronics, on-demand damage-free detachment, low skin contact impedance, a high signal-to-noise ratio, and precise wireless health monitoring.

Flexible metal–organic frameworks (MOFs) present significant potential for gas storage and separation due to their structural dynamic. This review explores the rationale behind the flexible MOFs' enhanced working capacity and separation factors. It also addresses key challenges, including phase transition kinetics, crystal robustness, cycling, shaping, and thermal management, and highlights advanced characterization methods essential for global understanding of flexibility phenomena.

Flexible metal–organic frameworks (MOFs) offer unique opportunities due to their dynamic structural adaptability. This review explores the impact of flexibility on gas adsorption, highlighting key concepts for gas storage and separation. Specific examples demonstrate the principal effectiveness of flexible frameworks in enhancing gas uptake and working capacity. Additionally, mixed gas adsorption and separation of mixtures are reviewed, showcasing their potential in selective gas separation. The review also discusses the critical role of the single gas isotherms analysis and adsorption conditions in designing separation experiments. Advanced combined characterization techniques are crucial for understanding the behavior of flexible MOFs, including monitoring of phase transitions, framework–guest and guest–guest interactions. Key challenges in the practical application of flexible adsorbents are addressed, such as the kinetics of switching, volume change, and potential crystal damage during phase transitions. Furthermore, the effects of additives and shaping on flexibility and the “slipping off effect” are discussed. Finally, the benefits of phase transitions beyond improved working capacity and selectivity are outlined, with a particular focus on the advantages of intrinsic thermal management. This review highlights the potential and challenges of using flexible MOFs in gas storage and separation technologies, offering insights for future research and application.

A unique self-assembled gap-rich PdMn nanofibers, featuring with high mass/electron transport highways, which is used as an efficient catalyst of polyethylene terephthalate to high-valued glycolic acid at an industrial current.

Innovating nanocatalysts with both high intrinsic catalytic activity and high selectivity is crucial for multi-electron reactions, however, their low mass/electron transport at industrial-level currents is often overlooked, which usually leads to low comprehensive performance at the device level. Herein, a Cl−/O2 etching-assisted self-assembly strategy is reported for synthesizing a self-assembled gap-rich PdMn nanofibers with high mass/electron transport highway for greatly enhancing the electrocatalytic reforming of waste plastics at industrial-level currents. The self-assembled PdMn nanofiber shows excellent catalytic activity in upcycling waste plastics into glycolic acid, with a high current density of 223 mA cm−2@0.75 V (vs RHE), high selectivity (95.6%), and Faraday efficiency (94.3%) to glycolic acid in a flow electrolyzer. Density functional theory calculation, X-ray absorption spectroscopy combined with in situ electrochemical Fourier transform infrared spectroscopy reveals that the introduction of highly oxophilic Mn induces a downshift of the d-band center of Pd, which optimizes the adsorption energy of the reaction intermediates on PdMn surface, thereby facilitating the desorption of glycolic acid as a high-value product. Computational fluid dynamics simulations confirm that the gap-rich nanofiber structure is conducive for mass transfer to deliver an industrial-level current.

Intra-particle pores play a practical role in cutting down the electrolyte quantity needed during wetting. A high pore-throat ratio empowers Li-rich layered oxides to withstand lean electrolyte conditions at 1.4 g Ah−1 and achieve a specific energy of 600 Wh kg−1 in a pouch cell. This accomplishment charts a course for pore-based regulation in high-energy storage devices.

Reducing excess electrolytes offers a promising approach to improve the specific energy of electrochemical energy storage devices. However, using lean electrolytes presents a significant challenge for porous electrode materials due to heterogeneous wetting. The spontaneous wetting of nano- or meso-pores within particles, though seldom discussed, adversely affects wetting under lean electrolyte conditions. Herein, this undesired wetting behavior is mitigated by enlarging the pore-throat ratio, enabling Li-rich layered oxide to function effectively at very low electrolyte/capacity (E/C) ratio of 1.4 g Ah−1. The resulting pouch cell achieves 606 Wh kg−1 and retains 80% capacity (75% energy) after 70 cycles. Through imaging techniques and molecular dynamics simulations, it is demonstrated that the pore-throat ratio effectively determines the permeability of electrolyte within particles. By elucidating pore-relating mechanisms, this work unveils promising potential of manipulating pore structures in porous electrode materials, an approach that can be applied to improve the specific energy of other devices including semi-solid-state lithium batteries.

Wearable electronics utilizing advanced carbon materials from fossil origins face issues like non-renewability, high energy consumption, and greenhouse gas emissions. Biopolymers present a sustainable alternative for carbon-based wearables. This review highlights the carbonization of key biopolymers—cellulose, lignin, chitin, and silk fibroin—discussing mechanisms, techniques, and applications of biopolymer-derived carbon materials in wearable technology.

Advanced carbon materials are widely utilized in wearable electronics. Nevertheless, the production of carbon materials from fossil-based sources raised concerns regarding their non-renewability, high energy consumption, and the consequent greenhouse gas emissions. Biopolymers, readily available in nature, offer a promising and eco-friendly alternative as a carbon source, enabling the sustainable production of carbon materials for wearable electronics. This review aims to discuss the carbonization mechanisms, carbonization techniques, and processes, as well as the diverse applications of biopolymer-derived carbon materials (BioCMs) in wearable electronics. First, the characteristics of four representative biopolymers, including cellulose, lignin, chitin, and silk fibroin, and their carbonization processes are discussed. Then, typical carbonization techniques, including pyrolysis carbonization, laser-induced carbonization, Joule heating carbonization, hydrothermal transformation, and salt encapsulation carbonization are discussed. The influence of the processes on the morphology and properties of the resultant BioCMs are summarized. Subsequently, applications of BioCMs in wearable devices, including physical sensors, chemical sensors, energy devices, and display devices are discussed. Finally, the challenges currently facing the field and the future opportunities are discussed.

Sodium-ion batteries (SIBs) are rapidly advancing to confront energy and environmental challenges, but the safety of SIBs has not received enough attention. The kinetic triplet model is constructed based on Arrhenius and nonisothermal kinetic equations to unveil a thermal decomposition kinetic mechanism of the P2-type layered transition metal oxides before and after doping.

The safety of the P2-type layered transition metal oxides (P2-NaxTMO2), a promising cathode material for sodium-ion batteries (SIBs), is a prerequisite for grid-scale energy storage systems. However, previous thermal runaway studies mainly focused on morphological changes resulting from gas production detection and thermogravimetric analysis, while the structural transition and chemical reactions underlying these processes are still unclear. Herein, a comprehensive methodology to unveil an interplay mechanism among phase structures, interfacial microcrack, and thermal stability of the charged P2-Na0.8Ni0.33Mn0.67O2 (NNMO) and the P2-Na0.8Ni0.21Li0.12Mn0.67O2 (NNMO-Li) at elevated temperatures is established. Combining a series of crystallographic and thermodynamic characterization techniques, the specific chemical reactions occurring in the NNMO materials during thermal runaway are clarified first and solidly proved that Li doping effectively hinders the dissolution of transition metal ions, reduces oxygen release, and enhances thermal stability at elevated temperatures. Importantly, based on Arrhenius and nonisothermal kinetic equations, the kinetic triplet model is successfully constructed to in-depth elucidate the thermal decomposition reaction mechanism of P2-NaxTMO2, demonstrating that such thermodynamic assessment provides a new perspective for building high-safety SIBs.

A ZrO2-SiO2 fiber aerogel with a supercontinuous nanolayer is developed for high-temperature thermal insulation. The supercontinuous arrangement of ultra-fine ZrO2 grains on the aerogel surface enables close connections between grains and fibers, promoting efficient transmission of mechanical and thermal stresses, which contributes to record-high specific strength and remarkable thermal-insulating behaviors.

Breaking the thermal, mechanical and lightweight performance limit of aerogels has pivotal significance on thermal protection, new energy utilization, high-temperature catalysis, structural engineering, and physics, but is severely limited by the serious discrete characteristics between grain boundary and nano-units interfaces. Herein, a thermodynamically driven surface reaction and confined crystallization process is reported to synthesize a centimeter-scale supercontinuous ZrO2 nanolayer on ZrO2-SiO2 fiber aerogel surface, which significantly improved its thermal and mechanical properties with density almost unchanged (≈26 mg cm−3). Systematic structure analysis confirms that the supercontinuous layer achieves a close connection between grains and fibers through Zr─O─Si bonds. The as-prepared aerogel exhibits record-breaking specific strength (≈84615 N m kg−1, can support up to ≈227 272 times aerogel mass) and dynamic impact resistance (withstanding impacts up to 500 times aerogel mass and up to 200 cycling stability at 80% strain). Besides, its temperature resistance has also been greatly optimized (400 °C enhancement, stability at 1500 °C). This work will provide a new perspective for exploring the limits of lightweight, high strength, and thermal properties of solid materials.

Light-mediated crosslinkers are incorporated into a polymer-grafted nanoparticle composite system. This method enables >15-fold enhancement of tensile modulus upon crosslinking and can be applied to a wide range of monomer compositions. Furthermore, the regio-selective nature of photocrosslinking allows for the fabrication of compositionally continuous composites with intentionally designed anisotropic mechanical responses, demonstrated via the fabrication of a stiffness-patterned soft electronic substrate.

Polymer-brush-grafted nanoparticles (PGNPs) that can be covalently crosslinked post-processing enable the fabrication of mechanically robust and chemically stable polymer nanocomposites with high inorganic filler content. Modifying PGNP brushes to append UV-activated crosslinkers along the polymer chains would permit a modular crosslinking strategy applicable to a diverse range of nanocomposite compositions. Further, light-activated crosslinking reactions enable spatial control of crosslink density to program intentionally inhomogeneous mechanical responses. Here, a method of synthesizing composites using UV-crosslinkable brush-coated nanoparticles (referred to as UV-XNPs) is introduced that can be applied to various monomer compositions by incorporating photoinitiators into the polymer brushes. UV crosslinking of processed UV-XNP structures can increase their tensile modulus up to 15-fold without any noticeable alteration to their appearance or shape. By using photomasks to alter UV intensity across a sample, intentionally designed inhomogeneities in crosslink density result in predetermined anisotropic shape changes under strain. This unique capability of UV-XNP materials is applied to stiffness-patterned flexible electronic substrates that prevent the delamination of rigid components under deformation. The potential of UV-XNPs as functional, soft device components is further demonstrated by wearable devices that can be modified post-fabrication to customize their performance, permitting the ability to add functionality to existing device architectures.

Recent advances in operando characterizations and computational simulations have unveiled the unconventional and dynamic nature of surface-bound reaction intermediates in aqueous electrochemical systems. By tailoring electronic properties and atomic structures of catalytic surfaces, researchers can manipulate adsorbate dynamics to enable energetically favorable reaction pathways, overcoming the thermodynamic and kinetic constraints inherent in conventional reaction mechanisms.

Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components to tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways and alleviate energy barriers, eliminating conventional thermodynamic constraints and ultimately optimizing energy flow within electrochemical systems. This approach has, therefore, garnered significant interest, presenting substantial potential for developing highly efficient catalysts that simultaneously enhance activity, selectivity, and stability. The immense promise and rapid evolution of this design strategy, however, do not overshadow the substantial challenges and ambiguities that persist, impeding the realization of significant breakthroughs in electrocatalyst development. This review explores the latest insights into the principles guiding the design of catalytic surfaces that enable favorable adsorbate dynamics within the contexts of hydrogen and oxygen electrochemistry. Innovative approaches for tailoring adsorbate-surface interactions are discussed, delving into underlying principles that govern these dynamics. Additionally, perspectives on the prevailing challenges are presented and future research directions are proposed. By evaluating the core principles and identifying critical research gaps, this review seeks to inspire rational electrocatalyst design, the discovery of novel reaction mechanisms and concepts, and ultimately, advance the large-scale implementation of electroconversion technologies.

A new design strategy is introduced to eliminate mutual excitation in stacked scintillator detectors by rare earth ions doped quantum-cutting scintillators with a significant absorption-emission shift as the top layer. The developed detector features non-overlapping optical absorption and RL emission spectra, improving the discrimination of materials with similar densities.

Traditional energy-integration X-ray imaging systems rely on total X-ray intensity for image contrast, ignoring energy-specific information. Recently developed multilayer stacked scintillators have enabled multispectral, large-area flat-panel X-ray imaging (FPXI), enhancing material discrimination capabilities. However, increased layering can lead to mutual excitation, which may affect the accurate discrimination of X-ray energy. This issue is tackled by proposing a novel design strategy utilizing rare earth ions doped quantum-cutting scintillators as the top layer. These scintillators create new luminescence centers via energy transfer, resulting in a significantly larger absorption-emission shift, as well as the potential to double the photoluminescence quantum yield (PLQY) and enhance light output. To verify this concept, a three-layer stacked scintillator detector is developed using ytterbium ions (Yb3+)-doped CsPbCl3 perovskite nanocrystals (PeNCs) as the top layer, which offers a high PLQY of over 100% and a significant absorption-emission shift of 570 nm. This configuration, CsAgCl2 and Cs3Cu2I5 as the middle and bottom layers, respectively, ensures non-overlapping optical absorption and radioluminescence (RL) emission spectra. By calculating the optimal thickness for each layer to absorb specific X-ray energies, the detector demonstrates distinct absorption differences across various energy bands, enhancing the identification of materials with similar densities.

This study reveals the transition of magnetic interlayer coupling in a van der Waals (vdW) magnet driven by an in-plane electrical bias, leading to a significant modulation of magnetoresistance. This finding introduces a novel approach to controlling magnetization through electrical bias for spintronic applications with vdW magnets.

Efficient magnetization control is a central issue in magnetism and spintronics. Particularly, there are increasing demands for manipulation of magnetic states in van der Waals (vdW) magnets with unconventional functionalities. However, the electrically induced phase transition between ferromagnetic-to-antiferromagnetic states without external magnetic field is yet to be demonstrated. Here, the current-induced magnetic phase transition in a vdW ferromagnet Fe5GeTe2 is reported. Based on magneto-transport measurements and theoretical analysis, it is demonstrated that transition in the interlayer magnetic coupling occurs through vertical voltage drop between layers induced by current which is attributed to high anisotropy of the resistivity caused by the vdW gaps. Such magnetic phase transition results in giant modulation of the longitudinal magnetoresistance from 5% to 170%. The electrical tunability of the magnetic phase in Fe5GeTe2 with current-in-plane geometry opens a path for electric control of magnetic properties, expanding the ability to use vdW magnets for spintronic applications.

Silk proteins can be fabricated into large scaffolds with cortical-bone-like lamellar structures through freeze-casting. The resultant freeze-cast scaffolds are made of parallel silk protein lamellae and can be implanted into pig models to achieve effective bone regeneration without side effects.

Assembling natural proteins into large, strong, bone-mimetic scaffolds for repairing bone defects in large-animal load-bearing sites remain elusive. Here this challenge is tackled by assembling pure silk fibroin (SF) into 3D scaffolds with cortical-bone-like lamellae, superior strength, and biodegradability through freeze-casting. The unique lamellae promote the attachment, migration, and proliferation of tissue-regenerative cells (e.g., mesenchymal stem cells [MSCs] and human umbilical vein endothelial cells) around them, and are capable of developing in vitro into cortical-bone organoids with a high number of MSC-derived osteoblasts. High-SF-content lamellar scaffolds, regardless of MSC inoculation, regenerated more bone than non-lamellar or low-SF-content lamellar scaffolds. They accelerated neovascularization by transforming macrophages from M1 to M2 phenotype, promoting bone regeneration to repair large segmental bone defects (LSBD) in minipigs within three months, even without growth factor supplements. The bone regeneration can be further enhanced by controlling the orientation of the lamella to be parallel to the long axis of bone during implantation. This work demonstrates the power of oriented lamellar bone-like protein scaffolds in repairing LSBD in large animal models.

A high-performance Pt/CuO@CF catalyst is designed for the electrocatalytic oxidation of biomass-derived HMF at high concentrations with excellent recyclability. Experimental results and theoretical simulations reveal that Pt modification enhances interfacial active sites, strengthens Pt-CuO coupling, induces charge redistribution, and adjusts the d-band structure. These changes effectively improve the adsorption of reactants and hydroxyl groups, contributing to the highly efficient HMFOR.

Electrochemical oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) provides an environmentally friendly route for producing the sustainable polymer monomer 2,5-furandicarboxylic acid (FDCA). Thus, precisely adjusting the synergistic adsorption among key reactive species, such as HMF and OHads, on the carefully designed catalyst surface is essential for achieving satisfactory catalytic performance for HMF oxidation to FDCA as it is closely related to the adsorption strength and configuration of the reaction substrates. This kind of regulation will ultimately facilitate the improvement of HMF oxidation performance. In this work, Pt nanoparticles modified CuO nanowires (denoted as Pt/CuO@CF) are constructed for the selective electrooxidation of HMF to FDCA under alkaline conditions. The well-designed Pt/CuO@CF demonstrates highly impressive catalytic performance across a range of HMF concentrations, ranging from the commonly used concentrations to higher levels typically not explored (10, 25, 50, 75, and 100 mm) with high FEFDCA (all above 95%) and outstanding long-term stability (15 cycles). In situ experimental characterizations confirm that the designed heterogeneous interface between Pt and CuO enhances the enrichment of HMF and OHads species on the catalyst surface. Theoretical calculations reveal the anchored Pt nanoparticles reduce the adsorption barrier for HMF and OHads, thereby promoting the highly selective oxidation of HMF to FDCA.