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Osmotic energy, often referred to as "blue energy", is the energy generated from the mixing of solutions with different salt concentrations, offering a vast, renewable, and environmentally friendly energy resource. The efficacy of osmotic power production considerably relies on the performance of the transmembrane process, which depends on ionic conductivity and the capability to differentiate between positive and negative ions. Recent advancements have led to the development of membrane materials featuring precisely tailored ion transport nanochannels, enabling high-efficiency osmotic energy harvesting. In this review, ion diffusion in confined nanochannels and the rational design and optimization of membrane architecture are explored. Furthermore, structural optimization of the membrane to mitigate transport resistance and the concentration polarization effect for enhancing osmotic energy harvesting is highlighted. Finally, an outlook on the challenges that lie ahead is provided, and the potential applications of osmotic energy conversion are outlined. This review offers a comprehensive viewpoint on the evolving prospects of osmotic energy conversion., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

T-cell immunotherapy offers outstanding advantages in the treatment of various diseases, and with the selection of appropriate targets, efficient disease treatment can be achieved. T-cell immunotherapy has made great progress, but clinical results show that only a small proportion of patients can benefit from T-cell immunotherapy. The extensive mechanistic work outlines a blueprint for using T cells as a new option for immunotherapy, but also presents new challenges, including the balance between different fractions of T cells, the inherent T-cell suppression patterns in the disease microenvironment, the acquired loss of targets, and the decline of T-cell viability. The diversity, flexibility, and intelligence of nanomedicines give them great potential for enhancing T-cell immunotherapy. Here, how T-cell immunotherapy strategies can be adapted with different nanomaterials to enhance therapeutic efficacy is discussed. For two different pathological states, immunosuppression and immune activation, recent advances in nanomedicines for T-cell immunotherapy in diseases such as cancers, rheumatoid arthritis, systemic lupus erythematosus, ulcerative colitis, and diabetes are summarized. With a focus on T-cell immunotherapy, this review highlights the outstanding advantages of nanomedicines in disease treatment, and helps advance one's understanding of the use of nanotechnology to enhance T-cell immunotherapy., (© 2023 Wiley‐VCH GmbH.)

Li-rich Mn-based (LRM) cathode materials, characterized by their high specific capacity (>250 mAh g - ¹) and cost-effectiveness, represent promising candidates for next-generation lithium-ion batteries. However, their commercial application is hindered by rapid capacity degradation and voltage fading, which can be attributed to transition metal migration, lattice oxygen release, and the toxicity of Mn ions to the anode solid electrolyte interphase (SEI). Recently, the application of LRM cathode in all-solid-state batteries (ASSBs) has garnered significant interest, as this approach eliminates the liquid electrolyte, thereby suppressing transition metal crosstalk and solid-liquid interfacial side reactions. This review first examines the historical development, crystal structure, and mechanisms underlying the high capacity of LRM cathode materials. It then introduces the current challenges facing LRM cathode and the associated degradation mechanisms and proposes solutions to these issues. Additionally, it summarizes recent research on LRM materials in ASSBs and suggests strategies for improvement. Finally, the review discusses future research directions for LRM cathode materials, including optimized material design, bulk doping, surface coating, developing novel solid electrolytes, and interface engineering. This review aims to provide further insights and new perspectives on applying LRM cathode materials in ASSBs., (© 2024 Wiley‐VCH GmbH.)

Introducing biological structures into materials design is expected to develop strong and tough structural materials. However, multiple interfaces are introduced simultaneously. They are always the weakest part of load transfer, becoming a critical vulnerability and failure-prone area. Here, it is the first found that the chiton achieves superior mechanical properties just by incorporating a unique sinusoidal interlocking interface into cross-lamellar architecture. These special interlocking interfaces make the chiton shell achieve damage delocalization and increase the resistance to crack initiation and propagation. Meanwhile, this "pre-engineered" path significantly increases the travel path of the cracks and balances the strength and toughness under quasi-static and impact loading. Inspired by this, a novel chiton-inspired composite is proposed. Through coupling the cross-lamellar structures and sinusoidal interlocking interfaces, its strength and toughness are increased by 88% and 107% under quasi-static loading, as well as by 17.8% and 52.4% under impact loading, respectively. These unusual interfaces make up the weak point of cross-lamellar structures and provide insights into the longer evolution of structural materials., (© 2024 Wiley‐VCH GmbH.)

Integrating bioelectronic devices with hard tissues, such as bones and teeth, is essential for advancing diagnostic and therapeutic technologies. However, stable and durable adhesion in dynamic, moist environments remains challenging. Traditional bioadhesives often fail to maintain strong bonds, especially when interfacing with metal electrodes and hard tissues. This study introduces a self-reinforcing ionogel bioadhesive interface (IGBI) combining silk fibroin and calcium ions, designed to provide robust and conductive integration of bioelectronic devices with hard tissues. The IGBI exhibits strong adhesion (up to 186 J m -2 ) and undergoes mechanical self-reinforcement through a structural transition in silk fibroin under physiological conditions. In vivo experiments demonstrate the IGBI's effectiveness in repairing bone defects and reimplanting teeth, with the added capability of wireless, real-time monitoring of bone healing. This approach allows for continuous tracking of tissue regeneration without a second invasive surgery for device removal. The IGBI represents a significant advancement in bioelectronic integration, offering a durable and versatile solution for challenging environments. Such unique self-reinforcing properties make the IGBI a promising material for biomedical applications where traditional adhesives are insufficient., (© 2024 Wiley‐VCH GmbH.)

Suppression of charge recombination caused by unfavorable grain boundaries (GBs) in polycrystalline thin films is essential for improving the optoelectronic performance of semiconductor devices. For emerging antimony selenide (Sb 2 Se 3 ) materials, the unique quasi-1D structure intensifies the dependence of GB properties on the grain size and orientation, which also increases the impact of defects related to grain structure on device performance. However, these characteristics pose significant challenges in the preparation of thin films. In this study, a novel annealing approach using ammonia-thiourea is developed mixed solution as the liquid medium (LM) to finely regulate the crystallization of Sb 2 Se 3 films, resulting in micron-sized large grains with enhanced [hk1] orientation and fewer defects. Mechanistic studies indicate that the intermediate phase formed at the GBs promotes the growth of large grains. Moreover, LM creates a closed and uniform environment for thin-film annealing, suppressing the volatilization of Se and reducing the types of deep-level defects. Consequently, the film delivers a device efficiency of 9.28%, the highest efficiency achieved for Sb 2 Se 3 solar cells fabricated via thermal evaporation. Hence, this study provides a facile and effective annealing method for controlling the crystallization of low-dimensional materials and offers valuable guidance for the development of chalcogenide materials., (© 2024 Wiley‐VCH GmbH.)

Solid sodium metal batteries (SSMBs) offer an alternative promising power source for electrochemical energy storage due to their high energy density and high safety. However, the inherent sodium dendrite growth and poor mechanical properties of electrolytes seriously limit their application. Herein, a network structure composed of polyethylene oxide-based composite polymer electrolyte (CPE) is designed with liquid metal nanoparticles (LM) for SSMBs, in which LM can move in the solid electrolyte with the electric field driven. This effect can facilitate the inactivated sodium return to the metal sodium anode, and alloy with dendrites at the same time, which is beneficial for inhibiting the growth of dendrites. The symmetric cell with the CPE containing LM achieves good cyclic stability of more than 1800 and 800 h at 0.1 and 0.2 mA cm -2 , respectively. The energy density of the pouch battery can reach 230 Wh kg -1 . In sum, LM presents great potential to be employed as a performance reinforcement filler for CPEs, which paves the way for achieving high-performance SSMBs., (© 2024 Wiley‐VCH GmbH.)

The development of sodium metal batteries has long been impeded by dendrite formation issues. State-of-the-art strategies, exemplified by sodiophilic hosting/seeding layers, have demonstrated great success in suppressing dendrite formation. However, addressing high-capacity applications (>10 mAh cm -2 ) remains a significant challenge. Herein, the study revisits the interlayer strategy by simply covering a carbon nanotube (CNT) film onto the surface of a sodium metal anode, unlocking its overlooked potential for ultrahigh capacity applications. In situ Raman spectroscopy reveals the interlayer's fast-ion-storage feature, enabling deposition at the interface without capacity limitations. Consequently, in symmetric cells, one-year long-term reversible cycling and a record-high capacity of 50 mAh cm -2 under 90% depth of discharge is achieved, representing a significant breakthrough for stabilizing Na anode. Furthermore, the full cell with a 50-µm thin metal anode and a high-loading Na 3 V 2 (PO 4 ) 3 cathode (12 mg cm -2 ) delivers a stable capacity of 94 mAh g -1 for 270 cycles (94% capacity retention)., (© 2024 Wiley‐VCH GmbH.)

Electrolyte additives are investigated to resolve dendrite growth, hydrogen evolution reaction, and corrosion of Zn metal. In particular, the electrostatic shielding cationic strategy is considered an effective method to regulate deposition morphology. However, it is very difficult for such a simple cationic modification to avoid competitive hydrogen evolution reactions, corrosion, and interfacial pH fluctuations. Herein, multifunctional additives of potassium hydrogen phthalate (KHP) based on the synergistic design of cationic shielding and anionic chemistry for ultrastable Zn||I 2 full batteries are demonstrated. K cations, acting as electrostatic shielding cations, constructed the smooth deposition morphology. HP anions can enter the first solvation shell of Zn 2+ for the reduced activities of H 2 O, while they remain in the primary solvation shell and are finally involved in the formation of SEI, thus accelerating the charge transfer kinetics. Furthermore, by in situ monitoring the near-surface pH of the Zn electrode, the KHP additives can effectively inhibit the accumulation of OH - and the formation of by-products. Consequently, the symmetric cells achieve a high stripping-plating reversibility of over 4500 and 2600 h at 1.0 and 5 mA cm -2 , respectively. The Zn||I 2 full cells deliver an ultralong term stability of over 1400 cycles with a high-capacity retention of 78.5%., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Flexible electronics are integral in numerous domains such as wearables, healthcare, physiological monitoring, human-machine interface, and environmental sensing, owing to their inherent flexibility, stretchability, lightweight construction, and low profile. These systems seamlessly conform to curvilinear surfaces, including skin, organs, plants, robots, and marine species, facilitating optimal contact. This capability enables flexible electronic systems to enhance or even supplant the utilization of cumbersome instrumentation across a broad range of monitoring and actuation tasks. Consequently, significant progress has been realized in the development of flexible electronic systems. This study begins by examining the key components of standalone flexible electronic systems-sensors, front-end circuitry, data management, power management and actuators. The next section explores different integration strategies for flexible electronic systems as well as their recent advancements. Flexible hybrid electronics, which is currently the most widely used strategy, is first reviewed to assess their characteristics and applications. Subsequently, transformational electronics, which achieves compact and high-density system integration by leveraging heterogeneous integration of bare-die components, is highlighted as the next era of flexible electronic systems. Finally, the study concludes by suggesting future research directions and outlining critical considerations and challenges for developing and miniaturizing fully integrated standalone flexible electronic systems., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

A dodecahedral activated N-doped porous carbon scaffold is synthesized and used for the nanoconfinement of Mg(BH 4 ) 2 . The optimized mesoporous scaffold possesses an accumulated pore width of 2.65 nm, high specific surface area (3955.9 m 2  g -1 ), and large pore volume (2.15 cm 3  g -1 ), providing ample space for the confinement of Mg(BH 4 ) 2 particles and numerous surface active sites for interactions with the same. The confined Mg(BH 4 ) 2 system features a dehydrogenation onset temperature of 81.5 °C, an extremely high capacity of 10.2 wt% H 2 , and an almost single-step dehydrogenation profile. Moreover, the system exhibits superior capacity retention of 82.7% after 20 cycles at a moderate temperature of 250 °C. Precise activation control enables a transformation from microporous carbon materials to mesoporous ones, and hence the efficient nanoconfinement of Mg(BH 4 ) 2 and realization of one-step dehydrogenation. The evolution of borohydride intermediates is systematically revealed throughout the cycling process. Density functional theory calculations demonstrate defective N heteroatoms within the scaffold are vital in reducing the strength of B─H bonds, and the N-doped carbon can facilitate decomposition of the irreversible MgB 12 H 12 intermediate. This study opens up new avenues for designing robust carbon scaffolds doped with heteroatoms and analyzing intermediate evolution in nanoconfined Mg-based borohydride systems., (© 2024 Wiley‐VCH GmbH.)

The development of superconducting materials has attracted significant attention not only for their improved performance, such as high transition temperature (T C ), but also for the exploration of their underlying physical mechanisms. Recently, considerable efforts have been focused on interfaces of materials, a distinct category capable of inducing superconductivity at non-superconducting material interfaces or augmenting the T C at the interface between a superconducting material and a non-superconducting material. Here, two distinct types of interfaces along with their unique characteristics are reviewed: interfacial superconductivity and interface-enhanced superconductivity, with a focus on the crucial factors and potential mechanisms responsible for enhancing superconducting performance. A series of materials systems is discussed, encompassing both historical developments and recent progress from the perspectives of technical innovations and the exploration of new material classes. The overarching goal is to illuminate pathways toward achieving high T C , expanding the potential of superconducting parameters across interfaces, and propelling superconductivity research toward practical, high-temperature applications., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Over the last decade, carbon-based metal-free electrocatalysts (C-MFECs) have become important in electrocatalysis. This field is started thanks to the initial discovery that nitrogen atom doped carbon can function as a metal-free electrode in alkaline fuel cells. A wide variety of metal-free carbon nanomaterials, including 0D carbon dots, 1D carbon nanotubes, 2D graphene, and 3D porous carbons, has demonstrated high electrocatalytic performance across a variety of applications. These include clean energy generation and storage, green chemistry, and environmental remediation. The wide applicability of C-MFECs is facilitated by effective synthetic approaches, e.g., heteroatom doping, and physical/chemical modification. These methods enable the creation of catalysts with electrocatalytic properties useful for sustainable energy transformation and storage (e.g., fuel cells, Zn-air batteries, Li-O 2 batteries, dye-sensitized solar cells), green chemical production (e.g., H 2 O 2 , NH 3 , and urea), and environmental remediation (e.g., wastewater treatment, and CO 2 conversion). Furthermore, significant advances in the theoretical study of C-MFECs via advanced computational modeling and machine learning techniques have been achieved, revealing the charge transfer mechanism for rational design and development of highly efficient catalysts. This review offers a timely overview of recent progress in the development of C-MFECs, addressing material syntheses, theoretical advances, potential applications, challenges and future directions., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Since wearable technologies for telemedicine have emerged to tackle global health concerns, the demand for well-attested wearable healthcare devices with high user comfort also arises. Skin-wearables for health monitoring require mechanical flexibility and stretchability for not only high compatibility with the skin's dynamic nature but also a robust collection of fine health signals from within. Stretchable electrical interconnects, which determine the device's overall integrity, are one of the fundamental units being understated in wearable bioelectronics. In this review, a broad class of materials and engineering methodologies recently researched and developed are presented, and their respective attributes, limitations, and opportunities in designing stretchable interconnects for wearable bioelectronics are offered. Specifically, the electrical and mechanical characteristics of various materials (metals, polymers, carbons, and their composites) are highlighted, along with their compatibility with diverse geometric configurations. Detailed insights into fabrication techniques that are compatible with soft substrates are also provided. Importantly, successful examples of establishing reliable interfacial connections between soft and rigid elements using novel interconnects are reviewed. Lastly, some perspectives and prospects of remaining research challenges and potential pathways for practical utilization of interconnects in wearables are laid out., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

The incorporation of functionalized nanofillers into polymers via photopolymerization approach has gained significant attention in recent years due to the unique properties of the resulting composite materials. Surface modification of nanofillers plays a crucial role in their compatibility and polymerization behavior within the polymer matrix during photopolymerization. This review focuses on the recent developments in surface modification of various nanofillers, enabling their integration into polymer systems through photopolymerization. The review discusses the key aspects of surface modification of nanofillers, including the selection of suitable surface modifiers, such as photoinitiators and polymerizable groups, as well as the optimization of modification conditions to achieve desired surface properties. The influence of surface modification on the interfacial interactions between nanofillers and the polymer matrix is also explored, as it directly impacts the final properties of the nanocomposites. Furthermore, the review highlights the applications of nanocomposites prepared by photopolymerization, such as sensors, gas separation membranes, purification systems, optical devices, and biomedical materials. By providing a comprehensive overview of the surface modification strategies and their impact on the photopolymerization process and the resulting nanocomposite properties, this review aims to inspire new research directions and innovative ideas in the development of high-performance polymer nanocomposites for diverse applications., (© 2024 Wiley‐VCH GmbH.)

Layered iron/manganese-based oxides are a class of promising cathode materials for sustainable batteries due to their high energy densities and earth abundance. However, the stabilization of cationic and anionic redox reactions in these cathodes during cycling at high voltage remain elusive. Here, an electrochemically/thermally stable P2-Na 0.67 Fe 0.3 Mn 0.5 Mg 0.1 Ti 0.1 O 2 cathode material with zero critical elements is designed for sodium-ion batteries (NIBs) to realize a highly reversible capacity of ≈210 mAh g -1 at 20 mA g -1 and good cycling stability with a capacity retention of 74% after 300 cycles at 200 mA g -1 , even when operated with a high charge cut-off voltage of 4.5 V versus sodium metal. Combining a suite of cutting-edge characterizations and computational modeling, it is shown that Mg/Ti co-doping leads to stabilized surface/bulk structure at high voltage and high temperature, and more importantly, enhances cationic/anionic redox reaction reversibility over extended cycles with the suppression of other undesired oxygen activities. This work fundamentally deepens the failure mechanism of Fe/Mn-based layered cathodes and highlights the importance of dopant engineering to achieve high-energy and earth-abundant cathode material for sustainable and long-lasting NIBs., (© 2024 UChicago Argonne, LLC, Operator of Argonne National Laboratory and University of California, Operator of Lawrence Berkeley National Laboratory and The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

The precise manipulation of the microstructure (pore size, free volume distribution, and connectivity of the free-volume elements), thickness, and mechanical characteristics of membranes holds paramount significance in facilitating the effective utilization of self-standing membranes. In this contribution, the synthesis of two innovative ester-linked covalent-organic framework (COF) membranes is first reported, which are generated through the selection of plant-derived ellagic acid and quercetin phenolic monomers in conjunction with terephthaloyl chloride as a building block. The optimization of the microstructure of these two COF membranes is systematically achieved through the application of three different interfacial electric field systems: electric neutrality, positive electricity, and negative electricity. It is observed that the positively charged system facilitates a record increase in the rate of membrane formation, resulting in a denser membrane with a uniform pore size and enhanced flexibility. In addition, a correlation is identified wherein an increase in the alkyl chain length of the surfactants leads to a more uniform pore size and a decrease in the molecular weight cutoff of the COF membrane. The resulting COF membrane exhibits an unprecedented combination of high water permeance, superior sieving capability, robust mechanical strength, chemical robustness for promising membrane-based separation science and technology., (© 2024 Wiley‐VCH GmbH.)

Solid polymer electrolytes (SPEs) for lithium metal batteries have garnered considerable interests owing to their low cost, flexibility, lightweight, and favorable interfacial compatibility with battery electrodes. Their soft mechanical nature compared to solid inorganic electrolytes give them a large advantage to be used in low pressure solid-state lithium metal batteries, which can avoid the cost and weight of the pressure cages. However, the application of SPEs is hindered by their relatively low ionic conductivity. In addressing this limitation, enormous efforts are devoted to the experimental investigation and theoretical calculations/simulation of new polymer classes. Recently, metal-organic frameworks (MOFs) have been shown to be effective in enhancing ion transport in SPEs. However, the mechanisms in enhancing Li + conductivity have rarely been systematically and comprehensively analyzed. Therefore, this review provides an in-depth summary of the mechanisms of MOF-enhanced Li + transport in MOF-based solid polymer electrolytes (MSPEs) in terms of polymer, MOF, MOF/polymer interface, and solid electrolyte interface aspects, respectively. Moreover, the understanding of Li + conduction mechanisms through employing advanced characterization tools, theoretical calculations, and simulations are also reviewed in this review. Finally, the main challenges in developing MSPEs are deeply analyzed and the corresponding future research directions are also proposed., (© 2024 Wiley‐VCH GmbH.)

Perovskite solar cells (PSCs) are developed rapidly in efficiency and stability in recent years, which can compete with silicon solar cells. However, an important obstacle to the commercialization of PSCs is the toxicity of lead ions (Pb 2+ ) from water-soluble perovskites. The entry of free Pb 2+ into organisms can cause severe harm to humans, such as blood lead poisoning, organ failure, etc. Therefore, this work reports a "lead isolation-capture" dual detoxification strategy with calcium disodium edetate (EDTA Na-Ca), which can inhibit lead leakage from PSCs under extreme conditions. More importantly, leaked lead exists in a nontoxic aggregation state chelated by EDTA. For the first time, in vivo experiments are conducted in mice to systematically prove that this material has a significant inhibitory effect on the toxicity of perovskites. In addition, this strategy can further enhance device performance, enabling the optimized devices to achieve an impressive power conversion efficiency (PCE) of 25.19%. This innovative strategy is a major breakthrough in the research on the prevention of lead toxicity in PSCs., (© 2024 Wiley‐VCH GmbH.)

Lithium-ion batteries (LIBs), in which lithium ions function as charge carriers, are considered the most competitive energy storage devices due to their high energy and power density. However, battery materials, especially with high capacity undergo side reactions and changes that result in capacity decay and safety issues. A deep understanding of the reactions that cause changes in the battery's internal components and the mechanisms of those reactions is needed to build safer and better batteries. This review focuses on the processes of battery failures, with voltage and temperature as the underlying factors. Voltage-induced failures result from anode interfacial reactions, current collector corrosion, cathode interfacial reactions, overcharge, and over-discharge, while temperature-induced failure mechanisms include SEI decomposition, separator damage, and interfacial reactions between electrodes and electrolytes. The review also presents protective strategies for controlling these reactions. As a result, the reader is offered a comprehensive overview of the safety features and failure mechanisms of various LIB components., (© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)

Linearly interlinked single atoms offer unprecedented physiochemical properties, but their synthesis for practical applications still poses significant challenges. Herein, linearly interlinked iron single-atom catalysts that are loaded onto interconnected carbon channels as cathodic sulfur hosts for room-temperature sodium-sulfur batteries are presented. The interlinked iron single-atom exhibits unique metallic iron bonds that facilitate the transfer of electrons to the sulfur cathode, thereby accelerating the reaction kinetics. Additionally, the columnated and interlinked carbon channels ensure rapid Na + diffusion kinetics to support high-rate battery reactions. By combining the iron atomic chains and the topological carbon channels, the resulting sulfur cathodes demonstrate effective high-rate conversion performance while maintaining excellent stability. Remarkably, even after 5000 cycles at a current density of 10 A g -1 , the Na-S battery retains a capacity of 325 mAh g -1 . This work can open a new avenue in the design of catalysts and carbon ionic channels, paving the way to achieve sustainable and high-performance energy devices., (© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)

Red phosphorus (P) as an anode material of potassium-ion batteries possesses ultra-high theoretical specific capacity (1154 mAh g -1 ). However, owing to residual white P during the preparation and sluggish kinetics of K-P alloying limit its practical application. Seeking an efficient catalyst to address the above problems is crucial for the secure preparation of red P anode with high performance. Herein, through the analysis of the activation energies in white P polymerization, it is revealed that the highest occupied molecular orbital energy of I 2 (-7.40 eV) is in proximity to P 4 (-7.25 eV), and the lowest unoccupied molecular orbital energy of I 2 molecule (-4.20 eV) is lower than that of other common non-metallic molecules (N 2 , S 8 , Se 8 , F 2 , Cl 2 , Br 2 ). The introduction of I 2 can thus promote the breaking of the P─P bond and accelerate the polymerization of white P molecules. Besides, the ab initio molecular dynamics simulations show that I 2 can enhance the kinetics of P-K alloying. The as-obtained red P/C composites with I 2 deliver excellent cycling stability (358 mAh g -1 after 1200 cycles at 1 A g -1 ). This study establishes catalysis as a promising pathway to tackle the challenges of P anode for alkali metal ion batteries., (© 2023 Wiley-VCH GmbH.)

In silicon heterojunction solar cell technology, thin layers of hydrogenated amorphous silicon (a-Si:H) are applied as passivating contacts to the crystalline silicon (c-Si) wafer. Thus, the properties of the a-Si:H is crucial for the performance of the solar cells. One important property of a-Si:H is its microstructure which can be characterized by the microstructure parameter R based on Si─H bond stretching vibrations. A common method to determine R is Fourier transform infrared (FTIR) absorption measurement which, however, is difficult to perform on solar cells for various reasons like the use of textured Si wafers and the presence of conducting oxide contact layers. Here, it is demonstrated that Raman spectroscopy is suitable to determine the microstructure of bulk a-Si:H layers of 10 nm or less on textured c-Si underneath indium tin oxide as conducting oxide. A detailed comparison of FTIR and Raman spectra is performed and significant differences in the microstructure parameter are obtained by both methods with decreasing a-Si:H film thickness., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Several thermally activated delayed fluorescence (TADF) materials have been studied and developed to realize high-performance organic light-emitting diodes (OLEDs). However, TADF macrocycles have not been sufficiently investigated owing to the synthetic challenges, resulting in limited exploration of their luminescent properties and the corresponding highly efficient OLEDs. In this study, a series of TADF macrocycles is synthesized using a modularly tunable strategy by introducing xanthones as acceptors and phenylamine derivatives as donors. A detailed analysis of their photophysical properties combined with fragment molecules reveals characteristics of high-performance macrocycles. The results indicate that: a) the ideal structure decreases the energy loss, which in turn reduces the non-radiative transitions; b) reasonable building blocks increase the oscillator strength providing a higher radiation transition rate; c) the horizontal dipole orientation (Θ) of the extended macrocyclic emitters is increased. Owing to the high photoluminescence quantum yields of ≈100% and 92% and excellent Θ of 80 and 79% for macrocycles MC-X and MC-XT in 5 wt% doped films, the corresponding devices exhibit record-high external quantum efficiencies of 31.6% and 26.9%, respectively, in the field of TADF macrocycles., (© 2023 Wiley-VCH GmbH.)

Environmentally friendly electrochemical reduction of contaminated nitrate to ammonia (NO 3 - RR) is a promising solution for large quantity ammonia (NH 3 ) production, which, however, is a complex multi-reaction process involving coordination between different reaction intermediates of nitrate reduction and water decomposition-provided active hydrogen (H ads ) species. Here, a dual-site catalyst of [W-O] group-doped CoP nanosheets (0.6W-O-CoP@NF) has been designed to synergistically catalyze the NO 3 - RR and water decomposition, especially the reactions between the intermediates of NO 3 - RR and water decomposition-provided H ads species. This catalytic NO 3 - RR exhibits an extremely high NH 3 yield of 80.92 mg h -1 cm -2 and a Faradaic efficiency (FE) of 95.2% in 1 m KOH containing 0.1 m NO 3 - . Significantly, 0.6W-O-CoP@NF presents greatly enhanced NH 3 yield and FE in a wide NO 3 - concentration ranges of 0.001-0.1 m compared to the reported. The excellent NO 3 - RR performance is attributed to a synergistic catalytic effect between [W-O] and CoP active sites, in which the doped [W-O] group promotes the water decomposition to supply abundant H ads , and meanwhile modulates the electronic structure of Co for strengthened adsorption of H ads and the hydrogen (H 2 ) release prevention, resultantly facilitating the NO 3 - RR. Finally, a Zn-NO 3 - battery has been assembled to simultaneously achieve three functions: electricity output, ammonia production, and nitrate treatment in wastewater., (© 2023 Wiley-VCH GmbH.)

Organic solid electrolytes offer an effective route for safe and high-energy-density all-solid-state Li metal batteries. However, it remains a challenge to devise a new strategy to promote the dissociation of strong ion pairs and the transport of ionic components in organic solid electrolytes. Herein, a zwitterionic covalent organic framework (Zwitt-COF) with well-defined chemical and pore structures is prepared as a solid electrolyte capable of accelerating the dissociation and transport of Li ions. The Zwitt-COF solid electrolyte exhibits a high room-temperature ionic conductivity of 1.65 × 10 -4  S cm -1 with a wide electrochemical stability window. Besides, the Zwitt-COF solid electrolyte displays stable Li plating/stripping behavior via effective inhibition of the formation of Li dendrites and dead Li, leading to superior long-term cycle performance with retention of 99% discharge capacity and 98% Coulombic efficiency in an all-solid-state Li-metal battery. Theoretical simulations reveal that the incorporation of zwitterionic groups into COF can facilitate the dissociation of strong ion pairs and reconstruct the AA-stacking configuration by dissociative adsorption of Li + ions on Zwitt-COF producing linear hexagonal ion channels in the Zwitt-COF solid electrolyte. This strategy based on Zwitt-COF can provide an alternative way to construct various solid-state Li batteries., (© 2023 Wiley-VCH GmbH.)

Fabricating solution-processible host material for thermally activated delayed fluorescence (TADF) emitter remains a formidable challenge for organic light-emitting diodes (OLEDs). In this work, two new host materials, namely 3CzAcPy and 9CzAcPy, are found to exhibit high triplet energy levels, high thermal stability, and excellent film morphology from a solution process. An in-depth analysis on the photophysical data and device performance reveals the isomeric effect of the host materials has a significant impact not only on the host properties, but also on the host-dopant interactions and thus the performance of the resulting solution-processed TADF OLEDs. Impressively, the new hosts are proven to be suitable for both donor-acceptor type and multi-resonance TADF emitters, achieving state-of-the-art device performance. By using the new host 9CzAcPy, solution-processed OLED based on a donor-acceptor TADF emitter of DPAC-PCN, a maximum external quantum efficiency (EQE) of 29.5% is achieved, and solution-processed narrowband OLED based on a multiple-resonance TADF emitter of BN-CP1 acquires a maximum EQE of 26.6%. These efficiencies represent the highest values among the solution-processed TADF OLEDs. This study highlights the significance of host-dopant interactions in modulating the electroluminescence performance of TADF emitters, and provides an effective design principle for solution-processible host materials., (© 2023 Wiley-VCH GmbH.)

Dual-ion batteries (DIBs) have been attracting great attention for the storage of stationary energy due to their low cost, environmental friendliness, and high working voltage. However, most reports on DIBs involve low-mass-loading electrodes (<2.5 mg), while the use of high mass-loading electrodes (>10 mg cm -2 ), which are critical for practical application, is overlooked. Herein, an integrated free-standing functional carbon positive electrode (named MSCG) with a "point-line-plane" hierarchical architecture at the practical level of ultrahigh mass-loading (>50 mg cm -2 ) is developed for high-energy-density DIBs. The rationally designed microstructure and the advanced assembly method that is adopted produce a well-interconnected ion/electron transport channel in the MSCG electrode, which confers rapid ion/electron kinetic properties while maintaining good mechanical properties. Consequently, the DIBs with ultrahigh-mass-loading MSCG electrodes exhibits a high discharge capacity of 100.5 mAh g -1 at 0.5 C (loading mass of 50 mg cm -2 ) and a long-term cycling performance with a capacity retention of 87.7% at 1 C after 500 cycles (loading mass of 23 mg cm -2 ). Moreover, the DIB with the ultrahigh-mass-loading positive electrode achieves a high energy density of 379 Wh kg -1 based on the mass of electrode materials, the highest value recorded to date for any DIBs., (© 2023 Wiley-VCH GmbH.)

Ferroelectric materials have been intensively investigated for high-performance nonvolatile memory devices in the past decades, owing to their nonvolatile polarization characteristics. Ferroelectric memory devices are expected to exhibit lower power consumption and higher speed than conventional memory devices. However, non-complementary metal-oxide-semiconductor (CMOS) compatibility and degradation due to fatigue of traditional perovskite-based ferroelectric materials have hindered the development of high-density and high-performance ferroelectric memories in the past. The recently developed hafnia-based ferroelectric materials have attracted immense attention in the development of advanced semiconductor devices. Because hafnia is typically used in CMOS processes, it can be directly incorporated into current semiconductor technologies. Additionally, hafnia-based ferroelectrics show high scalability and large coercive fields that are advantageous for high-density memory devices. This review summarizes the recent developments in ferroelectric devices, especially ferroelectric transistors, for next-generation memory and neuromorphic applications. First, the types of ferroelectric memories and their operation mechanisms are reviewed. Then, issues limiting the realization of high-performance ferroelectric transistors and possible solutions are discussed. The experimental demonstration of ferroelectric transistor arrays, including 3D ferroelectric NAND and its operation characteristics, are also reviewed. Finally, challenges and strategies toward the development of next-generation memory and neuromorphic applications based on ferroelectric transistors are outlined., (© 2023 Wiley-VCH GmbH.)

As equally essential as the synthesis of new materials, maneuvering new structure configurations can endow the brand-new functional properties to existing materials, which is also one of the core goals in the synthesis community. In this respect, pressure-induced emission (PIE) that triggers photoluminescence (PL) in nonemission materials is an emerging stimuli-responsive smart materials technology. In the PIE paradigms, harvesting bright PL at ambient conditions, however, has remained elusive. Herein, a remarkable PIE phenomenon is reported in initially nonemission Zn(BDC)(DMF)(H 2 O) (MOF-2), which shows bright blue-emission at 455 nm under pressure. Intriguingly, the bright blue PL with an excellent photoluminescence quantum yield up to 70.4% is unprecedentedly retained to ambient conditions upon decompression from 16.2 GPa. The detailed structural analyses combined with density functional theory calculations reveal that hydrogen bonding cooperativity effect elevates powerfully the rotational barrier of the linker rotor to 3.87 eV mol -1 from initial 0.91 eV mol -1 through pressure treatment. The downgrade rotational freedom turns on PL of MOF-2 after releasing pressure completely. This is the first case of harvesting PIE to ambient conditions. These findings offer a new platform for the creation of promising alternatives to high-performance PL materials based on initially nonemission counterparts., (© 2023 Wiley-VCH GmbH.)

In spite of recent research progress in red thermally activated delayed fluorescence (TADF) emitters, highly efficient solution-processable pure red TADF emitters are rarely reported. Most of the red TADF emitters reported to date are designed using a rigid acceptor unit which renders them insoluble and unsuitable for solution-processed organic light-emitting diodes (OLEDs). To resolve this issue, a novel TADF emitter, 6,7-bis(4-(bis(4-(tert-butyl)phenyl)amino)phenyl)-2,3-bis(4-(tert-butyl)phenyl)quinoxaline-5,8-dicarbonitrile (tBuTPA-CNQx) is designed and synthesized. The highly twisted donor-acceptor architecture and appropriate highest occupied molecular orbital/lowest unoccupied molecular orbital distribution lead to a very small singlet-triplet energy gap of 0.07 eV, high photoluminescence quantum yield of 92%, and short delayed fluorescence lifetime of 52.4 µs. The peripheral t-butyl phenyl decorated quinoxaline acceptor unit and t-butyl protected triphenylamine donor unit are proven to be useful building blocks to improve solubility and minimize the intermolecular interaction. The solution-processed OLED based on tBuTPA-CNQx achieves a high external quantum efficiency (EQE) of 16.7% with a pure red emission peak at 662 nm, which is one of the highest EQE values reported till date in the solution-processed pure red TADF OLEDs. Additionally, vacuum-processable OLED based on tBuTPA-CNQx exhibits a high EQE of 22.2% and negligible efficiency roll-off., (© 2023 Wiley-VCH GmbH.)

Ni-rich layered oxides are at the forefront of the development of high-energy Li-ion batteries, yet the extensive applications are retarded by the deteriorative capacity and thermal instability. Herein, an in situ co-precipitation strategy is implemented to achieve the novel super-dispersed Nb-doped Ni-rich cathode that consists of the elongated and radially aligned primary particles with increased oxygen stable {001} planes. The unique microstructure homogenizes the intragranular and intergranular strain distribution and stabilizes the spherical secondary particles, effectively inhibiting microcrack formation and propagation and surface degradation. The super-dispersed Nb doping prevents the Li/Ni disordering and lattice oxygen escape, thereby further strengthening the crystal structure and thermal stability. Accordingly, this cathode delivers a high reversible capacity of 229.0 mAh g -1 at 0.1 C with much better retention at 55 °C and 5 C after 100 cycles than the conventional Nb-doped Ni-rich cathodes. In a pouch-type full cell, it exhibits exceptionally long life with a capacity retention of 91.9% at 1 C after 500 cycles and 80.5% at 5 C after 2000 cycles within 3.0-4.2 V, greatly prolonging the service period to cater to the lightweight and intelligence of electric vehicles., (© 2022 Wiley-VCH GmbH.)

A phosphorus anode is a promising option for energy-storage applications because of its high theoretical specific capacity and safe lithiation potential. However, the multiphase phosphorus lithiation/delithiation reactions and soluble reaction intermediates cause sluggish reaction kinetics and loss of active materials. Herein, a novel local electric field (LEF) strategy is proposed to inhibit the intermediates dissolution and promote the reaction kinetics by optimizing ionic covalent organic frameworks (iCOFs). Among them, the LEF induced by the cationic covalent organic framework effectively enhances the electrochemical performance of the phosphorus anode. The strong electrostatic interaction between the polyphosphides and cationic covalent organic framework confines the dissolution of active materials and tailors the electronic structure of polyphosphides to accelerate the reaction kinetics. The cationic covalent-organic-framework-assisted phosphorus anode provides a high capacity of 1227.8 mAh g -1 at 10.4 A g -1 (8.6 C) and a high-capacity retention of 87% after 500 cycles at 1.3 A g -1 . This work not only broadens the application of iCOFs for phosphorus anode but also inspires the great potential of the local electric field in battery technology., (© 2022 Wiley-VCH GmbH.)

Sb 2 S 3 as a light-harvesting material has attracted great attention for applications in both single-junction and tandem solar cells. Such solar cell has been faced with current challenge of low power conversion efficiency (PCE), which has stagnated for 8 years. It has been recognized that the synthesis of high-quality absorber film plays a critical role in efficiency improvement. Here, using fresh precursor materials for antimony (antimony potassium tartrate) and combined sulfur (sodium thiosulfate and thioacetamide), a unique chemical bath deposition procedure is created. Due to the complexation of sodium thiosulfate and the advantageous hydrolysis cooperation between these two sulfur sources, the heterogeneous nucleation and the S 2- releasing processes are boosted. As a result, there are noticeable improvements in the deposition rate, film morphology, crystallinity, and preferred orientations. Additionally, the improved film quality efficiently lowers charge trapping capacity, suppresses carrier recombination, and prolongs carrier lifetimes, leading to significantly improved photoelectric properties. Ultimately, the PCE exceeds 8% for the first time since 2014, representing the highest efficiency in all kinds of Sb 2 S 3 solar cells to date. This study is expected to shed new light on the fabrication of high-quality Sb 2 S 3 film and further efficiency improvement in Sb 2 S 3 solar cells., (© 2022 Wiley-VCH GmbH.)

The primary roles of precision medicine are to perform real-time examination, administer on-demand medication, and apply instruments continuously. However, most current therapeutic systems implement these processes separately, leading to treatment interruption and limited recovery in patients. Personalized healthcare and smart medical treatment have greatly promoted research on and development of biosensing and drug-delivery integrated systems, with intelligent wearable medical devices (IWMDs) as typical systems, which have received increasing attention because of their non-invasive and customizable nature. Here, the latest progress in research on IWMDs is reviewed, including their mechanisms of integrating biosensing and on-demand drug delivery. The current challenges and future development directions of IWMDs are also discussed., (© 2022 Wiley-VCH GmbH.)

The design of defects and porous structures into metallene with functional surfaces is highly desired to improve its permeability, surface area, and active sites, but remains a great challenge. In this work, polyallylamine-encapsulated Ir metallene with defects and porous structure (Ir@PAH metallene) is easily fabricated by a one-step wet chemical reduction method. The Ir@PAH metallene exhibits excellent hydrogen evolution reaction (HER) performance with an overpotential of only 14 mV at 10 mA cm -2 , a low Tafel slope of 31.2 mV dec -1 , and almost no activity decay after stability test. The abundant defects and pores as well as several-atomic-layer nanosheet structures of Ir@PAH metallene provide a large specific surface area, high conductivity, and efficient mass transport/diffusion. In addition, surface-functionalized PAH molecules can modulate the electronic structure through strong Ir-N interaction and act as proton carriers to capture hydrogen ions, which is very beneficial for the HER in acidic media. This work provides a useful strategy for the synthesis of the defective and porous metallene with functionalized surfaces for various catalytic applications., (© 2022 Wiley-VCH GmbH.)

The human cutaneous sensory organ is a highly evolved biosensor that is efficient, sensitive, selective, and adaptable. Recently, with the development of various materials and structures inspired by sensory organs, artificial cutaneous sensors have been widely studied. In this study, the acquisition of biophysical signals is demonstrated at one point on the body using a wearable all-gel-integrated multimodal sensor composed of four element sensors, inspired by the slow/rapid adapting functions of the skin sensory receptors. The gel-type sensors ensure flexibility, compactness, portability, adherence, and integrity. The wearable all-gel multimodal sensor is easily attached to the wrist and simultaneously gathers blood pressure (BP), electrocardiogram (ECG), electromyogram (EMG), and mechanomyogram (MMG) signals related to cardiac and muscle health. Human activity causes muscle contraction, which affects blood flow; therefore, the relationship between the muscle and heart is crucial for screening and predicting heart health. Cardiac health is monitored by obtaining the two types of phase time differences (i.e., Δt be : BP and ECG, Δt em : ECG and MMG) generated during muscle movement. The suggested multimodal sensor has potential applicability in monitoring biophysical conditions and diagnosing cardiac-related health problems., (© 2022 Wiley-VCH GmbH.)

Increasing the energy density and long-term cycling stability of lithium-ion batteries necessitates the stability of electrolytes under high/low voltage application and stable electrode/electrolyte interfacial contact. However, neither a single polymer nor liquid electrolyte can realize this due to their limited internal energy gap, which cannot avoid lithium-metal deposition and electrolyte oxidation simultaneously. Herein, a novel type of quasi-double-layer composite polymer electrolytes (QDL-CPEs) is proposed by using plasticizers with high oxidation stability (propylene carbonate) and high reduction stability (diethylene glycol dimethyl ether) in a poly(vinylidene fluoride) (PVDF)-based electrolyte composites. In-situ-polymerized propylene carbonate can function as a cathode electrolyte interface (CEI) film, which can enhance the antioxidant ability. The nucleophilic substitution reaction between diethylene glycol dimethyl ether and PVDF increases the reduction stability of the electrolyte on the anodic side, without the formation of lithium dendrites. The QDL-CPEs has high ionic conductivity, an enhanced electrochemical reaction window, adjustable electrode/electrolyte interphases, and no additional electrolyte-electrolyte interfacial resistance. Thus, this ingenious design of the QDL-CPEs improves the cycling performance of a fabricated LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)//QDL-CPEs//hard carbon full cell at room temperature, paving a new way for designing solid-state battery systems accessible for practical applications., (© 2022 Wiley-VCH GmbH.)

Owing to their outstanding comprehensive performance, polyimide (PI) composite films are widely used on the external surfaces of spacecraft to protect them from the adverse conditions of low Earth orbit (LEO). However, current PI composite films have inadequate mechanical properties and atomic oxygen (AO) resistance. Herein, this work fabricates a new PI-based nanocomposite film with greatly enhanced mechanical properties and AO resistance by integrating mica nanosheets with PI into a unique double-layer nacre-inspired structure with a much higher density of mica nanosheets in the top layer. In addition, the unique microstructure and the intrinsic properties of mica also impart the nanocomposite film with favorable ultraviolet and high-temperature resistance. The comprehensive performance of this material is superior to those of pure PI, single-layer PI-mica, and previously reported PI-based composite films. Thus, the double-layer nanocomposite film displays great potential as an aerospace material for use in LEO., (© 2021 Wiley-VCH GmbH.)

The worldwide energy demand in electric vehicles and the increasing global temperature have called for development of high-energy and long-life lithium-ion batteries (LIBs) with improved high-temperature operational resiliency. However, current attention has been mostly focused on cycling aging at elevated temperature, leaving considerable gaps of knowledge in the failure mechanism, and practical control of abusive calendar aging and thermal runaway that are highly related to the eventual operational lifetime and safety performance of LIBs. Herein, using a combination of various in situ synchrotron X-ray and electron microscopy techniques, a multiscale understanding of surface structure effects involved in regulating the high-temperature operational tolerance of polycrystalline Ni-rich layered cathodes is reported. The results collectively show that an ultraconformal poly(3,4-ethylenedioxythiophene) coating can effectively prevent a LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode from undergoing undesired phase transformation and transition metal dissolution on the surface, atomic displacement, and dislocations within primary particles, intergranular cracking along the grain boundaries within secondary particles, and intensive bulk oxygen release during high state-of-charge and high-temperature aging. The present work highlights the essential role of surface structure controls in overcoming the multiscale degradation pathways of high-energy battery materials at extreme temperature., (© 2021 Wiley-VCH GmbH.)

Biomaterials is an exciting and dynamic field, which uses a collection of diverse materials to achieve desired biological responses. While there is constant evolution and innovation in materials with time, biomaterials research has been hampered by the relatively long development period required. In recent years, driven by the need to accelerate materials development, the applications of machine learning in materials science has progressed in leaps and bounds. The combination of machine learning with high-throughput theoretical predictions and high-throughput experiments (HTE) has shifted the traditional Edisonian (trial and error) paradigm to a data-driven paradigm. In this review, each type of biomaterial and their key properties and use cases are systematically discussed, followed by how machine learning can be applied in the development and design process. The discussions are classified according to various types of materials used including polymers, metals, ceramics, and nanomaterials, and implants using additive manufacturing. Last, the current gaps and potential of machine learning to further aid biomaterials discovery and application are also discussed., (© 2021 Wiley-VCH GmbH.)

Lithium metal is one of the most promising anode candidates for next-generation high-energy batteries. Nevertheless, lithium pulverization and associated loss of electrical contact remain significant challenges. Here, an antipulverization and high-continuity lithium metal anode comprising a small number of solid-state electrolyte (SSE) nanoparticles as conformal/sacrificial fillers and a copper (Cu) foil as the supporting current collector is reported. Guiding by the SSE, this new anode facilitates lithium nucleation, contributing to form a roundly shaped, micro-sized, and dendrite-free electrode during cycling, which effectively mitigates the lithium dendrite growth. The embedded Cu current collector in the hybrid anode not only reinforces the mechanical strength but also improves the efficient charge transfer among active lithium filaments, affording good electrode structural integrity and electrical continuity. As a result, this antipulverization and high-continuity lithium anode delivers a high average Coulombic efficiency of ≈99.6% for 300 cycles under a current density of 1 mA cm -2 . Lithium-sulfur batteries (elemental sulfur or sulfurized polyacrylonitrile cathodes) equipped with this anode show high-capacity retentions in their corresponding ether-based or carbonate-based electrolytes, respectively. This new electrode provides important insight into the design of electrodes that may experience large volume variation during operations., (© 2021 Wiley-VCH GmbH.)

Soft ferroelectrics based on organic and organic-inorganic hybrid materials have gained much interest among researchers owing to their electrically programmable and remnant polarization. This allows for the development of numerous flexible, foldable, and stretchable nonvolatile memories, when combined with various crystal engineering approaches to optimize their performance. Soft ferroelectrics have been recently considered to have an important role in the emerging human-connected electronics that involve diverse photoelectronic elements, particularly those requiring precise programmable electric fields, such as tactile sensors, synaptic devices, displays, photodetectors, and solar cells for facile human-machine interaction, human safety, and sustainability. This paper provides a comprehensive review of the recent developments in soft ferroelectric materials with an emphasis on their ferroelectric switching principles and their potential application in human-connected intelligent electronics. Based on the origins of ferroelectric atomic and/or molecular switching, the soft ferroelectrics are categorized into seven subgroups. In this review, the efficiency of soft ferroelectrics with their distinct ferroelectric characteristics utilized in various human-connected electronic devices with programmable electric field is demonstrated. This review inspires further research to utilize the remarkable functionality of soft electronics., (© 2020 Wiley-VCH GmbH.)

Biochemical sensing probes based on aggregation-induced-emission luminogens (AIEgens) are widely used in biological imaging and therapy, chemical sensing, and material sciences. However, it is still a great challenge to quantify the targets through fluorescence intensity of AIEgen probes due to their undesirable aggregations. Here, a PyTPA-ZGO probe with three lifetime signals for precise quantification of furin is constructed: the lifetime signal 1 and signal 2 comes from AIEgen PyTPA-P (τ Pn ) and inorganic nanoparticles Zn 2 GeO 4 :Mn 2+ -NH 2 (τ Zn ), respectively, while the lifetime signal 3 is marked as the composite dual-lifetime signal (CDLS n , C D L S n = τ Z n τ P n ). In contrast, the fluorescence intensity signal of PyTPA-P shows defectively quantitative performance. Furthermore, it is found that the CDLS n exhibits higher significant differences than the two other lifetime signals (τ Pn and τ Zn ) thanks to its wide range between the maximum and minimum signal values and small standard deviation. Therefore, CDLS n is further used to accurately identify cell subtypes based on the specific concentration of furin in each subtype. The lifetime criterion can realize precise quantification, and it should be a promising direction of AIEgen-based quantitative analysis in the future., (© 2021 Wiley-VCH GmbH.)

Ultrathin 2D metal nanostructures have sparked a lot of research interest because of their improved electrocatalytic properties for fuel cells. So far, no effective technique for preparing ultrathin 2D Pd-based metal nanostructures with more than three compositions has been published. Herein, a new visible-light-induced template technique for producing PdAuBiTe alloyed 2D ultrathin nanosheets is developed. The mass activity of the PdAuBiTe nanosheets against the oxygen reduction reaction (ORR) is 2.48 A mg Pd -1 , which is 27.5/17.7 times that of industrial Pd/C/Pt/C, respectively. After 10 000 potential cyclings, there is no decrease in ORR activity. The PdAuBiTe nanosheets exhibit high methanol tolerance and in situ anti-CO poisoning properties. The PdAuBiTe nanosheets, as cathode electrocatalysts in direct methanol fuel cells, can thus give significant improvement in terms of power density and durability. In O 2 /air, the power density can be increased to 235.7/173.5 mW cm -2 , higher than that reported in previous work, and which is 2.32/3.59 times higher than Pt/C., (© 2021 Wiley-VCH GmbH.)

The electrochemical method of combining N 2 and H 2 O to produce ammonia (i.e., the electrochemical nitrogen reduction reaction [E-NRR]) continues to draw attention as it is both environmentally friendly and well suited for a progressively distributed farm economy. Despite the multitude of recent works on the E-NRR, further progress in this field faces a bottleneck. On the one hand, despite the extensive exploration and trial-and-error evaluation of E-NRR catalysts, no study has stood out to become the stage protagonist. On the other hand, the current level of ammonia production (microgram-scale) is an almost insurmountable obstacle for its qualitative and quantitative determination, hindering the discrimination between true activity and contamination. Herein i) the popular theory and mechanism of the NRR are introduced; ii) a comprehensive summary of the recent progress in the field of the E-NRR and related catalysts is provided; iii) the operational procedures of the E-NRR are addressed, including the acquisition of key metrics, the challenges faced, and the most suitable solutions; iv) the guiding principles and standardized recommendations for the E-NRR are emphasized and future research directions and prospects are provided., (© 2021 Wiley-VCH GmbH.)

Immunotherapy that can activate immunity or enhance the immunogenicity of tumors has emerged as one of the most effective methods for cancer therapy. Nevertheless, single-mode immunotherapy is still confronted with several critical challenges, such as the low immune response, the low tumor infiltration, and the complex immunosuppression tumor microenvironment. Recently, the combination of immunotherapy with other therapeutic modalities has emerged as a powerful strategy to augment the therapeutic outcome in fighting against cancer. In this review, recent research advances of the combination of immunotherapy with chemotherapy, phototherapy, radiotherapy, sonodynamic therapy, metabolic therapy, and microwave thermotherapy are summarized. Critical challenges and future research direction of immunotherapy-based cancer therapeutic strategy are also discussed., (© 2021 Wiley-VCH GmbH.)

Unevenly distributed magnesium (Mg) electrodeposits have emerged as a major obstacle for Mg-metal batteries. A comprehensive design matrix is reported for 3D magnesiophilic hosts, which regulate the uniform Mg electrodeposition through a synergistic coupling of homogenizing current distribution, geometric confinement, and chemisorptive interaction. Vertically aligned nitrogen- and oxygen-doped carbon nanofiber arrays on carbon cloth (denoted as "VNCA@C") are developed as a proof of concept. The evenly arranged short nanoarray architecture helps to homogenize the surface current density and the microchannels built in this 3D host allow the preferential nucleation of Mg due to their geometrical confinement effect. Besides, the nitrogen-/oxygen-doped carbon species exhibit strong chemisorptive interaction toward Mg atoms, providing preferential nucleation sites as demonstrated by first-principle calculation results. Electrochemical analysis reveals a peculiar yet highly reversible microchannel-filling growth behavior of Mg metals, which empowers the delicately designed VNCA@C host with the ability to deliver a reduced nucleation overpotential of 429 mV at 10.0 mA cm -2 and an elongated Mg plating/stripping cycle life (110 cycles) under high current density of 10.0 mA cm -2 . The proposed design matrix can be extended to other metal anodes (such as lithium and zinc) for high-energy-density batteries., (© 2021 Wiley-VCH GmbH.)

The growing enthusiasm for cancer immunotherapies and adoptive cell therapies has prompted increasing interest in biomaterials development mimicking natural antigen-presenting cells (APCs) for T-cell expansion. In contrast to conventional bottom-up approaches aimed at layering synthetic substrates with T-cell activation cues, transformation of live dendritic cells (DCs) into artificial APCs (aAPCs) is demonstrated herein using a facile and minimally disruptive hydrogelation technique. Through direct intracellular permeation of poly(ethylene glycol) diacrylate (PEG-DA) hydrogel monomer and UV-activated radical polymerization, intracellular hydrogelation is rapidly accomplished on DCs with minimal influence on cellular morphology and surface antigen display, yielding highly robust and modular cell-gel hybrid constructs amenable to peptide antigen exchange, storable by freezing and lyophilization, and functionalizable with cytokine-releasing carriers for T-cell modulation. The DC-derived aAPCs are shown to induce prolonged T-cell expansion and improve anticancer efficacy of adoptive T-cell therapy in mice compared to nonexpanded control T cells, and the gelation technique is further demonstrated to stabilize primary DCs derived from human donors. The work presents a versatile approach for generating a new class of cell-mimicking biomaterials and opens new venues for immunological interrogation and immunoengineering., (© 2021 Wiley-VCH GmbH.)

Two new orange-red thermally activated delayed fluorescence (TADF) materials, PzTDBA and PzDBA, are reported. These materials are designed based on the acceptor-donor-acceptor (A-D-A) configuration, containing rigid boron acceptors and dihydrophenazine donor moieties. These materials exhibit a small ΔE ST of 0.05-0.06 eV, photoluminescence quantum yield (PLQY) as high as near unity, and short delayed exciton lifetime (τ d ) of less than 2.63 µs in 5 wt% doped film. Further, these materials show a high reverse intersystem crossing rate (k risc ) on the order of 10 6 s -1 . The TADF devices fabricated with 5 wt% PzTDBA and PzDBA as emitting dopants show maximum EQE of 30.3% and 21.8% with extremely low roll-off of 3.6% and 3.2% at 1000 cd m -2 and electroluminescence (EL) maxima at 576 nm and 595 nm, respectively. The low roll-off character of these materials is analyzed by using a roll-off model and the exciton annihilation quenching rates are found to be suppressed by the fast k risc and short delayed exciton lifetime. These devices show operating device lifetimes (LT 50 ) of 159 and 193 h at 1000 cd m -2 for PzTDBA and PzDBA, respectively. The high efficiency and low roll-off of these materials are attributed to the good electronic properties originatng from the A-D-A molecular configuration., (© 2021 Wiley-VCH GmbH.)