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Capitalizing on the extensive spectral capacity and minimal crosstalk properties inherent in optical signals, photoelectric synapses are poised to assume a pivotal stance in the realm of neuromorphic computation. Herein, a photoelectric synapse based on Lewis acid-doped semiconducting tungsten diselenide (WSe 2 ) is introduced, exhibiting tunable short-term and long-term plasticity. The device consumes a mere 0.1 fJ per synaptic operation, which is lower than the energy required by a single synaptic event observed in the human brain. Furthermore, these devices demonstrate high-pass filtering capabilities, highlighting their potential in image-sharpening applications. In particular, by synergistically modulating the photoconductivity and electrical gate bias, versatile logic capabilities are demonstrated within a single device, enabling it to flexibly perform both Boolean AND and OR gate operations. This work demonstrates a viable approach for Lewis acid-treated TMDs to realize multifunctional photoelectric synapses for neuromorphic computing., (© 2024 Wiley‐VCH GmbH.)

The multi-electron transfer I-/IO3- redox couple is attractive for high energy aqueous batteries. Shifting from an acidic to an alkaline electrolyte significantly enhances the IO3- formation kinetics due to the spontaneous disproportionation reaction, while the alkaline environment also offers more favorable Zn anode compatibility. However, sluggish kinetics during the reduction of IO3- persists in both acidic and alkaline electrolytes, compromising the energy efficiency of this glorious redox couple. Here, we establish the fundamental redox mechanism of the I-/IO3- couple in alkaline electrolytes for the first time and propose that Bi/Bi2O3 acts as a redox mediator (RM) to "catalyze" the reduction of IO3-. This mediation significantly reduces the voltage gap between charge/discharge from 1.6 V to 1 V with improved conversion efficiency and rate capability. By pairing the Zn anode and the Bi/Bi2O3 RM cathode, the full battery with I-/IO3- redox mechanism achieves high areal capacity of 12 mAh cm-2 and stable operation at 5 mAh cm-2 for over 400 cycles., (© 2024 Wiley‐VCH GmbH.)

Deep eutectic electrolytes (DEEs) have attracted significant interest due to the unique physiochemical properties, yet challenges persist in achieving satisfactory Li anode compatibility through a binary DEE formula. In this study, we introduce a nonflammable binary DEE electrolyte comprising of lithium bis(trifluoro-methane-sulfonyl)imide (LiTFSI) and solid butadiene sulfone (BdS), which demonstrates enhanced Li metal compatibility while exhibiting high Li + ion migration number (0.52), ionic conductivity (1.48 mS ⋅ cm -1 ), wide electrochemical window (~4.5 V vs. Li/Li + ) at room temperature. Experimental and theoretical results indicate that the Li compatibility derives from the formation of a LiF-rich SEI, attributed to the undesirable adsorption and deformation of BdS on Li surface that facilitates the preferential reactions between LiTFSI and Li metal. This stable SEI effectively suppresses dendrites growth and gas evolution reactions, ensuring a long lifespan and high coulombic efficiency in both the Li||Li symmetric cells, Li||LiCoO 2 and Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells. Moreover, the BdS eutectic strategy exhibit universal applicability to other metal such as Na and Zn by pairing with the corresponding TFSI-based salts., (© 2024 Wiley-VCH GmbH.)

The sluggish kinetics of hydrogen evolution reaction (HER) via water reduction limits the efficiency of alkaline water electrolysis. The HER kinetics is not only intimately related to the catalyst surface structure but also relevant to the cation identity of the electrolyte. The cation dependence also relies on the surface electronic structure and applied potential, but this interrelated effect and its underlying mechanism awaits elucidation. Herein, differently-charged molybdenum sulfide (MoS x ) cluster supports ([Mo 3 S 13 ] 2- and [Mo 3 S 7 ] 4+ ) are utilized to hybridize with the identical metallic Ru centers. The specific electrostatic interaction between MoS x clusters and Ru precursors induces different Ru valences of the hybrids, with a higher valence state for Ru/Mo 3 S 13 endowing a higher activity. The Ru/Mo 3 S 13 and Ru/Mo 3 S 7 exhibited drastically-different cation dependence, in which the charged support determines the local accumulation of cations and resulting water structures. The more negatively-charged Mo 3 S 13 support induces the facile accumulation of cations, especially for less-hydrated K + cations. The water activation capability by Ru valences and cation accumulation from the support effect in-together determine the cation-dependent alkaline HER activity. This work not only enriches the understanding about the cation-dependent HER mechanism but also shines a light on the rational optimization strategy of electrode/electrolyte interfaces., (© 2024 Wiley‐VCH GmbH.)

Solid polymer electrolytes (SPEs) are pivotal in advancing the practical implementation of all-solid-state batteries. Poly(1,3-dioxane) (PDOL)-based electrolytes have attracted significant attention due to the pseudo-high conductivity achieved through sophisticated in situ polymerization methods; however, such PDOL-based electrolytes present challenges of crystallization over time and monomers residual during processing. In this study, integrating LiTFSI and LiDFOB as a universal copolymerization strategy for developing high-performance PDOL electrolytes with a wide range of epoxy crosslinkers is proposed. It is discovered that this approach leverages the protective effects of TFSI anions on the boron active center and catalyzes polymer chain growth via crosslinking. The homogenously crosslinked (benzene-centered) PDOL electrolyte exhibits remarkable thermo-mechanical stability (up to 100 °C), high ion migration number (t Li+ = 0.42), a wide electrochemical window (≈5.0 V vs Li + /Li), and high ionic conductivity (4.5×10 -4 S cm -1 ). Notably, the crosslinked PDOL electrolyte is in the all-solid-state with minimal monomer/oligomer residual, exhibiting no crystallization during relaxation, delivering a robust performance in all-solid-state lithium metal batteries., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

An expanded carbaporphyrinoid analogue, octaphyrin(2,1,1,1,2,1,1,1), containing two rigid diphenylacetylene moieties is reported. In contrast to traditional pyrrolic macrocycles where flexible conformers coexist in dynamic equilibrium, this macrocycle exists as two separable, conformationally stable stereoisomers, denoted as 1A and 1B. The conformational effect of both conformers, as well as their protonated forms, were thoroughly studied using NMR spectroscopy, UV/Vis, and single crystal X-ray diffraction analyses. Importantly, heating conformer 1B leads to its irreversible conversion to 1A, whereas in its protonated form, 1A ⋅ 2MSA undergoes irreversible transformation to 1B ⋅ 2MSA at lower temperatures. These temperature-dependent features establish a foundation for developing new accumulated heat sensors, as demonstrated by the use of the present octaphyrins as a customized thermochromic indicator in steam sterilization. The present study thus underscores how the conformational rigidity of these new polypyrrolic macrocycles imparts properties that are distinct from historically flexible expanded porphyrinoids., (© 2024 Wiley-VCH GmbH.)

The cycling performance of zinc-ion batteries is greatly affected by dendrite formation and side reactions on zinc anode, particularly in scenarios involving high depth of discharge (DOD) and low negative/positive capacity (N/P) ratios in full cells. Herein, drawing upon principles of host-guest interaction chemistry, we investigate the impact of molecular structure of electrolyte additives, specifically the -COOH and -OH groups, on the zinc negative electrode through molecular design. Our findings reveal that molecules containing these groups exhibit strong adsorption onto zinc anode surfaces and chelate with Zn 2+ , forming a H 2 O-poor inner Helmholtz plane. This effectively suppresses side reactions and promotes dendrite-free zinc deposition of exposed (002) facets, enhancing stability and reversibility of an average coulombic efficiency of 99.89 % with the introduction of Lactobionic acid (LA) additive. Under harsh conditions of 92 % DOD, Zn//Zn cells exhibit stable cycling at challenging current densities of 15 mA ⋅ cm -2 . Even at a low N/P ratio of 1.3, Zn//NH 4 V 4 O 10 full cells with LA electrolyte exhibit high-capacity retention of 73 % after 300 cycles, significantly surpassing that of the blank electrolyte. Moreover, in a conversion type Zn//Br static battery with a high areal capacity (~5 mAh ⋅ cm -2 ), LA electrolyte sustains an improved cycling stability of 700 cycles., (© 2024 Wiley-VCH GmbH.)

In the pursuit of high-performance energy storage systems, four-electron zinc-iodine aqueous batteries (4eZIBs) with successive I - /I 2 /I + redox couples are appealing for their potential to deliver high energy density and resource abundance. However, susceptibility of positive valence I + to hydrolysis and instability of Zn plating/stripping in conventional aqueous electrolyte pose significant challenges. In response, polyethylene glycol (PEG 200) is introduced as co-solvent in 2 m ZnCl 2 aqueous solution to design a wide temperature electrolyte. Through a comprehensive investigation combining spectroscopic characterizations and theoretical simulations, it is elucidated that PEG disrupts the intrinsic strong H-bonds of water by global weak PEG-H 2 O interaction, which strengthens the O─H covalent bond of water and intensifies the coordination with Zn 2+ . This synergistic effect substantially reduces water activity to restrain the I + hydrolysis, facilitating I - /I 2 /I + redox kinetics, mitigating I 3 formation and smoothening Zn deposition. The 4eZIBs in the optimized hybrid electrolyte not only deliver superior cyclability with a low fading rate of 0.0009% per cycle over 20 000 cycles and a close-to-unit coulombic efficiency but also exhibit stable performance in a wide temperature range from 40 °C to -40 °C. This study offers valuable insights into the rational design of electrolytes for 4eZIBs.- formation and smoothening Zn deposition. The 4eZIBs in the optimized hybrid electrolyte not only deliver superior cyclability with a low fading rate of 0.0009% per cycle over 20 000 cycles and a close-to-unit coulombic efficiency but also exhibit stable performance in a wide temperature range from 40 °C to -40 °C. This study offers valuable insights into the rational design of electrolytes for 4eZIBs., (© 2024 Wiley‐VCH GmbH.)

Bistable electrochromic (EC) materials and systems offer significant potential for building decarbonization through their optical modulation and energy efficiency. However, challenges such as limited design strategies and bottlenecks in cost, fabrication, and color have hindered the full commercialization of energy-saving EC windows and displays, with few materials achieving true bistability. Herein, a novel strategy for designing bistable electrochromic materials is proposed by leveraging supramolecular interactions. These interactions facilitate reversible color transitions, stabilize the colored structure, and enable spatial confinement to inhibit diffusion, thereby achieving bistable electrochromism. The mechanisms and materials underlying these unconventional electrochromic systems are substantiated through detailed characterization. This strategy enables the preparation of low-cost and sustainable transparent electrochromic displays with high performance. Notably, the display information remains clearly visible for more than 2 h without consuming energy. Involving biomass materials and removable device structures also enhances the sustainability and scalability of EC technology applications and development. These results demonstrate the crucial role of supramolecular chemistry in the development of cutting-edge materials for applications such as energy-saving smart windows., (© 2024 Wiley‐VCH GmbH.)

The directional conversion of methane to ethylene is challenging due to the dissociation of the C─H bond and the self-coupling of methyl intermediates. Herein, a novel W/WO 3- x and W is developed. Impressively, the catalyst achieves an unprecedented C 3- x and W is developed. Impressively, the catalyst achieves an unprecedented C 2 H 4 yield of 1822.73 µmol g -1  h -1 , thus reducing the dissociation energy barrier of the C─H bond. The CH 3- x . Oxygen vacancies provide abundant coordination of unsaturation sites, which promotes the adsorption and activation of CH 4 , thus reducing the dissociation energy barrier of the C─H bond. The CH 2 coupling barrier on the metal W surface is significantly lower compared to WO 3 , so CH 2 can migrate to the W site for coupling. Importantly, the W/WO 3- x with high periodicity provides multiple ordered local microelectric fields, and CH 2 intermediates with dipole moments undergo orientation polarization and displacement polarization driven by the electric field, thus enabling CH 2 migration. This work opens a new avenue for the structural design and modulation of photocatalysts, and provides new perspectives on the migration of methylene between multiple active sites., (© 2024 Wiley‐VCH GmbH.)

Avascular dense connective tissues (e.g., the annulus fibrosus (AF) rupture, the meniscus tear, and tendons and ligaments injury) repair remains a challenge due to the "biological barrier" that hinders traditional drug permeation and limits self-healing of the injured tissue. Here, accurate delivery of nitric oxide (NO) to penetrate the "AF biological barrier" is achieved thereby enabling programmable AF repair. NO-loaded BioMOFs are synthesized and mixed in a modified polyvinyl alcohol and PCL-composited electrospun fiber membrane with excellent reactive oxygen species-responsive capability (LN@PM). The results show that LN@PM could respond to the high oxidative stress environment at the injured tissue and realize continuous and substantial NO release. Based on low molecular weight and lipophilicity, NO could penetrate through the "biological barrier" for accurate AF drug delivery. Moreover, the dynamic characteristics of the LN@PM reaction can be matched with the pathological microenvironment to initiate programmable tissue repair including sequential remodeling microenvironment, reprogramming the immune environment, and finally promoting tissue regeneration. This tailored programmable treatment strategy that matches the pathological repair process significantly repairs AF, ultimately alleviating intervertebral disc degeneration. This study highlights a promising approach for avascular dense connective tissue treatment through intelligent NO release, effectively overcoming "AF biological barriers" and programmable treatment., (© 2024 Wiley‐VCH GmbH.)

Maximizing the loadings of active centers without aggregation for a supported catalyst is a grand challenge but essential for achieving high gravimetric catalytic activity, especially toward multi-step reactions. The oxidation of 5-hydroxymethylfurfural (HMF), a key biomass-derived platform molecule, into 2,5-furandicarboxylic acid (FDCA), a promising alternative to polyester monomer, is such a multi-step reaction that involves 6 proton and electron transfers. This process often demands strong alkaline environment but also suffers from the alkali-driven polymerization side-reaction. Meanwhile, neutral media ameliorates the polymerization, but lacks efficient catalyst toward deep oxidation. Herein, we devised a strategy of creating ultra-dense supported Ru oxide clusters via directed ion exchange in a Co hydroxyanion (CoHA) support material. Pyrimidine ligands were first incorporated into the CoHA interlayers, and the subsequent evacuation of pyrimidines created porous channels for the directed ion exchange with the built-in anions in CoHA, which allowed the dense and mono-disperse functionalization of RuCl 6 anions and their resulting Ru oxide clusters. These ultra-dense Ru oxide clusters not only enable high HMF electrooxidation currents under neutral conditions but also create microscopic channels in-between the clusters for the expedited re-adsorption and oxidation of intermediates toward highly oxidized product, such as 5-formyl-2-furoic acid (FFCA) and FDCA. A two-stage HMF oxidation process, consisting of ambient conversion of HMF into FFCA and FFCA oxidation into FDCA under 60 °C, was eventually developed to first achieve a high FDCA yield of 92.1 % under neutral media with significantly reduced polymerization.2- anions and their resulting Ru oxide clusters. These ultra-dense Ru oxide clusters not only enable high HMF electrooxidation currents under neutral conditions but also create microscopic channels in-between the clusters for the expedited re-adsorption and oxidation of intermediates toward highly oxidized product, such as 5-formyl-2-furoic acid (FFCA) and FDCA. A two-stage HMF oxidation process, consisting of ambient conversion of HMF into FFCA and FFCA oxidation into FDCA under 60 °C, was eventually developed to first achieve a high FDCA yield of 92.1 % under neutral media with significantly reduced polymerization., (© 2024 Wiley-VCH GmbH.)

Aqueous fluoride ion batteries (FIBs) have garnered attention for their high theoretical energy density, yet they are challenged by sluggish fluorination kinetics, active material dissolution, and electrolyte instability. Here, we present a room temperature rocking-chair aqueous FIBs featuring KOAc-KF binary salt electrolytes, enabling concurrent fluorination and defluorination reactions at both cathode and anode electrodes. Experimental and theoretical results reveal that acetate ions in the electrolyte compete with fluoride ions in hydrogen bonding formation, weakening the excessively strong solvation between H 2 O and F - ions. This results in the suppression of detrimental HF formation and a reduced desolvation energy of F - ions, enhancing the electrochemical reaction kinetics. The bismuth-based cathode exhibits direct conversion in the optimized electrolyte, effectively suppressing the detrimental disproportionation reactions from Bi 2+ intermediates. Additionally, zinc anode undergoes a typical fluorination process, forming solid KZnF 3 as the electrode product, minimizing the risks of hydrogen evolution. The proposed aqueous FIBs with the optimized electrolyte demonstrate high discharge capacity, long-term cycling stability and excellent rate capabilities., (© 2024 Wiley‐VCH GmbH.)

Lithium carbonate (Li 2 CO 3 ) plays a crucial role in advancing state-of-the-art lithium-ion batteries (LIBs) for efficient energy storage. The primary source of lithium is lithium-rich brines, which have complex compositions. Conventional extraction processes from brines involve cumbersome methods that often lead to emissions and/or large volumes of wastewater. To address these environmental challenges, a novel and eco-friendly lithium extraction process under ambient pressure is necessary. In this project, we developed an electrolytic process utilizing a NASICON-type solid-state electrolyte (LATP) to extract lithium chloride from low-purity sources at a temperature of 380 °C. To reduce the melting points of the lithium sources, ZnCl 2 was introduced as a fluxing agent. The electrolytic process effectively separated Li + from other coexisting ions, but resulted in their mixture with Zn 2+ . Subsequently, purification and carbonation processes were employed to produce high-purity Li 2 CO 3 (98.9 %). We also obtained high-purity Zn(OH) 2 (>99.9 %) as a value by-product. Despite the formation of color centers that caused the LATP disk to change from white to black during the electrolytic process, it exhibited sufficient ionic conductivity for successful lithium extraction. Our environmentally friendly approach offers a promising pathway for efficient and sustainable lithium extraction, contributing to the advancement of LIB technology for energy storage applications., (© 2024 Wiley-VCH GmbH.)

Proteins capable of switching between distinct active states in response to biochemical cues are ideal for sensing and controlling biological processes. Activatable CRISPR-Cas systems are significant in precise genetic manipulation and sensitive molecular diagnostics, yet directly controlling Cas protein function remains challenging. Herein, we explore anti-CRISPR (Acr) proteins as modules to create synthetic Cas protein switches (CasPSs) based on computational chemistry-directed rational protein interface engineering. Guided by molecular fingerprint analysis, electrostatic potential mapping, and binding free energy calculations, we rationally engineer the molecular interaction interface between Cas12a and its cognate Acr proteins (AcrVA4 and AcrVA5) to generate a series of orthogonal protease-responsive CasPSs. These CasPSs enable the conversion of specific proteolytic events into activation of Cas12a function with high switching ratios (up to 34.3-fold). These advancements enable specific proteolysis-inducible genome editing in mammalian cells and sensitive detection of viral protease activities during virus infection. This work provides a promising strategy for developing CRISPR-Cas tools for controllable gene manipulation and regulation and clinical diagnostics., (© 2024 Wiley‐VCH GmbH.)

Enamel repair is crucial for restoring tooth function and halting dental caries. However, contemporary research often overlooks the retention of organic residues within the repair layer, which hinders the growth of dense crystals and compromises the properties of the repaired enamel. During the maturation of natural enamel, the organic matrix undergoes enzymatic processing to facilitate further crystal growth, resulting in a highly mineralized tissue. Inspired by this process, a biomimetic self-maturation mineralization system is developed, comprising ribonucleic acid-stabilized amorphous calcium phosphate (RNA-ACP) and ribonuclease (RNase). The RNA-ACP induces initial mineralization in the form of epitaxial crystal growth, while the RNase present in saliva automatically triggers a biomimetic self-maturation process. The mechanistic study further indicates that RNA degradation prompts conformational rearrangement of the RNA-ACP, effectively excluding the organic matter introduced earlier. This exclusion process promotes lateral crystal growth, resulting in the generation of denser enamel-like apatite crystals that are devoid of organic residues. This strategy of eliminating organic residues from enamel crystals enhances the mechanical and physiochemical properties of the repaired enamel. The present study introduces a conceptual biomimetic mineralization strategy for effective enamel repair in clinical practice and offers potential insights into the mechanisms of biomineral formation., (© 2024 Wiley‐VCH GmbH.)

Triboelectric nanogenerators (TENGs) have manifested a remarkable potential for harvesting environmental energy and have the prospects to be utilized for various uses, for instance, self-powered sensing devices, flexible wearables, and marine corrosion protection. However, the potential for further development of TENGs is restricted on account of their low output power that in turn is determined by their surface charge density. The current review majorly focuses on the selection and optimization of triboelectric materials. Subsequently, various methods capable of enhancing the surface charge density of TENGs, including environmental regulation, charge excitation, charge pumping, electrostatic breakdown, charge trapping, and liquid-solid structure are comprehensively reviewed. Lastly, the review is concluded by highlighting the existing challenges in enhancing the surface charge density of TENGs and exploring potential opportunities for future research endeavors in this area., (© 2023 Wiley‐VCH GmbH.)

Anthraquinone electrode materials are promising candidates for lithium-ion batteries (LIBs) due to the abundance of anthraquinone and the high theoretical capacity, and good reversibility of the anthraquinone electrodes. However, the active anthraquinone materials are soluble in organic electrolytes, resulting in a sharp decay of capacity during the charge and discharge processes. Herein, we report on a two-dimensional calcium anthraquinone 2,3-dicarboxy metal-organic framework (2D CaAQDC MOF) fabricated using a simple hydrothermal method. The 2D CaAQDC MOF not only effectively inhibits the dissolution of active electrode substances into the electrolyte, but also promotes the diffusion of lithium ion into the pores of the MOF. When used as a cathode for the LIBs, the resulting CaAQDC electrode delivers a high specific capacity of ~100 mAh g -1 at a current density of 50 mA g -1 after 200 cycles, demonstrating its good cycle stability. Even at a high current density of 200 mA g -1 , the CaAQDC electrode exhibits a specific capacity of ~60 mAh g -1 . The fabricated 2D coordination polymers effectively restrains the dissolution of anthraquinone into the organic electrolyte and enhances the structural stability, which greatly improves the electrochemical performance of anthraquinone. These research results offer a rational molecular design strategy to address the dissolution of this and other active organic electrode materials., (© 2024 Wiley-VCH GmbH.)

The stability of aqueous Zn-ion batteries (AZIBs) is detrimentally influenced by the formation of Zn dendrites and the occurrence of parasitic side reactions at the Zn metal anode (ZMA)-electrolyte interface. The strategic manipulation of the preferential crystal orientation during Zn 2+ plating serves as an essential approach to mitigate this issue. Here, Zn aspartate (Zn-Asp), an electrolyte additive for AZIBs, is introduced not only to optimize the solvation structure of Zn 2+ , but also to crucially promote preferential Zn 2+ plating on the (002) crystal plane of ZMA. As a result, both side reactions and Zn dendrites are effectively inhibited, ensuring an anode surface free of both dendrites and by-products. The implementation of Zn-Asp leads to significant enhancements in both Zn||Zn symmetric and Zn||Ti batteries, which demonstrate robust cyclability of over 3200 h and high Coulombic efficiency of 99.29%, respectively. Additionally, the Zn||NaV 3 O 8 ·1.5H 2 O full battery exhibits remarkable rate capability, realizing a high capacity of 240.77 mA h g -1 at 5 A g -1 , and retains 92.7% of its initial capacity after 1000 cycles. This research underscores the vital role of electrolyte additives in regulating the preferential crystal orientation of ZMA, thereby contributing to the development of high-performing AZIBs., (© 2023 Wiley-VCH GmbH.)

Sorbent-based atmospheric water harvesting (AWH) has emerged as a promising decentralized water-production technology to mitigate the freshwater crisis in arid areas. Hydrogels have been regarded as attractive sorbents due to their high water retention and tailorable polymer-water interactions. Yet, the kinetics of water sorption and desorption at low relative humidity (RH) shall be improved for their practical implementation. Here, hygroscopic microgels (HMGs) composed of hydroxypropyl cellulose (HPC) and hygroscopic salt are reported, which achieve a water uptake of ca. 0.5-0.8 g g -1 at 15-30% RH. HMGs enable rapid sorption-desorption kinetics owing to the short-distance diffusion in the microgels and hydrophilicity-hydrophobicity switching of the thermoresponsive HPC. To validate the feasibility of HMGs for moisture extraction, a potential daily water collection of up to equivalent 7.9-19.1 L kg -1 at low RH is demonstrated, enabled by 24-36 operation cycles per day based on the material-level experiments. With renewable raw materials and superior performance, HMGs provide a sustainable approach for rapid moisture extraction in arid climates., (© 2022 Wiley‐VCH GmbH.)

Planar gliding along with anisotropic lattice strain of single-crystalline nickel-rich cathodes (SCNRC) at highly delithiated states will induce severe delamination cracking that seriously deteriorates LIBs' cyclability. To address these issues, a novel lattice-matched MgTiO 3 (MTO) layer, which exhibits same lattice structure as Ni-rich cathodes, is rationally constructed on single-crystalline LiNi 0.9 Co 0.05 Mn 0.05 O 2 (SC90) for ultrastable mechanical integrity. Intensive in/ex situ characterizations combined with theoretical calculations and finite element analysis suggest that the uniform MTO coating layer prevents direct contact between SC90 and organic electrolytes and enables rapid Li-ion diffusion with depressed Li-deficiency, thereby stabilizing the interfacial structure and accommodating the mechanical stress of SC90. More importantly, a superstructure is simultaneously formed in SC90, which can effectively alleviate the anisotropic lattice changes and decrease cation mobility during successive high-voltage de/intercalation processes. Therefore, the as-acquired MTO-modified SC90 cathode displays desirable capacity retention and high-voltage stability. When paired with commercial graphite anodes, the pouch-type cells with the MTO-modified SC90 can deliver a high capacity of 175.2 mAh g -1 with 89.8% capacity retention after 500 cycles. This lattice-matching coating strategy demonstrate a highly effective pathway to maintain the structural and interfacial stability in electrode materials, which can be a pioneering breakthrough in commercialization of Ni-rich cathodes., (© 2023 Wiley-VCH GmbH.)

Hyperuricemia, caused by an imbalance between the rates of production and excretion of uric acid (UA), may greatly increase the mortality rates in patients with cardiovascular and cerebrovascular diseases. Herein, for fast-acting and long-lasting hyperuricemia treatment, armored red blood cell (RBC) biohybrids, integrated RBCs with proximal, cascaded-enzymes of urate oxidase (UOX) and catalase (CAT) encapsulated within ZIF-8 framework-based nanoparticles, have been fabricated based on a super-assembly approach. Each component is crucial for hyperuricemia treatment: 1) RBCs significantly increase the circulation time of nanoparticles; 2) ZIF-8 nanoparticles-based superstructure greatly enhances RBCs resistance against external stressors while preserving native RBC properties (such as oxygen carrying capability); 3) the ZIF-8 scaffold protects the encapsulated enzymes from enzymatic degradation; 4) no physical barrier exists for urate diffusion, and thus allow fast degradation of UA in blood and neutralizes the toxic by-product H 2 O 2 . In vivo results demonstrate that the biohybrids can effectively normalize the UA level of an acute hyperuricemia mouse model within 2 h and possess a longer elimination half-life (49.7 ± 4.9 h). They anticipate that their simple and general method that combines functional nanomaterials with living cell carriers will be a starting point for the development of innovative drug delivery systems., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Chirality is a fundamental characteristic of nature. Expanded porphyrinoids and their analogues offer an attractive platform for delving into the intricacies of chirality. Expanded porphyrinoids comprise pyrrolic macrocycles and related heterocyclic systems. As a class, expanded porphyrinoids are widely recognized for their flexible structural features, nontrivial coordination capabilities, and intriguing optical and electronic properties. With limited exceptions, their inherent conformational flexibility coupled with a low racemization barrier allows for the facile interchange between enantiomers. As a result, achieving the effective chiral resolution of individual enantiomers and the subsequent exploration of their chiroptical properties represents a significant challenge. This review summarizes strategies used to realize the chiral resolution of expanded porphyrinoids and the understanding of intrinsic chiroptical properties that has emerged from these separation efforts. It is our hope that this review will serve not only to codify our current understanding of chiral expanded porphyrinoids, but also inspire advances in the generalized area of chiral functional materials., (© 2023 Wiley-VCH GmbH.)

To make sodium-ion batteries a realistic option for everyday energy storage, a practicable method is to enhance the kinetics of Na + reactions through the development of structurally stable electrode materials. This study utilizes ternary Sn-based dichalcogenide (SnS 1.5 Se 0.5 ) in the design of electrode material to tackle several issues that adversely hinder the performance and longevity of sodium-ion batteries. First, the incorporation of Se into the SnS structure enhances its electrical conductivity and stability. Second, the ternary composition restricts the formation of intermediates during the desodiation/sodiation process, resulting in better electrode reaction reversibility. Finally, SnS 1.5 Se 0.5 lowers the diffusion barrier of Na, thereby facilitating rapid and efficient ion transport within the electrode material. Moreover, nitrogen and sulfur dual-doped carbon (NS-C) is used to enhance surface chemistry and ionic/electrical conductivity of SnS 1.5 Se 0.5 , leading to a pseudocapacitive storage effect that presents a promising potential for high-performance energy storage devices. The study has successfully developed a SnS 1.5 Se 0.5 /NS-C anode, exhibiting remarkable rate capability and cycle stability, retaining a capacity of 647 mAh g -1 even after 10 000 cycles at 5 A g -1 in half-cell tests. In full-cell tests, Na 3 V 2 (PO 4 ) 3 //SnS 1.5 Se 0.5 /NS-C delivers a high energy density of 176.6 Wh kg -1 . In addition, the Na + storage mechanism of SnS 1.5 Se 0.5 /NS-C is explored through ex situ tests and DFT calculations. The findings suggest that the ternary Sn-based dichalcogenides can considerably enhance the performance of the anode, enabling efficient large-scale storage of sodium. These findings hold great promise for the advancement of high-performance energy storage devices for practical applications., (© 2023 Wiley-VCH GmbH.)

The global crisis in antimicrobial resistance continues to grow. Estimating the risks of antibiotic resistance transmission across habitats is hindered by the lack of data on mobility and habitat-specificity. Metagenomic samples of 6092 are analyzed to delineate the unique core resistomes from human feces and seven other habitats. This is found that most resistance genes (≈85%) are transmitted between external habitats and human feces. This suggests that human feces are broadly representative of the global resistome and are potentially a hub for accumulating and disseminating resistance genes. The analysis found that resistance genes with ancient horizontal gene transfer (HGT) events have a higher efficiency of transfer across habitats, suggesting that HGT may be the main driver for forming unique but partly shared resistomes in all habitats. Importantly, the human fecal resistome is historically different and influenced by HGT and age. The most important routes of cross-transmission of resistance are from the atmosphere, buildings, and animals to humans. These habitats should receive more attention for future prevention of antimicrobial resistance. The study will disentangle transmission routes of resistance genes between humans and other habitats in a One Health framework and can identify strategies for controlling the ongoing dissemination and antibiotic resistance., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Neutral water oxidation is a crucial half-reaction for various electrochemical applications requiring pH-benign conditions. However, its sluggish kinetics with limited proton and electron transfer rates greatly impacts the overall energy efficiency. In this work, we created an electrode/electrolyte synergy strategy for simultaneously enhancing the proton and electron transfers at the interface toward highly efficient neutral water oxidation. The charge transfer was accelerated between the iridium oxide and in situ formed nickel oxyhydroxide on the electrode end. The proton transfer was expedited by the compact borate environment that originated from hierarchical fluoride/borate anions on the electrolyte end. These concerted promotions facilitated the proton-coupled electron transfer (PCET) events. Due to the electrode/electrolyte synergy, Ir-O and Ir-OO - intermediates could be directly detected by in situ Raman spectroscopy, and the rate-limiting step of Ir-O oxidation was determined. This synergy strategy can extend the scope of optimizing electrocatalytic activities toward more electrode/electrolyte combinations., (© 2023 Wiley-VCH GmbH.)

High-voltage lithium-ion batteries (LIBs) have attracted great attention due to their promising high energy density. However, severe capacity degradation is witnessed, which originated from the incompatible and unstable electrolyte-electrode interphase at high voltage. Herein, a robust additive-induced sulfur-rich interphase is constructed by introducing an additive with ultrahigh S-content (34.04 %, methylene methyl disulfonate, MMDS) in 4.6 V LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523)||graphite pouch cell. The MMDS does not directly participate the inner Li + sheath, but the strong interactions between MMDS and PF 6 - anions promote the preferential decomposition of MMDS and broaden the oxidation stability, facilitating the formation of an ultrathin but robust sulfur-rich interfacial layer. The electrolyte consumption, gas production, phase transformation and dissolution of transition metal ions were effectively inhibited. As expected, the 4.6 V NCM523||graphite pouch cell delivers a high capacity retention of 87.99 % even after 800 cycles. This work shares new insight into the sulfur-rich additive-induced electrolyte-electrode interphase for stable high-voltage LIBs., (© 2023 Wiley-VCH GmbH.)

Imaging flow cytometry based on optical time-stretch (OTS) imaging combined with a microfluidic chip attracts much attention in the large-scale single-cell analysis due to its high throughput, high precision, and label-free operation. Compressive sensing has been integrated into OTS imaging to relieve the pressure on the sampling and transmission of massive data. However, image decompression brings an extra overhead of computing power to the system, but does not generate additional information. In this work, we propose and demonstrate OTS imaging flow cytometry in the compressed domain. Specifically, we constructed a machine-learning network to analyze the cells without decompressing the images. The results show that our system enables high-quality imaging and high-accurate cell classification with an accuracy of over 99% at a compression ratio of 10%. This work provides a viable solution to the big data problem in OTS imaging flow cytometry, boosting its application in practice., (© 2023 Wiley-VCH GmbH.)

While the structures of Brønsted acid sites (BAS) in zeolites are well understood, those of Lewis acid sites (LAS) remain an active area of investigation. Under hydrated conditions, the reversible formation of framework-associated octahedral aluminum has been observed in zeolites in the acidic form. However, the structure and formation mechanisms are currently unknown. In this work, combined experimental 27 Al NMR spectroscopy and computational data reveal for the first time the details of the zeolite framework-associated octahedral aluminium. The octahedral LAS site becomes kinetically allowed and thermodynamically stable under wet conditions in the presence of multiple nearby BAS sites. The critical condition for the existence of such octahedral LAS appears to be the availability of three protons: at lower proton concentration, either by increasing the Si/Al or by ion-exchange to non-acidic form, the tetrahedral BAS becomes thermodynamically more stable. This work resolves the question about the nature and reversibility of framework-associated octahedral aluminium in zeolites., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

A non-aromatic expanded carbaporphyrinoid, incorporating two built-in 2,7-pyrenylene moieties was synthesized. The intrinsically labile structure was demonstrated by proton-triggered conformational changes between the figure-of-eight and quasi-Möbius conformers. Upon treatment with Pd(OAc) 2 , the reaction produces two bis-Pd II complexes with distinct coordination modes. Metal coordination serves to fix the macrocyclic frameworks with the net result that both bis-Pd II complexes could be resolved by high performance liquid chromatography (HPLC) on a chiral stationary phase. The isolated enantiomers showed persistent chiroptical properties as evidenced by the intense response in the circular dichroism (CD) spectra and the record high absorption dissymmetry factors (g abs of up to 0.038) seen in the near-infrared spectral region. Moreover, the mutual interconversion of these two Pd II complexes was found to be stereospecific and to favor the more stable isomers under weakly acidic conditions., (© 2022 Wiley-VCH GmbH.)

Water scarcity caused by climate change and population growth poses a grave threat to human society. Of the different water purification technologies put forward, one presents a promising strategy that is spatially or temporally non-restricted-atmospheric water harvesting (AWH). Here we review recent progress in the design and study of AWH sorbents, ranging from the innovative chemistries to the integration of sophisticated architectures and functional components, and clarify the structure-property-performance relationship that governs the water capture and release processes. Features and limitations of each type of sorbents are summarized to elucidate the optimal working environments and modes. Progress in applications extending from water generation to thermal management and agriculture are discussed. Future developments regarding material modifications, performance measurements, and system optimizations are provided to overcome lingering barriers to sorbent design and implementation., (© 2022 Wiley-VCH GmbH.)

Mitochondrial dysfunction of cardiomyocytes (CMs) has been identified as a significant pathogenesis of early myocardial infarction (MI). However, only a few agents or strategies have been developed to improve mitochondrial dysfunction for the effective MI treatment. Herein, a reactive oxygen species (ROS)-responsive PAMB-G-TK/4-arm-PEG-SG hydrogel is developed for localized drug-loaded liposome delivery. Notably, the liposomes contain both elamipretide (SS-31) and sphingosine-1-phosphate (S1P), where SS-31 acts as an inhibitor of mitochondrial oxidative damage and S1P as a signaling molecule for activating angiogenesis. Liposome-encapsulated PAMB-G-TK/4-arm-PEG-SG hydrogels demonstrate myocardium-like mechanical strength and electrical conductivity, and ROS-sensitive release of SS-31 and S1P-loaded liposomes. Further liposomal release of SS-31, which can target cytochrome c in the mitochondrial inner membrane of damaged CMs, inhibits pathological ROS production, improving mitochondrial dysfunction. Meanwhile, S1P released from the liposome induces endothelial cell angiogenesis by activating the S1PR1/PI3K/Akt pathway. In a rat MI model, the resulting liposomal composite hydrogel improves cardiac function by scavenging excess ROS, improving mitochondrial dysfunction, and promoting angiogenesis. This study reports for the first time a liposomal composite hydrogel that can directly target mitochondria of damaged CMs for a feedback-regulated release of encapsulated liposomes to consume the overproduced pathological ROS for improved CM activity and enhanced MI treatment., (© 2022 Wiley-VCH GmbH.)

Interfacial solar vapor generation (SVG) is regarded as a promising and sustainable strategy for clean water production. While many materials have demonstrated excellent evaporation rates under one sun, it remains challenging to design solar evaporators without compromising SVG performance in high-salinity brines (≥10 wt %). Herein, polyzwitterionic hydrogels (PZHs) are proposed as a novel platform for high-salinity solar desalination. Taking advantage of the unique anti-polyelectrolyte effects, PZHs can trap salt ions from the brine water to form a more hydrated polymer network, leading to enhanced SVG performance. PZHs exhibit an exceptional solar evaporation rate of 4.14 kg m -2  h -1 in 10 wt % brine, which is ≈20 % higher than that in pure water. It is anticipated that salt-responsive PZHs may provide insights for the design of next-generation solar desalination systems., (© 2022 Wiley-VCH GmbH.)

The ubiquitous nature of atmospheric moisture makes it a significant water resource available at any geographical location. Atmospheric water harvesting (AWH) technology, which extracts moisture from the ambient air to generate clean water, is a promising strategy to realize decentralized water production. The high water uptake by salt-based sorbents makes them attractive for AWH, especially in arid environments. However, they often have relatively high desorption heat, rendering water release an energy-intensive process. A  LiCl-incorporating polyacrylamide hydrogel (PAM-LiCl) capable of effective moisture harvesting from arid environments is proposed. The interactions between the hydrophilic hydrogel network and the captured water generate more free and weakly bonded water, significantly lowering the desorption heat compared with conventional neat salt sorbents. Benefiting from the affinity for swelling of the polymer backbones, the developed PAM-LiCl achieves a high water uptake of ≈1.1 g g -1 at 20% RH with fast sorption kinetics of ≈0.008 g g -1  min -1  and further demonstrates a daily water yield up to ≈7 g g -1 at this condition. These findings provide a new pathway for the synthesis of materials with efficient water absorption/desorption properties, to reach energy-efficient water release for AWH in arid climates., (© 2022 Wiley-VCH GmbH.)

Passivation of the sulfur electrode by insulating lithium sulfide (Li 2 S) restricts the reversibility and sulfur utilization of lithium-sulfur (Li-S) batteries. Although electrolytes with high donor number (DN) solvents induce tri-sulfur radical intermediate thus 3D nucleation of Li 2 S with fast kinetics can be achieved, their catastrophic reactivities with Li metal hinder practical applications. Here, the use of high DN solvent as an additive instead of as co-solvent to solve their incompatibility between cathode and anode is proposed, by adopting N-methyl-2-pyrrolidone (NMP) as a proof-of-concept. Such a strategy is accomplished by the unique solvation structure of the NMP added electrolyte, where the preference of NMP-Li + coordination squeezes out partial 1,2-dimethoxyethane (DME) molecules while enriching 1,3-dioxolane (DOL) molecules in the first solvation sheath of Li + ions. It affords the robust SEI on Li metal from corrosion either by NMP or the dissolved polysulfides. Spectral analyses (Raman and UV-vis) also verify that the coordinated NMP additive preserves its S 3 •- radicals stabilization ability as it does as a co-solvent, which effectively improves the sulfur conversion kinetics and reversibility. This approach enables competitive capacity retention and a stable cycling performance of 340 cycles, which is one of the longest lifespans known for the high DN solvent involved Li-S batteries., (© 2022 Wiley-VCH GmbH.)

Atmospheric water harvesting (AWH) is regarded as one of the promising strategies for freshwater production desirable to provide sustainable water for landlocked and arid regions. Hygroscopic materials have attracted widespread attention because of their water harvesting performance. However, the introduction of many inorganic salts often leads to aggregation and leakage issues in practical use. Here, polyzwitterionic hydrogels are developed as an effective AWH material platform. Via anti-polyelectrolyte effects, the hygroscopic salt coordinated with polymer chains could capture moisture and enhance the swelling property, leading to a strong moisture sorption capacity. The hydrogel shows superior AWH performance (0.62 g g -1 , 120 minutes for equilibrium at 30 % relative humidity) and produces 5.87 L kg -1 freshwater per day. It is anticipated that the polyzwitterionic hydrogels with unique salt-responsive properties could provide new insights into the design and synthesis of next-generation AWH materials., (© 2022 Wiley-VCH GmbH.)

Recently, dendritic mesoporous silica nanoparticles with widespread applications have attracted great interest. Despite many publications (>800), the terminology "dendritic" is ambiguous. Understanding what possible "dendritic structures" are, their formation mechanisms and the underlying structure-property relationship is fundamentally important. With the advance of characterization techniques such as electron tomography, two types of tree-branch-like and flower-like structures can be distinguished, both described as "dendritic" in the literature. In this Review, we start with the definition of "dendritic", then provide critical analysis of reported dendritic silica nanoparticles according to their structural classification. We update the understandings of the formation mechanisms of two types of "dendritic" nanoparticles, highlighting how to control their structural parameters. Applications of dendritic mesoporous nanoparticles are also reviewed with a focus on the biomedical field, providing new insights into the structure-property relationship in this family of nanomaterials., (© 2021 Wiley-VCH GmbH.)

Atmospheric water harvesting (AWH) is emerging as a promising strategy to produce fresh water from abundant airborne moisture to overcome the global clean water shortage. The ubiquitous moisture resources allow AWH to be free from geographical restrictions and potentially realize decentralized applications, making it a vital parallel or supplementary freshwater production approach to liquid water resource-based technologies. Recent advances in regulating chemical properties and micro/nanostructures of moisture-harvesting materials have demonstrated new possibilities to promote enhanced device performance and new understandings. This perspective aims to provide a timely overview on the state-of-the-art materials design and how they serve as the active components in AWH. First, the key processes of AWH, including vapor condensation, droplet nucleation, growth, and departure are outlined, and the desired material properties based on the fundamental mechanisms are discussed. Then, how tailoring materials-water interactions at the molecular level play a vital role in realizing high water uptake and low energy consumption is shown. Last, the challenges and outlook on further improving AWH from material designs and system engineering aspects are highlighted., (© 2022 Wiley-VCH GmbH.)

Microglia modulate pro-inflammatory and neurotoxic activities. Edible plant-derived factors improve brain function. Current knowledge of the molecular interactions between edible plant-derived factors and the microglial cell is limited. Here an alcohol-induced chronic brain inflammation model is used to identify that the microglial cell is the novel target of oat nanoparticles (oatN). Oral administration of oatN inhibits brain inflammation and improves brain memory function of mice that are fed alcohol. Mechanistically, ethanol activates dectin-1 mediated inflammatory pathway. OatN is taken up by microglial cells via β-glucan mediated binding to microglial hippocalcin (HPCA) whereas oatN digalactosyldiacylglycerol (DGDG) prevents assess of oatN β-glucan to dectin-1. Subsequently endocytosed β-glucan/HPCA is recruited in an endosomal recycling compartment (ERC) via interaction with Rab11a. This complex then sequesters the dectin-1 in the ERC in an oatN β-glucan dependent manner and alters the location of dectin-1 from Golgi to early endosomes and lysosomes and increases exportation of dectin-1 into exosomes in an Rab11a dependent manner. Collectively, these cascading actions lead to preventing the activation of the alcoholic induced brain inflammation signing pathway(s). This coordinated assembling of the HPCA/Rab11a/dectin-1 complex by oral administration of oatN may contribute to the prevention of brain inflammation., (© 2021 The Authors. Small published by Wiley-VCH GmbH.)

Osteomyelitis is considered as the most serious bone infection, which can lead to the bone destruction or fatal sepsis. Clinical treatments through frequent antibiotics administration and surgical debridement bring inevitable side effects including drug-resistance and disfigurements. It is urgent to develop an antibiotics-free and rapid strategy to treat osteomyelitis. Herein, a bifunctional sonosensitizer that consists of porphyrin-like Zn single-atom catalysts (g-ZnN 4 ) and MoS 2 quantum dots is developed, which exhibits excellent sonodynamic antibacterial efficiency and osteogenic ability. It is found that the construction of heterogeneous interfaces of g-ZnN 4 -MoS 2 fully activates the adsorbed O 2 due to the increased interface charge transfer, enhanced spin-flip, and reduced activation energy of O 2 . The generated 1 O 2 can kill methicillin-resistant Staphylococcus aureus (MRSA) with an antibacterial efficiency of 99.58% under 20 min of ultrasound (US) irradiation. The Zn single atoms immobilized in g-ZnN 4 can be released steadily in the form of Zn 2+ for 28 days within safe concentration, realizing the great osteoinductive ability of such a sonosensitizer. For the treatment of MRSA-infected osteomyelitis, the inflammation and bone loss can be significantly suppressed through sonodynamic ion therapy. This work provides another strategy for developing high efficiency sonosensitizer through ultrasound interfacial engineering., (© 2021 The Authors. Small published by Wiley-VCH GmbH.)

Vertically aligned structures, which are a series of characteristic conformations with thickness-direction alignment, interconnection, or assembly of filler in polymeric composite materials that can provide remarkable structural performance and advanced anisotropic functions, have attracted considerable attention in recent years. The past two decades have witnessed extensive development with regard to universal fabrication methods, subtle control of morphological features, improvement of functional properties, and superior applications of vertically aligned structures in various fields. However, a systematic review remains to be attempted. The various configurations of vertical structures inspired from biological samples in nature, such as vertically aligned structures with honeycomb, reed, annual ring, radial, and lamellar configurations are summarized here. Additionally, relevant processing methods, which include the transformation of oriented direction, external-field inducement, template method, and 3D printing method, are discussed in detail. The diverse applications in mechanical, thermal, electric, dielectric, electromagnetic, water treatment, and energy fields are also highlighted by providing representative examples. Finally, future opportunities and prospects are listed to identify current issues and potential research directions. It is expected that perspectives on the vertically aligned structures presented here will contribute to the research on advanced multifunctional composites., (© 2021 Wiley-VCH GmbH.)

A pair of meso-unsubstituted expanded carbaporphyrins containing two carbazole moieties were prepared in high isolated yields (82 and 76 %, respectively). The two macrocycles, namely 3 and 4, differ with respect to their substitution at the carbazole N-atoms i. e. by H and i-Bu, respectively. As prepared in their free-base forms, macrocycles 3 and 4 adopt figure-of-eight conformations and are best characterized as 40 π-electron, non-aromatic species possessing a decaphyrin(1.1.0.0.0.1.1.0.0.0) skeleton. Protonation of 3 with either trifluoroacetic acid (TFA) or perchloric acid (HClO 4 ) produces a parallelogram-shaped structure. A similar structure is produced when N-functionalized system 4 is treated with TFA. In contrast, protonation of 4 with HClO 4 leads it to adopt a twisted Möbius strip-like structure in the solid state, thus allowing access to three distinct conformational states as a function of the conditions., (© 2021 Wiley-VCH GmbH.)

Electrically insulating polymers are indispensable for electronic and energy applications, but their poor thermal conduction has increasingly become a bottleneck for high-performance devices. Highly drawn low-dimensional polymeric fibers and thin films can exhibit metallic conductivity. Extending this to bulk materials required by real world applications is prohibitive due to the additional interfacial thermal conduction barriers. It is demonstrated that highly aligned ultrahigh molecular weight polyethylene microfibers can be incorporated into a silicone matrix to yield a fully organic bulk polymer composite with a continuous vertical phonon pathway. This leads to a perpendicular thermal conductivity of 38.27 W m -1 K -1 , at par with metals and two orders of magnitude higher than other bulk organic polymers. Taking further advantage of the mechanical flexibility of the microfibers, the processing method offers the freedom to tailor heat transfer pathways in a macroscopic 3D space. The material/process opens up opportunities for efficient thermal management in high-performance devices., (© 2021 The Authors. Advanced Science published by Wiley-VCH GmbH.)

The direct depletion of lactate accumulated in the tumor microenvironment holds promise for cancer therapy but remains challenging. Herein, we report a one-pot synthesis of openwork@ dendritic mesoporous silica nanoparticles (ODMSNs) to address this problem. ODMSNs self-assembled through a time-resolved lamellar growth mechanism feature an openworked core and a dendritic shell, both constructed by silica nanosheets of ≈3 nm. With a large pore size, high surface area and pore volume, ODMSNs exhibited a high loading capacity (>0.7 g g -1 ) of lactate oxidase (LOX) and enabled intratumoral lactate depletion by >99.9 %, leading to anti-angiogenesis, down-regulation of vascular endothelial growth factor, and increased tumor hypoxia. The latter event facilitates the activation of a co-delivered prodrug for enhancing anti-tumor and anti-metastasis efficacy. This study provides an innovative nano-delivery system and demonstrates the first example of direct lactate-depletion-enabled chemotherapy., (© 2020 Wiley-VCH GmbH.)

There are a large number of zeolites, such as ITH, that cannot be prepared in the aluminosilicate form. Now, the successful synthesis of aluminosilicate ITH zeolite using a simple cationic oligomer as an organic template is presented. Key to the success is that the cationic oligomer has a strong complexation ability with aluminum species combined with a structural directing ability for the ITH structure similar to that of the conventional organic template. The aluminosilicate ITH zeolite has very high crystallinity, nanosheet-like crystal morphology, large surface area, fully four-coordinated Al species, and abundant acidic sites. Methanol-to-propylene (MTP) tests reveal that the Al-ITH zeolite shows much higher selectivity for propylene and longer lifetime than commercial ZSM-5. FCC tests show that Al-ITH zeolite is a good candidate as a shape-selective FCC additive for enhancing propylene and butylene selectivity., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Two giant calix[n]phyrin derivatives namely calix[8]- (4) and calix[16]phyrin (5), involving two and four BF 2 units, respectively, were prepared through the condensation of the bis-naphthobipyrrolylmethene-BF 2 complex (3) with pentafluorobenzaldehyde. Calix[n]phyrins 4 and 5 display extremely high extinction coefficients (3.67 and 4.82×10 5  m -1  cm -1 , respectively) in the near-IR region, which was taken as initial evidence for strong excitonic coupling within these cyclic multi-chromophoric systems. Detailed insights into the effect of excitonic coupling dynamics on the electronic structure and photophysical properties of the macrocycles came from fluorescence, time-correlated single-photon counting (TCSPC) and transient absorption (TA) measurements. Support for these experimental findings came from theoretical studies. Theory and experiment confirmed that the coupling between the excitons depends on the specifics of the calix[n]phyrin structure, not just its size., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Emerging single-atom catalysts (SACs) hold great promise for CO 2 electroreduction (CO 2 ER) , but the design of highly active and cost-efficient SACs is still challenging. Herein, a gas diffusion strategy, along with one-step thermal activation, for fabricating N-doped porous carbon polyhedrons with trace isolated Fe atoms (Fe 1 NC) is developed. The optimized Fe 1 NC/S 1 -1000 with atomic Fe-N 3 sites supported by N-doped graphitic carbons exhibits superior CO 2 ER performance with the CO Faradaic efficiency up to 96% at -0.5 V, turnover frequency of 2225 h -1 , and outstanding stability, outperforming almost all previously reported SACs based on N-doped carbon supported nonprecious metals. The observed excellent CO 2 ER performance is attributed to the greatly enhanced accessibility and intrinsic activity of active centers due to the increased electrochemical surface area through size modulation and the redistribution of doped N species by thermal activation. Experimental observations and theoretical calculations reveal that the Fe-N 3 sites possess balanced adsorption energies of *COOH and *CO intermediates, facilitating CO formation. A universal gas diffusion strategy is used to exclusively yield a series of dimension-controlled carbon-supported SACs with single Fe atoms while a rechargeable Zn-CO 2 battery with Fe 1 NC/S 1 -1000 as cathode is developed to deliver a maximal power density of 0.6 mW cm -2 ., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Polymer-based thermal management materials have many irreplaceable advantages not found in metals or ceramics, such as easy processing, low density, and excellent flexibility. However, their limited thermal conductivity and unsatisfactory resistance to elevated temperatures (<200 °C) still prevent effective heat dissipation during applications with high-temperature conditions or powerful operation. Therefore, herein highly thermoconductive and thermostable polymer nanocomposite films prepared by engineering 1D aramid nanofiber (ANF) with worm-like microscopic morphologies into rigid rod-like structures with 2D boron nitride nanosheets (BNNS) are reported. With no coils or entanglements, the rigid polymer chain enables a well-packed crystalline structure resulting in a 20-fold (or greater) increase in axial thermal conductivity. Additionally, strong interfacial interactions between the weaved ANF rod and the stacked BNNS facilitate efficient heat flux through the 1D/2D configuration. Hence, unprecedented in-plane thermal conductivities as high as 46.7 W m -1 K -1 can be achieved at only 30 wt% BNNS loading, a value of 137% greater than that of a worm-like ANF/BNNS counterpart. Moreover, the thermally stable nanocomposite films with light weight (28.9 W m -1 K -1 /10 3 (kg m -3 )) and high strength (>100 MPa, 450 °C) enable effective thermal management for microelectrodes operating at temperatures beyond 200 °C., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Osteoarthritis (OA) is a common joint degenerative disease that causes pain, joint damage, and dysfunction. External hyaluronic acid (HA) supplement is a common method for the management of osteoarthritis which requires multi-injections. It is demonstrated that biodegradable mesoporous silica nanoparticles successfully deliver an enzyme, hyaluronan synthase type 2 (HAS2), into synoviocytes from the temporomandibular joint (TMJ) and generate endogenous HA with high molecular weights. In a rat TMJ osteoarthritis inflammation model, this strategy promotes endogenous HA production and inhibits the synovial inflammation of OA for more than 3 weeks with one-shot administration. Such nanotherapy also helps repairing the bone defects in a rat OA bone defect model., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Implementing sustainable energy conversion and storage technologies is highly reliant on crucial oxygen electrocatalysis, such as the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). However, the pursuit of low cost, energetic efficient and robust bifunctional catalysts for OER and ORR remains a great challenge. Herein, the novel Na-ion-deficient Na 2-x CoP 2 O 7 catalysts are proposed to efficiently electrocatalyze OER and ORR in alkaline solution. The engineering of Na-ion deficiency can tune the electronic structure of Co, and thus tailor the intrinsically electrocatalytic performance. Among the sodium cobalt phosphate catalysts, the Na 1.95 CoP 2 O 7 (NCPO5) catalyst exhibits the lowest ΔE (E J10,OER -E J-1,ORR ) of only 0.86 V, which favorably outperforms most of the reported non-noble metal catalysts. Moreover, the Na-ion deficiency can stabilize the phase structure and morphology of NCPO5 during the OER and ORR processes. This study highlights the Na-ion deficient Na 2-x CoP 2 O 7 as a promising class of low-cost, highly active and robust bifunctional catalysts for OER and ORR., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)