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The chemical instability of traditional organically-decorated superhydrophobic metal surfaces is a significant issue, severely limiting practical applications. This is due to the susceptibility of low surface energy coatings to ion permeation, decomposition, and exfoliation, especially in harsh environments. Here, organic coating-free, durable superhydrophobic surfaces on Al alloys by developing the paracrystalline state of a bionic anthill tribe structure is successfully achieved, using femtosecond laser element-doping microstructuring followed by repetitive annealing processes. Remarkably, the inherent superhydrophobic properties of the sample are maintained for ≈2000 h in a corrosive 3.5 wt.% NaCl aqueous solution, significantly surpassing the performance of traditional organic coatings. Moreover, this inherent superhydrophobicity remains nearly unchanged, even after rigorous electrochemical reaction measurements. Additional tests involving UV irradiation (>100 h), freezing cycles (>100 cycles), and acid/alkali resistance (>65 h) further demonstrate that the environmental adaptability of the surface far exceeds that of silane-coated surfaces. Ab initio calculations reveal that the formation of the paracrystalline state reduces surface energy and enhances chemical stability, thereby extending the durability of the superhydrophobic metal. These findings offer a powerful strategy for utilizing atomic-level structural rearrangements to design inherent superhydrophobic surfaces without the need for organic coatings., (© 2024 Wiley‐VCH GmbH.)

Redox-active covalent organic frameworks (COFs) have been demonstrated as promising organic electrodes in many electrochemical devices. However, their inherently low conductivity significantly hinders the full utilization of their internal redox-active sites. To address this issue, a simple solvothermal method is used to in situ polymerize 2,4,6-triformylphloroglucinol (TP) and p-phenylenediamine (PA) on the surface of carbon nanotubes (CNTs), generating a nanocable-like COF-based nanocomposite, TpPa-COF@CNT nanocables, which contain abundant β-ketoenamine groups. By combining the high specific surface area and dense active sites of COFs with the superior conductivity of CNTs, the TpPa-COF@CNT nanocables as the anode in potassium-ion batteries displayed excellent performance. The reason is that the isomerization between the enolic and keto forms reinforces the stability of molecular architecture, while the transformation of active sites from C=N to C=O improves the K+ adsorption capability. Notably, the TpPa-COF@CNT nanocable anode exhibits a high reversible capacity of 446.1 mAh g-1 at 0.1 A g-1 and maintains 282.5 mAh g-1 even after 2000 cycles at a higher current density of 2.0 A g-1. Additionally, a full battery assembled with 3,4,9,10-Perylenetetracarboxylic dianhydride heat-treated at 450 °C as the cathode retains a reversible capacity of 273.6 mAh g-1 after 200 cycles at 0.1 A g-1., (© 2024 Wiley‐VCH GmbH.)

Paclitaxel (PTX) is a first-line chemotherapeutic drug for non-small cell lung cancer (NSCLC) but it can induce indoleamine 2,3-dioxygenase (IDO) activation, which severely lowers down its immuno-chemotherapeutic effect. To address this issue, a smart peptide hydrogelator Nap-Phe-Phe-Phe-Lys-Ser-Thr-Gly-Gly-Lys-Ala-Pro-Arg-OH (Nap-T), which co-assembles with PTX and an IDO inhibitor GDC0919 to form a hydrogel GP@Gel Nap-T, is rationally designed. Upon specific phosphorylation by pyruvate kinase M2 (PKM2), an overexpressed biomarker of NSCLC, Nap-T is gradually converted to Nap-Phe-Phe-Phe-Lys-Ser-Thr(H 2 PO 3 )-Gly-Gly-Lys-Ala-Pro-Arg-OH (Nap-Tp), leading to dehydrogelation and sustained release of PTX and GDC0919 within NSCLC tissues. The released PTX exerts chemotherapy on NSCLC cells as well as immunogenic cell death induction, while GDC0919 promotes the immuno-chemotherapeutic effect of PTX through IDO inhibition. We find that GP@Gel Nap-T enhances the infiltration of tumor-infiltrating immune cells and reduces the number of immunosuppressive cells in either tumor tissues or tumor-draining lymph nodes, thus enhancing the immuno-chemotherapy of PTX toward NSCLC. With this PKM2-responsive drug release strategy, the smart peptide hydrogel platform might be applied for NSCLC treatment in clinic in near future., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Zero-dimensional (0D) hybrid metal halides have been emerged as room-temperature phosphorescence (RTP) materials, but synchronous optimization of multiple phosphorescence performance in one structural platform remains less resolved, and stable RTP activity in aqueous medium is also unrealized due to serious instability toward water and oxygen. Herein, we demonstrated a photophysical tuning strategy in a new 0D hybrid zinc halide family of (BTPP) 2 ZnX 4 (BTPP=benzyltriphenylphosphonium, X=Cl and Br). Infrequently, the delicate combination of organic and inorganic species enables this family to display multiple ultralong green afterglow and efficient self-trapped exciton (STE) associated cyan phosphorescence. Compared with inert luminescence of [BTPP] + cation, incorporation of anionic [ZnX 4 ] 2- effectively enhance the spin-orbit coupling effect, which significantly boosts the photoluminescence quantum yield (PLQY) up to 30.66 % and 54.62 % for afterglow and phosphorescence, respectively. Synchronously, the corresponding luminescence lifetime extend to 143.94 ms and 0.308 μs surpassing the indiscernible phosphorescence of [BTPP]X salt. More importantly, this halide family presents robust RTP emission with nearly unattenuated PLQY in water and harsh condition (acid and basic aqueous solution) over half a year. The highly efficient integrated afterglow and STE phosphorescence as well as ultrahigh aqueous state RTP realize multiple anti-counterfeiting applications in wide chemical environments., (© 2024 Wiley-VCH GmbH.)

Pathogenic infectious diseases have persistently posed significant threats to public health. Phototheranostics, which combines the functions of diagnostic imaging and therapy, presents an extremely promising solution to block the spread of pathogens as well as the outbreak of epidemics owing to its merits of a wide-spectrum of activity, high controllability, non-invasiveness, and difficult to acquire resistance. Among multifarious phototheranostic agents, second near-infrared (NIR-II, 1000-1700 nm) aggregation-induced emission luminogens (AIEgens) are notable by virtue of their deep penetration depth, excellent biocompatibility, balanced radiative and nonradiative decay and aggregation-enhanced theranostic performance, making them an ideal option for combating pathogens. This minireview provides a systematical summary of the latest advancements in NIR-II AIEgens with emphasis on the molecular design and nanoplatform formulation to fulfill high-efficiency in treating bacterial and viral pathogens, classified by disease models. Then, the current challenges, potential opportunities, and future research directions are presented to facilitate the further progress of this emerging field., (© 2024 Wiley-VCH GmbH.)

Developing versatile photosensitizers to actualize selective antibacteria over normal cells presents an appealing yet significantly challenging task. In this study, a novel photosensitizer named DMMA-SCPI is rationally designed and facilely synthesized, which is demonstrated as a type-I photosensitizer featured by aggregation-induced emission tendency. DMMA-SCPI is capable of effectively eliminating both Galanz positive bacteria and Galanz negative bacteria in vitro and in vivo, and showed insignificant injury to normal cells and tissues, probably resulting from its pyridinium halide that has stronger adsorption property on negatively charged bacteria compared to normal cells, as well as its suitable antimicrobial activity. The antimicrobial activity of pyridinium salt type photosensitizer depends on the adsorptive activities on the surface of bacterial cells as well as the antimicrobial activity of the reactive oxygen species (ROS). Among three photosensitizers, DMMA-SCPI has better water solubility, which provides greater surface activity to adsorb bacteria. Moreover, DMMA-SCPI produces more superoxide anion radicals as ROS, which has proper antimicrobial activity with high biosafety for effect extracellular antibacteria., (© 2024 Wiley‐VCH GmbH.)

Glioblastoma (GBM) remains a daunting oncological challenge because of its aggressive nature and resistance to conventional therapies. Inhibition of the intrinsic STING pathway in GBM hampers the effectiveness of immunotherapies. To overcome this clinical limitation, a Sequential Release HydroLipo System (SRHLS) is developed, in which hydrogels and nanoparticles are combined for controlled drug release. The SRHLS sequentially released decitabine and STING agonists, thereby correcting STING signaling dysfunction through epigenetic reprogramming and enhancing antitumor immunity. According to in vitro and in vivo experiments, the SRHLS reshaped the tumor microenvironment and markedly inhibited tumor growth, recurrence, and metastasis. These findings underscore the potential of the SRHLS as a promising therapeutic strategy for GBM., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Chemodynamic therapy (CDT) has become an emerging cancer treatment strategy with advantages of tumor-specificity, high selectivity, and low systemic toxicity. However, it usually suffers from low therapeutic efficacy. This is caused by low hydroxyl radical (·OH) yield arising because of the relatively high pH, overexpressed glutathione, and low H 2 O 2 concentration in the tumor microenvironment (TME). Herein, a probiotic metabolism-initiated pH reduction and H 2 O 2 supply-enhanced CDT strategy is reported to eradicate tumors by generating ·OH, in which Lactobacillus acidophilus is coupled with CoFeCe-layered double hydroxide nanosheets loaded with CaO 2 nanoparticles (NPs) as a chemodynamic platform for high-efficiency CDT (CaO 2 /LDH@L. acidophilus). Owing to the hypoxia tropism of L. acidophilus, CaO 2 /LDH@L. acidophilus exhibits increased accumulation at tumor sites compared with the CaO 2 /LDH. The CaO 2 NPs loaded on CoFeCe-LDH nanosheets are decomposed into H 2 O 2 in the TME. L. acidophilus metabolite-induced pH reduction (<5.5) and CaO 2 -mediated in situ H 2 O 2 generation synergistically boost ·OH generation activity of the CoFeCe-LDH nanosheets, effectively damaging cancer cells and ablating tumors with a tumor inhibition rate of 96.4%, 2.32-fold higher than that of CaO 2 /LDH. This work demonstrates that probiotics can function as a tumor-targeting platform to remodel the TME and amplify ROS generation for highly efficient and precise CDT., (© 2024 Wiley‐VCH GmbH.)

Efficient synthesis of C n H 2n+1 OH (n=1, 2) via photochemical CO 2 reduction holds promise for achieving carbon neutrality but remains challenging. Here, we present rare earth dual single atoms (SAs) catalysts containing ErN 6 and NdN 6 moieties, fabricated via an atom-confinement and coordination method. The dual Er-Nd SAs catalysts exhibit unprecedented generation rates of 1761.4 μmol g -1  h -1 and 987.7 μmol g -1  h -1 for CH 3 CH 2 OH and CH 3 OH, respectively. Through a combination of theoretical calculation, XAFS analysis, aberration-corrected HAADF-STEM, and in-situ FTIR spectroscopy, we demonstrate that the Er SAs facilitate charge transfer, serving as active centers for C-C bond formation, while Nd SAs provide the necessary *CO for C-C coupling in C 2 H 5 OH synthesis under visible light. Furthermore, the experiment and DFT calculation elucidate that the variety of electronic states induced by 4 f orbitals of the Er SAs and the p-f orbital hybridization of Er-N moieties enable the formation of charge-transfer channel. Therefore, this study sheds light on the pivotal role of *CO adsorption in achieving efficient conversion from CO 2 to C n H 2n+1 OH (n=1, 2) via a novel rare earth-based dual SAs photocatalysis approach., (© 2024 Wiley-VCH GmbH.)

Dry eye affects majority of the global population, causing significant discomfort or even visual impairment, of which inflammation plays a crucial role in the deterioration process. This highlights the need for effective and safe anti-inflammatory treatments to achieve satisfactory therapeutic outcomes. This study focuses on the potential of tetrahedral framework nucleic acids (tFNA), a self-assembled nucleic acid material, as a simple and rapid treatment for oxidative stress and inflammation-induced disorders associated with dry eye. Mechanistically, tFNA is found to effectively alleviate dry eye damage by promoting corneal epithelial healing, restoring goblet cell function, and facilitating tear secretion recovery. Through RNA-seq analysis, it is observed that tFNA treatment normalizes the expression levels of most genes. Further exploration of the mechanism reveals that tFNA reduces excessive production of reactive oxygen species and modulates the inflammatory microenvironment, especially through cGAS-STING pathway thereby levels of inflammatory cytokines, including MMP9 and IL-6, are reduced. Additionally, tFNA demonstrates excellent safety performance without causing damage to the eye. Importantly, this study represents a successful application of nanophase materials with nucleic acid biological features for the effective treatment of dry eye, highlighting the potential clinical use of tFNA in the treatment of dry eye., (© 2024 Wiley‐VCH GmbH.)

Design and synthesis of highly active and robust bifunctional cathode catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are of vital significance for practical applications of lithium-oxygen (Li-O 2 ) batteries. Herein, a built-in electric field (BIEF) strategy is reported to fabricate MnTe/MnO heterostructures with a large work function difference (ΔΦ) as a bifunctional cathode catalyst in Li-O 2 batteries. The MnTe/MnO heterostructures with nanosheets and microporous structures result in an abundance of exposed active sites and facilitate mass transfer. More importantly, the heterogeneous MnTe/MnO nano-interface region provides a BIEF that can trigger interfacial charge redistribution, fine-tune the adsorption energy of oxygen intermediates, and alter the morphology of discharge products to accelerate ORR/OER kinetics. Impressively, the fabricated Li-O 2 batteries with MnTe/MnO cathode showcases exhibit excellent electrochemical performances, including low charging overpotential, a high specific capacity of 11930 mA h g -1 , and good cycle stability over 350 cycles even with a fixed specific capacity of 500 mA h g -1 at a current density of 500 mA g -1 . This work provides an avenue for the rational design of high performance heterostructure electrocatalysts toward practical applications for rechargeable Li-O 2 batteries., (© 2024 Wiley‐VCH GmbH.)

Flexible heterojunctions based on molecular systems are in high demand for applications in photonics, electronics, and smart materials, but fabrication challenges have hindered progress. Herein, we present an in situ approach to creating optical heterojunctions using hydration-mediated flexible molecular crystals. These hydrated multi-component molecular solids display strong blue emitting optical waveguides with minimal optical loss (0.005 dB/μm) and excellent flexibility (elastic modulus: 3.87 GPa). The water-mediated process enables the molecular microwires with tunable elastic and plastic deformation, as well as reversible uptake and release of lattice water, facilitating the formation of flexible heterojunctions. Spectral analysis and theoretical modeling reveal that these microwires exhibit both photochromism and color-tunable dual emission (fluorescence and phosphorescence), expanding their utility in photonic information encoding. Therefore, this work introduces a hydration-mediated molecular engineering strategy for fabricating crystalline heterojunctions with on-demand processability and controllable emission sequences, enabling optical signal manipulation at the micro/nanoscale., (© 2024 Wiley-VCH GmbH.)

Manganese Hexacyanoferrate (Mn─HCF) is a preferred cathode material for sodium-ion batteries used in large-scale energy storage. However, the inherent vacancies and the presence of H 2 O within the imperfect crystal structure of Mn─HCF lead to material failure and interface failure when used as a cathode. Addressing the challenge of constructing a stable cathode is an urgent scientific problem that needs to be solved to enhance the performance and lifespan of these batteries. In this review, the crystal structure of Mn─HCF is first introduced, explaining the formation mechanism of vacancies and exploring the various ways in which H 2 O molecules can be present within the crystal structure. Then comprehensively summarize the mechanisms of material and interfacial failure in Mn─HCF, highlighting the key factors contributing to these issues. Additionally, eight modification strategies designed to address these failure mechanisms are encapsulated, including vacancy regulation, transition metal substitution, high entropy, the pillar effect, interstitial H 2 O removal, surface coating, surface vacancy repair, and cathode electrolyte interphase reinforcement. This comprehensive review of the current research advances on Mn─HCF aims to provide valuable guidance and direction for addressing the existing challenges in their application within SIBs., (© 2024 Wiley‐VCH GmbH.)

Rational design of highly active and stable catalysts for dopamine oxidation is still a great challenge. Herein, inspired by the catalytic pocket of natural enzymes, an iodine (I)-doped single Fe-site catalyst (I/Fe SA NC) is synthesized to mimic the catalytic center of heme enzymes in both geometrical and electronic structures, aiming to enhance dopamine (DA) oxidation. Experimental studies and theoretical calculations show that electronic communication between I and FeN 5 effectively modulates the electronic structure of the active site, greatly optimizing the overlap of Fe 3d and O 2p orbitals, thereby enhancing OH adsorption. In addition, the electronic communication induced by iodine doping attenuates the attack of proton hydrogen on the active center, thereby enhancing the stability of I/Fe SA NC. This work provides new insights into the design of highly active and stable single-atom catalysts and enhances the understanding of catalytic mechanisms for DA oxidation at the atomic scale., (© 2024 Wiley‐VCH GmbH.)

n-Type conjugated polymers featuring low-lying lowest unoccupied molecular orbital (LUMO) energy levels are essential for achieving high-performance n-type organic thin-film transistors (OTFTs) and organic thermoelectrics (OTEs). However, the synthesis of acceptors with strong electron-withdrawing characteristics presents a significant challenge. Herein, a peripheral functionalization strategy is employed on the tricyclic framework anthracene by introducing dual N,O-bidentate BF 2 /B(CN) 2 groups to enhance its electron-withdrawing capability. This approach successfully navigates synthetic challenges, leading to the development of two novel acceptor building blocks: DBNF and DBNCN. Compared to the counterparts with a single N,O-bidentate BF 2 /B(CN) 2 moiety, DBNF and DBNCN exhibit an extended π-backbone, enhanced molecular packing, and improved electron-withdrawing properties. Utilizing these innovative acceptor monomers, copolymers, PDBNF and PDBNCN, are synthesized, which exhibit considerably suppressed LUMO ≈-4.0 eV. The deep LUMO of PDBNF together with its favourable bimodal packing orientation leads to remarkable electron mobility of 3.04 cm 2  V -1  s -1 with improved stability in OTFTs. Importantly, efficient n-doping in OTEs is achieved with PDBNCN, exhibiting exceptional conductivity of 95.5 S cm -1 and a maximum power factor of 147.8 μW m -1 K -2 -among the highest reported for solution-processed n-type polymers. This work underscores the effectiveness of introducing dual B←N and cyano functionalities in attaining high-performance n-type plastic electronics., (© 2024 Wiley-VCH GmbH.)

The catalytic activity of platinum for CO oxidation depends on the interaction of electron donation and back-donation at the platinum center. Here we demonstrate that the platinum bromine nanoparticles with electron-rich properties on bromine bonded with sp-C in graphdiyne (PtBr NPs/Br-GDY), which is formed by bromine ligand and constitutes an electrocatalyst with a high CO-resistant for methanol oxidation reaction (MOR). The catalyst showed peak mass activity for MOR as high as 10.4 A mg Pt -1 , which is 20.8 times higher than the 20 % Pt/C. The catalyst also showed robust long-term stability with slight current density decay after 100 hours at 35 mA cm -2 . Structural characterization, experimental, and theoretical studies show that the electron donation from bromine makes the surface of platinum catalysts highly electron-rich, and can strengthen the adsorption of CO as well as enhance π back-donation of Pt to weaken the C-O bond to facilitate CO electrooxidation and enhance catalytic performance during MOR. The results highlight the importance of electron-rich structure among active sites in Pt-halogen catalysts and provide detailed insights into the new mechanism of CO electrooxidation to overcome CO poisoning at the Pt center on an orbital level., (© 2024 Wiley-VCH GmbH.)

As a new avenue for cancer research, phototheranostics has shown inexhaustible and vigorous vitality as it permits real-time diagnosis and concurrent in situ therapy upon non-invasive light-initiation. However, construction of an advanced material, allowing prominent phototheranostic outputs and synchronously surmounting the inherent deficiency of phototheranostics, would be an appealing yet significantly challenging task. Herein, an aggregation-induced emission (AIE)-active luminogen (namely DBD-TM) featured by intensive electron donor-acceptor strength and twisted architecture with finely modulated intramolecular motion, is tactfully designed and prepared. DBD-TM simultaneously possessed fluorescence emission in the second near-infrared (NIR-II) region and high-efficiency photothermal conversion. By integrating DBD-TM with anti-angiogenic agent sorafenib, a versatile nanomaterial is smoothly fabricated and utilized for trimodal imaging-navigated synergistic therapy involving photothermal therapy and anti-angiogenesis toward cancer. This advanced approach is capable of affording accurate tumor diagnosis, complete tumor elimination, and largely restrained tumor recurrence, evidently denoting a prominent theranostic formula beyond phototheranostics. This study will offer a blueprint for exploiting a new generation of cancer theranostics., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Tuberculosis, a fatal infectious disease caused by Mycobacterium tuberculosis (M.tb), is difficult to treat with antibiotics due to drug resistance and short drug half-life. Phototherapy represents a promising alternative to antibiotics in combating M.tb. Exploring an intelligent material allowing effective tuberculosis treatment is definitely appealing, yet a significantly challenging task. Herein, an all-in-one biomimetic therapeutic nanoparticle featured by aggregation-induced second near-infrared emission, granuloma-targeting, and self-oxygenation is constructed, which can serve for prominent fluorescence imaging-navigated combined phototherapy toward tuberculosis. After camouflaging the biomimetic erythrocyte membrane, the nanoparticles show significantly prolonged blood circulation and increased selective accumulation in tuberculosis granuloma. Upon laser irradiation, the loading photosensitizer of aggregation-induced emission photosensitizer elevates the production of reactive oxygen species (ROS), causing M.tb damage and death. The delivery of oxygen to relieve the hypoxic granuloma microenvironment supports ROS generation during photodynamic therapy. Meanwhile, the photothermal agent, Prussian blue nanoparticles, plays the role of good photothermal killing effect on M.tb. Moreover, the growth and proliferation of granuloma and M.tb colonies are effectively inhibited in the nanoparticle-treated tuberculous granuloma model mice, suggesting the combined therapeutic effects of enhancing photodynamic therapy and photothermal therapy., (© 2024 Wiley‐VCH GmbH.)

A concise synthetic strategy utilizing a Zr catalyst for the construction of cyctetryptomycin A and B is reported. Cyctetryptomycin A and B are recently isolated, complex tetrameric natural products for which total synthesis has not been previously reported. This study presents a practical approach for the construction of two consecutive quaternary carbon centers with a Zr catalyst. Furthermore, the first total synthesis of cyctetryptomycin A and B was achieved by this Zr-catalyzed radical coupling. The radical dimerization reaction mediated by the Zr catalyst required 1,2-bis(diphenylphosphino)ethane (dppe) as an indispensable additive. Through both experimental and theoretical investigations into the mechanism of this Zr-catalyzed reaction, the specific role of dppe was elucidated. In addition, the synthetic approach was extended to enable the practical synthesis of other dimeric natural products, including tetratryptomycin A, dibrevianamide F, and ditryptophenaline. Finally, the synthetic mechanism of cyctetryptomycin A and B, through the oxidative macrocyclization of tetratryptomycin A by CttpC, was newly elucidated by both experimental and docking simulations., (© 2024 Wiley-VCH GmbH.)

In response to carbon neutrality, photocatalytic reduction of CO 2 has been the subject of growing interest for researchers over the past few years. Multi-carbon products (C 2+ ) with higher energy density and larger market value produced from photocatalytic reduction of CO 2 are still very limited owing to the low photocatalytic productivity and poor selectivity of products. This review focuses on the recent progress on photocatalytic reduction of CO 2 towards C 2+ products from the perspective of performance evaluation and mechanistic understanding. We first provide a systematic description of the entire fundamental procedures of photocatalytic reduction of CO 2 . An in-depth strategy analysis for improving the selectivity of photocatalytic reduction of CO 2 to C 2+ products is then addressed. Then the focus was on summarizing the ways to improve C 2+ selectivity. The intrinsic mechanisms of photocatalytic reduction of CO 2 to C 2+ products are summarized in the final. Combining the foundation of photocatalysis with promising catalyst strategies, this review will offer valuable guidance for the development of efficient photocatalytic systems for the synthesis of C 2+ products., (© 2024 Wiley-VCH GmbH.)

Innovative advances in the exploitation of effective electrocatalytic materials for the reduction of nitrogen (N 2 ) to ammonia (NH 3 ) are highly required for the sustainable production of fertilizers and zero-carbon emission fuel. In order to achieve zero-carbon footprints and renewable NH 3 production, electrochemical N 2 reduction reaction (NRR) provides a favorable energy-saving alternative but it requires more active, efficient, and selective catalysts. In current work, sulfur vacancy (Sv)-rich NiCo 2 S 4 @MnO 2 heterostructures are efficaciously fabricated via a facile hydrothermal approach followed by heat treatment. The urchin-like Sv-NiCo 2 S 4 @MnO 2 heterostructures serve as cathodes, which demonstrate an optimal NH 3 yield of 57.31 µg h -1  mg cat -1 and Faradaic efficiency of 20.55% at -0.2 V versus reversible hydrogen electrode (RHE) in basic electrolyte owing to the synergistic interactions between Sv-NiCo 2 S 4 and MnO 2 . Density functional theory (DFT) simulation further verifies that Co-sites of urchin-like Sv-NiCo 2 S 4 @MnO 2 heterostructures are beneficial to lowering the energy threshold for N 2 adsorption and successive protonation. Distinctive micro/nano-architectures exhibit high NRR electrocatalytic activities that might motivate researchers to explore and concentrate on the development of heterostructures for ambient electrocatalytic NH 3 generation., (© 2024 Wiley‐VCH GmbH.)

Alkali metals (e.g. Li, Na, and K) and multivalent metals (e.g. Zn, Mg, Ca, and Al) have become star anodes for developing high-energy-density rechargeable batteries due to their high theoretical capacity and excellent conductivity. However, the inevitable dendrites and unstable interfaces of metal anodes pose challenges to the safety and stability of batteries. To address these issues, covalent organic frameworks (COFs), as emerging materials, have been widely investigated due to their regular porous structure, flexible molecular design, and high specific surface area. In this minireview, we summarize the research progress of COFs in stabilizing metal anodes. First, we present the research origins of metal anodes and delve into their advantages and challenges as anodes based on the physical/chemical properties of alkali and multivalent metals. Then, special attention has been paid to the application of COFs in the host design of metal anodes, artificial solid electrolyte interfaces, electrolyte additives, solid-state electrolytes, and separator modifications. Finally, a new perspective is provided for the research of metal anodes from the molecular design, pore modulation, and synthesis of COFs., (© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

The second near-infrared (NIR-II, 1000-1700 nm) light-activated organic photothermal agent that synchronously enables satisfying NIR-II fluorescence imaging is highly warranted yet rather challenging on the basis of the overwhelming nonradiative decay. Herein, such an agent, namely TPABT-TD, was tactfully designed and constructed via employing benzo[c]thiophene moiety as bulky electron donor/π-bridge and tailoring the peripheral molecular rotors. Benefitting from its high electron donor-acceptor strength and finely modulated intramolecular motion, TPABT-TD simultaneously exhibits ultralong absorption in NIR-II region, intense fluorescence emission in the NIR-IIa (1300-1500 nm) region as nanoaggregates, and high photothermal conversion upon 1064 nm laser irradiation. Those intrinsic advantages endow TPABT-TD nanoparticles with prominent fluorescence/photoacoustic/photothermal trimodal imaging-guided NIR-II photothermal therapy against orthotopic 4T1 breast tumor with negligible adverse effect., (© 2024 Wiley-VCH GmbH.)

Transition metal chalcogenides (TMCs) emerge as promising anode materials for sodium-ion batteries (SIBs), heralding a new era of energy storage solutions. Despite their potential, the mechanisms underlying their performance enhancement and susceptibility to failure in ether-based electrolytes remain elusive. This study delves into these aspects, employing CoS 2 electrodes as a case in point to elucidate the phenomena. The investigation reveals that CoS 2 undergoes a unique irreversible and progressive solid-liquid-solid phase transition from its native state to sodium polysulfides (NaPSs), and ultimately to a Cu 1.8 S/Co composite, accompanied by a gradual morphological transformation from microspheres to a stable 3D porous architecture. This reconstructed 3D porous structure is pivotal for its exceptional Na + diffusion kinetics and resilience to cycling-induced stress, being the main reason for ultrastable cycling and ultrahigh rate capability. Nonetheless, the CoS 2 electrode suffers from an inevitable cycle life termination due to the microshort-circuit induced by Na metal corrosion and separator degradation. Through a comparative analysis of various TMCs, a predictive framework linking electrode longevity is established to electrode potential and Gibbs free energy. Finally, the cell failure issue is significantly mitigated at a material level (graphene encapsulation) and cell level (polypropylene membrane incorporation) by alleviating the NaPSs shuttling and microshort-circuit., (© 2024 Wiley‐VCH GmbH.)

Microbial factories lacking the ability of dynamically regulating the pathway enzymes overexpression, according to in situ metabolite concentrations, are suboptimal, especially when the metabolic intermediates are competed by growth and chemical production. The production of higher alcohols (HAs), which hijacks the amino acids (AAs) from protein biosynthesis, minimizes the intracellular concentration of AAs and thus inhibits the host growth. To balance the resource allocation and maintain stable AA flux, this work utilizes AA-responsive transcriptional attenuator ivbL and HA-responsive transcriptional activator BmoR to establish a concentration recognition-based auto-dynamic regulation system (CRUISE). This system ultimately maintains the intracellular homeostasis of AA and maximizes the production of HA. It is demonstrated that ivbL-driven enzymes overexpression can dynamically regulate the AA-to-HA conversion while BmoR-driven enzymes overexpression can accelerate the AA biosynthesis during the HA production in a feedback activation mode. The AA flux in biosynthesis and conversion pathways is balanced via the intracellular AA concentration, which is vice versa stabilized by the competition between AA biosynthesis and conversion. The CRUISE, further aided by scaffold-based self-assembly, enables 40.4 g L -1 of isobutanol production in a bioreactor. Taken together, CRUISE realizes robust HA production and sheds new light on the dynamic flux control during the process of chemical production., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Molecular ultralong room-temperature phosphorescence (RTP), exhibiting multiple stimuli-responsive characteristics, has garnered considerable attention due to its potential applications in light-emitting devices, sensors, and information safety. This work proposes the utilization of photochemical cascade processes (PCCPs) in molecular crystals to design a stepwise smart RTP switch. By harnessing the sequential dynamics of photo-burst movement (induced by [2+2] photocycloaddition) and photochromism (induced by photogenerated radicals) in a bismuth (Bi)-based metal-organic halide (MOH), a continuous and photo-responsive ultralong RTP can be achieved. Furthermore, utilizing the same Bi-based MOH, diverse application demonstrations, such as multi-mode anti-counterfeiting and information encryption, can be easily implemented. This work thus not only serves as a proof-of-concept for the development of solid-state PCCPs that integrate photosalient effect and photochromism with light-chemical-mechanical energy conversion, but also lays the groundwork for designing new Bi-based MOHs with dynamically responsive ultralong RTP., (© 2024 Wiley-VCH GmbH.)

Poly(p-phenylene-benzimidazole-terephthalamide) (PBIA) fibers with excellent mechanical properties are widely used in fields that require impact-resistant materials such as ballistic protection and aerospace. The introduction of heterocycles in polymer chains increases their flexibility and makes it easier to optimize the fiber structure. However, the inadequate orientation of polymer chains is one of the main reasons for the large difference between the measured and theoretical mechanical properties of PBIA fibers. Herein, carbon nanotubes (CNTs) are selected as an orientation seed. Their structural features allow CNTs to orient during the spinning process, which can induce an orderly arrangement of polymers and improve the orientation of the fiber microstructure. To ensure the complete 1D topology of long CNTs (≈10 µm), PBIA is used as an efficient dispersant to overcome dispersion challenges. The p-CNT/PBIA fibers (10 µm single-walled carbon nanotube 0.025 wt%) exhibit an increase of 22% in tensile strength and 23% in elongation, with a maximum tensile strength of 7.01 ± 0.31 GPa and a reinforcement efficiency of 893.6. The artificial muscle fabricated using CNT/PBIA fibers exhibits a 34.8% contraction and a 25% lifting of a 2 kg dumbbell, providing a promising paradigm for high-performance organic fibers as high-load smart actuators., (© 2023 Wiley‐VCH GmbH.)

Ensuring information security has emerged as a paramount concern in contemporary human society. Substantial advancements in this regard can be achieved by leveraging photonic signals as the primary information carriers, utilizing photonic logical gates capable of wavelength tunability across various time and spatial domains. However, the challenge remains in the rational design of materials possessing space-time-color multiple-resolution capabilities. In this work, a facile approach is proposed for crafting metal-organic halides (MOHs) that offer space-time-color resolution. These MOHs integrate time-resolved room temperature phosphorescence and color-resolved excitation wavelength dependencies with both space-resolved ex situ optical waveguides and in situ heterojunctions. Capitalizing on these multifaceted properties, MOHs-based two-dimensional (2D) optical waveguides and heterojunctions exhibit the ability to tune full-color emissions across the spectra from blue to red, operating within different spatial and temporal scales. Therefore, this work introduces an effective methodology for engineering space-time-color resolved MOH microstructures, holding significant promise for the development of high-density photonic logical devices., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Bio-catalysis represents a highly efficient and stereoselective method for the synthesis of valuable chiral compounds, however, the poor stability and limited reaction types of free enzymes restrict their wide application in industrial production. In this work, to overcome these problems, a multifunctional photoenzymatic nanoreactor CALB@COF-Ir was developed through the encapsulation of Candida antarctica lipase B (CALB) in a photosensitive covalent organic framework COF-Ir. This bio-nanocluster serves as efficient catalysts in asymmetric dynamic kinetic resolution (DKR) of secondary amines to give a series of chiral amines in high yields (up to 99 %) and enantioselectivities (up to 99 % ee). The well-designed COF-Ir not only acts as safety cover to prevent CALB from deactivation but promotes racemization of secondary amines via photo-induced hydrogen atom transfer (HAT) process. Photoelectric characterization and TDDFT calculation revealed that (ppy) 2 Ir units in COF-Ir play crucial role in this photocatalytic system which enhance its photo-redox properties through facilitating the separation between photoelectrons (e - ) and holes (h + ). Furthermore, the heterogeneous photoenzymatic nanoreactor could be recycled for five rounds with slight decline of catalytic reactivity., (© 2024 Wiley‐VCH GmbH.)

The fabrication of a multimodal phototheranostic platform on the basis of single-component theranostic agent to afford both imaging and therapy simultaneously, is attractive yet full of challenges. The emergence of aggregation-induced emission luminogens (AIEgens), particularly those emit fluorescence in the second near-infrared window (NIR-II), provides a powerful tool for cancer treatment by virtue of adjustable pathway for radiative/non-radiative energy consumption, deeper penetration depth and aggregation-enhanced theranostic performance. Although bulky thiophene π-bridges such as ortho-alkylated thiophene, 3,4-ethoxylene dioxythiophene and benzo[c]thiophene are commonly adopted to construct NIR-II AIEgens, the subtle differentiation on their theranostic behaviours has yet to be comprehensively investigated. In this work, systematical investigations discovered that AIEgen BT-NS bearing benzo[c]thiophene possesses acceptable NIR-II fluorescence emission intensity, efficient reactive oxygen species generation, and high photothermal conversion efficiency. Eventually, by using of BT-NS nanoparticles, unprecedented performance on NIR-II fluorescence/photoacoustic/photothermal imaging-guided synergistic photodynamic/photothermal elimination of tumors was demonstrated. This study thus offers useful insights into developing versatile phototheranostic systems for clinical trials., (© 2024 Wiley‐VCH GmbH.)

Accumulating evidence suggests that changes in the tumor microenvironment caused by radiotherapy are closely related to the recurrence of glioma. However, the mechanisms by which such radiation-induced changes are involved in tumor regrowth have not yet been fully investigated. In the present study, how cranial irradiation-induced senescence in non-neoplastic brain cells contributes to glioma progression is explored. It is observed that senescent brain cells facilitated tumor regrowth by enhancing the peripheral recruitment of myeloid inflammatory cells in glioblastoma. Further, it is identified that astrocytes are one of the most susceptible senescent populations and that they promoted chemokine secretion in glioma cells via the senescence-associated secretory phenotype. By using senolytic agents after radiotherapy to eliminate these senescent cells substantially prolonged survival time in preclinical models. The findings suggest the tumor-promoting role of senescent astrocytes in the irradiated glioma microenvironment and emphasize the translational relevance of senolytic agents for enhancing the efficacy of radiotherapy in gliomas., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

In this concept, we showcase the upsurge in the studies of dynamic ultralong room-temperature phosphorescence (RTP) materials containing inorganic and/or organic components as versatile photo-responsive platforms. The goal is to provide a comprehensive analysis of photo-controllable RTP, and meanwhile delve into the underlying RTP properties of various classes of photochromic materials including metal-organic complexes, organic-inorganic co-crystals, purely organic small molecules and organic polymers. In particular, the design principles governing the integration of the photochromic and RTP moieties within a single material system, and the tuning of dynamic RTP in response to light are emphasized. As such, this concept sheds light on the challenges and opportunities of using these tunable RTP materials for potential applications in optoelectronics, particularly highlighting their use of reversible information encryption, erasable light printing and rewritable smart paper., (© 2023 Wiley-VCH GmbH.)

Highly anticipated potassium metal batteries possess abundant potassium reserves and high theoretical capacity but currently suffer from poor cycling stability as a result of dendritic growth and volume expansion. Here, carbon cloths modified with different functional groups treated with ethylene glycol, ethanolamine, and ethylenediamine are designed as 3D hosts, exhibiting different wettability to molten potassium. Among them, the hydroxyl-decorated carbon cloth with a high affinity for potassium can achieve molten potassium perfusion (K@EG-CC) within 3 s. By efficiently inducing the uniform deposition of metal potassium, buffing its volume expansion, and lowering local current density, the developed K@EG-CC anode alleviates the dendrite growth issue. The K@EG-CC||K@EG-CC symmetric battery can be cycled stably for 2100 h and has only a small voltage hysteresis of ≈93 mV at 0.5 mA cm -2 . Moreover, the high-voltage plateau, high energy density, and long cycle life of K metal full batteries can be realized with a low-cost KFeSO 4 F@carbon nanotube cathode. This study provides a simple strategy to promote the commercial applications of potassium metal batteries., (© 2024 Wiley-VCH GmbH.)

The recent prevalence of monkeypox has led to the declaration of a Public Health Emergency of International Concern. Monkeypox lesions are typically ulcers or pustules (containing high titers of replication-competent virus) in the skin and mucous membranes, which allow monkeypox virus to transmit predominantly through intimate contact. Currently, effective clinical treatments for monkeypox are lacking, and strategies for blocking virus transmission are fraught with drawbacks. Herein, this work constructs a biomimetic nanotemplate (termed TBD@M NPs) with macrophage membranes as the coat and polymeric nanoparticles loading a versatile aggregation-induced emission featured photothermal molecule TPE-BT-DPTQ as the core. In a surrogate mouse model of monkeypox (vaccinia-virus-infected tail scarification model), intravenously injected TBD@M NPs show precise tracking and near-infrared region II fluorescence imaging of the lesions. Upon 808 nm laser irradiation, the virus is eliminated by the photothermal effect and the infected wound heals rapidly. More importantly, the inoculation of treated lesion tissue suspensions does not trigger tail infection or inflammatory activation in healthy mice, indicating successful blockage of virus transmission. This study demonstrates for the first time monkeypox theranostics using nanomedicine, and may bring a new insight into the development of a viable strategy for monkeypox management in clinical trials., (© 2023 Wiley-VCH GmbH.)

Photovoltaic thin film solar cells based on kesterite Cu 2 ZnSn(S, Se) 4 (CZTSSe) have reached 13.8% sunlight-to-electricity conversion efficiency. However, this efficiency is still far from the Shockley-Queisser radiative limit and is hindered by the significant deficit in open circuit voltage (V OC ). The presence of high-density interface states between the absorber layer and buffer or window layer leads to the recombination of photogenerated carriers, thereby reducing effective carrier collection. To tackle this issue, a new window structure ZnO/AgNW/ZnO/AgNW (ZAZA) comprising layers of ZnO and silver nanowires (AgNWs) is proposed. This structure offers a simple and low-damage processing method, resulting in improved optoelectronic properties and junction quality. The ZAZA-based devices exhibit enhanced V OC due to the higher built-in voltage (V bi ) and reduced interface recombination compared to the usual indium tin oxide (ITO) based structures. Additionally, improved carrier collection is demonstrated as a result of the shortened collection paths and the more uniform carrier lifetime distribution. These advances enable the fabrication of the first ITO-free CZTSSe solar cells with over 10% efficiency without an anti-reflective coating., (© 2023 The Authors. Small published by Wiley-VCH GmbH.)

MXenes are considered a promising negative electrode material for potassium ion batteries (PIBs) in view of their low potassium ion diffusion barrier and excellent electrical conductivity. However, the stacking phenomenon in practical applications severely reduces their active surface and leads to slow K + diffusion. Herein, a facile composite template method is proposed to construct stacking-resistance 3D carbon-supported Ti 3 C 2 T x (3D-C@Ti 3 C 2 T x ) hollow spheres. Due to the unique structure, when used as a negative electrode material, as-prepared 3D-C@Ti 3 C 2 T x hollow spheres show not only improved rate capability with 160.4 mAh g -1 at 100 mA g -1 and 133.7 mAh g -1 at 500 mA g -1 , but also stable cycling performance with 142.5 mAh g -1 specific capacity remained at 2 A g -1 after 4200 cycles. Furthermore, the full cells with 3D-C@Ti 3 C 2 T x anode can operate stably for 1000 cycles at 100 mA g -1 . Moreover, the linear fit analysis demonstrates that 3D-C@Ti 3 C 2 T x hollow spheres have a fast and stable capacitive potassium storage mechanism. This method is simple and easy to implement, which provide a feasible path to solve the stacking problem of 2D materials., (© 2023 Wiley-VCH GmbH.)

Electrocatalytic C-N coupling process is indeed a sustainable alternative for direct urea synthesis and co-upgrading of carbon dioxide and nitrate wastes. However, the main challenge lies in the unactivated C-N coupling process. Here, we proposed a strategy of intermediate assembly with alkali metal cations to activate C-N coupling at the electrode/electrolyte interface. Urea synthesis activity follows the trend of Li + + + + . In the presence of K + , a world-record performance was achieved with a urea yield rate of 212.8±10.6 mmol h -1  g -1 on a single-atom Co supported TiO 2 catalyst at -0.80 V versus reversible hydrogen electrode. Theoretical calculations and operando synchrotron-radiation Fourier transform infrared measurements revealed that the energy barriers of C-N coupling were significantly decreased via K + mediated intermediate assembly. By applying this strategy to various catalysts, we demonstrate that intermediate assembly at the electrode/electrolyte interface is a universal approach to boost sustainable urea synthesis., (© 2023 Wiley-VCH GmbH.)

Transition-metal sulfides have been regarded as perspective anode candidates for high-energy Na-ion batteries. Their application, however, is precluded severely by either low charge storage or huge volumetric change along with sluggish reaction kinetics. Herein, an effective synergetic Sn incorporation-Zn substitution strategy is proposed based on copper-based sulfides. First, Na-ion storage capability of copper sulfide is significantly improved via incorporating an alloy-based Sn element. However, this process is accompanied by sacrifice of structural stability due to the high Na-ion uptake. Subsequently, to maintain the high Na-ion storage capacity, and concurrently improve cycling and rate capabilities, a Zn substitution strategy (taking partial Sn sites) is carried out, which could significantly promote Na-ion diffusion/reaction kinetics and relieve mechanical strain-stress within the crystal framework. The synergetic Sn incorporation and Zn substitution endow copper-based sulfides with high specific capacity (≈560 mAh g -1 at 0.5 A g -1 ), ultrastable cyclability (80 k cycles with ≈100% capacity retention), superior rate capability up to 200 A g -1 , and ultrafast charging feature (≈4 s per charging with ≈190 mAh g -1 input). This work provides in-depth insights for developing superior anode materials via synergetic multi-cation incorporation/substitution, aiming at solving their intrinsic issues of either low specific capacity or poor cyclability., (© 2023 Wiley-VCH GmbH.)

An iridium-catalyzed remote site-switchable hydroarylation of alkenes was reported, delivering the products functionalized at the subterminal methylene and terminal methyl positions on an alkyl chain controlled by two different ligands, respectively, in good yields and with good to excellent site-selectivities. The catalytic system showed good functional group tolerance and a broad substrate scope, including unactivated and activated alkenes. More importantly, the regioconvergent transformations of mixtures of isomeric alkenes were also successfully realized. The results of the mechanistic studies demonstrate that the reaction undergoes a chain-walking process to give an [Ar-Ir-H] complex of terminal alkene. The subsequent processes proceed through the modified Chalk-Harrod-type mechanism via the migratory insertion of terminal alkene into the Ir-C bond followed by C-H reductive elimination to afford the hydrofunctionalization products site-selectively., (© 2023 Wiley-VCH GmbH.)

Controlling the structure and properties of catalysts through atomic arrangement is the source of producing a new generation of advanced catalysts. A highly active and stable catalyst in catalytic reactions strongly depends on an ideal arrangement structure of metal atoms. We demonstrated that the introduction of the defect-rich structures, low coordination number (CN), and tensile strain in three-dimensional (3D) urchin-like palladium nanoparticles through chlorine bonded with sp-C in graphdiyne (Pd-UNs/Cl-GDY) can regulate the arrangement of metal atoms in the palladium nanoparticles to form a special structure. In situ Fourier infrared spectroscopy (FTIR) and theoretical calculation results show that Pd-UNs/Cl-GDY catalyst is beneficial to the oxidation and removal of CO intermediates. The Pd-UNs/Cl-GDY for methanol oxidation reaction (MOR) that display high current density (363.6 mA cm -2 ) and mass activity (3.6 A mg Pd -1 ), 12.0 and 10.9 times higher than Pd nanoparticles, respectively. The Pd-UNs/Cl-GDY catalyst also exhibited robust stability with still retained 95 % activity after 2000 cycles. A defects libraries of the face-centered cubic and hexagonal close-packed crystal catalysts (FH-NPs) were synthesized by introducing chlorine in graphdiyne. Such defect-rich structures, low CN, and tensile strain tailoring methods have opened up a new way for the catalytic reaction of MOR., (© 2023 Wiley-VCH GmbH.)

Integrating hematite nanostructures with efficient layer double hydroxides (LDHs) is highly desirable to improve the photoelectrochemical (PEC) water oxidation performance. Here, an innovative and facile strategy is developed to fabricate the FeTi-LDH overlayer decorated Fe 2 O 3 /Fe 2 TiO 5 photoanode via a surface self-transformation induced by the co-treatment of hydrazine and NaOH at room temperature. Electrochemical measurements find that this favorable structure can not only facilitate the charge transfer/separation at the electrode/electrolyte interface but also accelerate the surface water oxidation kinetics. Consequently, the as-obtained Fe 2 O 3 /Fe 2 TiO 5 /LDH photoanode exhibits a remarkably increased photocurrent density of 3.54 mA cm -2 at 1.23 V versus reversible hydrogen electrode (RHE) accompanied by an obvious cathodic shift (≈140 mV) in the onset potential. This work opens up a new and effective pathway for the design of high-performance hematite photoanodes toward efficient PEC water oxidation., (© 2023 Wiley-VCH GmbH.)

Harnessing the potential of thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) is crucial for developing light-emitting diodes (LEDs), lasers, sensors, and many others. However, effective strategies in this domain are still relatively scarce. This study presents a new approach to achieving highly efficient deep-blue TADF (with a PLQY of 25 %) and low-energy orange RTP (with a PLQY of 90 %) through the fabrication of lead-free hybrid halides. This new class of monomeric and dimeric 0D antimony halides can be facilely synthesized using a bottom-up solution process, requiring only a few seconds to minutes, which offer exceptional stability and nontoxicity. By leveraging the highly adaptable molecular arrangement and crystal packing modes, the hybrid antimony halides demonstrate the ability to self-assemble into regular 1D microrod and 2D microplate morphologies. This self-assembly is facilitated by multiple non-covalent interactions between the inorganic cores and organic shells. Notably, these microstructures exhibit outstanding polarized luminescence and function as low-dimensional optical waveguides with remarkably low optical-loss coefficients. Therefore, this work not only presents a pioneering demonstration of deep-blue TADF in hybrid antimony halides, but also introduces 1D and 2D micro/nanostructures that hold promising potential for applications in white LEDs and low-dimensional photonic systems., (© 2023 Wiley-VCH GmbH.)

Dual-ion battery is a new type of battery in which both anions and cations participate in the energy storage process. However, this unique battery configuration imposes high requirements on the cathode, which typically presents a poor rate performance due to the sluggish diffusion dynamics and intercalation reaction kinetics of anions. Herein, we report petroleum coke-based soft carbon as the cathode for dual-ion batteries, exhibiting a superior rate performance with a specific capacity of 96 mAh g -1 at a rate of 2 C and 72 mAh g -1 remained even at 50 C. In situ XRD and Raman demonstrate that the anions can directly form lower-stage graphite intercalation compounds during the charge process owing to the surface effect, skipping the long evolutionary process from higher to lower stage, thus significantly improving the rate performance. This study highlights the impact of the surface effect and provides a promising perspective for dual-ion batteries., (© 2023 Wiley-VCH GmbH.)

Constructing Van der Waals heterojunction is a crucial strategy to achieve excellent photocatalytic activity. However, in most Van der Waals heterojunctions synthesized by ex situ assembly, electron transfer encounters huge hindrances at the interface between the two components due to the large spacing and potential barrier. Herein, a phosphate-bridged Van der Waals heterojunction of cobalt phthalocyanine (CoPc)/tungsten disulfide (WS 2 ) bridged by phosphate (xCoPc-nPO 4 - -WS 2 ) is designed and prepared by the traditional wet chemistry method. By introducing a small phosphate molecule into the interface of CoPc and WS 2 , creates an electron "bridge", resulting in a compact combination and eliminating the space barrier. Therefore, the phosphate (PO 4 - ) bridge can serve as an efficient electron transfer channel in heterojunction and can efficiently transmit photoelectrons from WS 2 to CoPc under excited states. These excited photoelectrons are captured by the catalytic central Co 2+ in CoPc and subsequently convert CO 2 molecules into CO and CH 4 products, achieving 17-fold enhancement on the 3CoPc-0.6PO 4 - -WS 2 sample compared to that of pure WS 2 . Introducing a small molecule "bridge" to create an electron transfer channel provides a new perspective in designing efficient photocatalysts for photocatalytic CO 2 reduction into valuable products., (© 2023 Wiley-VCH GmbH.)

Freshwater scarcity crisis threatens human life and economic security. Collecting water from the fog seems to be an effective method to defuse this crisis. Nonetheless, the existing fog collection methods have the limitations of the low fog collection rate and efficiency because of their gravity-based droplet shedding. Here, the aforementioned limitations are resolved by proposing a new fog collection method based on the self-driven jet phenomenon of the mini fog droplets. A prototype fog collector (PFC) composed of a square container that is filled with water is first designed. Both sides of the PFC are superhydrophobic but covered with superhydrophilic pore array. The mini fog droplets touching the side wall are easily captured and spontaneously and rapidly penetrate into the pores to form jellyfish-like jets, which greatly increases the droplet shedding frequency, guaranteeing a higher fog collection rate and efficiency compared with the existing fog collection methods. Based on this, a more practical super-fast fog collector is finally successfully designed and fabricated which is assembled by several PFCs. This work is hoping to resolve the water crisis in some arid but foggy regions., (© 2023 Wiley-VCH GmbH.)

Multimodal phototheranostics on the basis of a single molecule with one-for-all characteristics represents a convenient approach for effective cancer treatment. In this report, a versatile molecule featured by aggregation-induced emission, namely DHTDP, synchronously enabling second near-infrared (NIR-II) fluorescence emission and efficient photothermal conversion is developed by elaborate structural modulation. By camouflaging DHTDP nanoparticles with cancer cell membrane, the resultant biomimetic nanoparticles exhibit significantly both facilitated delivery efficiency and homologous targeting capability, and afford precise imaging guidance and maximize therapeutic outcomes in form of NIR-II fluorescence imaging (FLI)-photoacoustic imaging (PAI)-photothermal imaging (PTI) trimodal imaging-guided photothermal therapy (PTT). This study presents the first example of biomimetic multimodal phototheranostics loaded by homogeneity-targeting cell membrane, thus brings a new insight into the exploration of superior phototheranostics for practical cancer theranostics., (© 2023 Wiley-VCH GmbH.)

Glassy materials, with desirable mechanical rigidity, shaping ability, high transparency, are attracting great interest in diverse fields. However, optically bulk molecule-based glasses are still rare, mainly due to limited monomeric species and harsh preparation conditions. Herein, we report a facile bottom-up solution fabrication process to obtain metal-free supramolecular glasses (SMGs) at the macroscopic scale using L-Histidine and hexamethylenetetramine as building blocks. The chiral SMGs possess color-tunable ultralong room temperature phosphorescence (decay lifetime up to 141.2 ms) and circular polarized luminescence (g factor up to 8.7×10 -3 ). The strong hydrogen bonds effectively drive the formation of SMGs, and provide a rigid microenvironment to boost triplet exciton generation. By virtue of excitation- and temperature-dependent ultralong phosphorescence of the SMGs, applications including multicolored displays, visual UV detection, and persistently luminescent thermometer are demonstrated., (© 2023 Wiley-VCH GmbH.)

Binary metal nickel-iron alloys have been proven to have great potential in oxygen evolution reaction (OER) electrocatalysis, but there are still certain challenges in how to construct more efficient nickel-iron alloy electrocatalysts and maximize their own advantages. In this work, a heterometallic nickel-iron cluster (L = C 64 H 66 Fe 4 N 8 Ni 2 O 19 ) of Schiff base (LH 3  = 2-amino-1,3-propanediol salicylaldehyde) is designed as a precursor to explore its behavior in the pyrolysis process under inert atmosphere. The combination of TG-MS, morphology, and X-ray characterization techniques shows that the Schiff base ligands in the heterometallic clusters produces a strong reductive atmosphere during pyrolysis, which enable the two 3d metals Ni and Fe to form NiFe alloys. Moreover, Fe 2 O 3 /Fe 0.64 Ni 0.36 @Cs carbon nanomaterials are formed, in which Fe 2 O 3 /Fe 0.64 Ni 0.36 is the potential active material for OER. It is also found that the centrosymmetric structure of the heterometallic Schiff base precursor is potentially related to the formation of the Fe 2 O 3 /Fe 0.64 Ni 0.36 alloy@carbon structures. The Fe 2 O 3 /Fe 0.64 Ni 0.36 @C-800 provides 274 mV overpotential in 1 m KOH solution at 10 mA cm -2 in OER. This work provides an effective basis for further research on Schiff base bimetallic doping-derived carbon nanomaterials as excellent OER electrocatalysts., (© 2023 Wiley-VCH GmbH.)

Renewable H 2 production by water electrolysis has attracted much attention due to its numerous advantages. However, the energy consumption of conventional water electrolysis is high and mainly driven by the kinetically inert anodic oxygen evolution reaction. An alternative approach is the coupling of different half-cell reactions and the use of redox mediators. In this review, we, therefore, summarize the latest findings on innovative electrochemical strategies for H 2 production. First, we address redox mediators utilized in water splitting, including soluble and insoluble species, and the corresponding cell concepts. Second, we discuss alternative anodic reactions involving organic and inorganic chemical transformations. Then, electrochemical H 2 production at both the cathode and anode, or even H 2 production together with electricity generation, is presented. Finally, the remaining challenges and prospects for the future development of this research field are highlighted., (© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

In this work, an efficient visible light promoted aerobic dehydro-coupling of amines, oxidation of thioethers and hydroxylation of arylboronic acids under benign conditions by using pyrene-based donor-acceptor (D-A) conjugated organic molecules was described. Donor-acceptor structure influences their π-conjugation and band gap a lot, and thereby enhances their visible light absorption ability, single electron transfer and oxidative behaviors. Alkynyl units in PS-IV play a crucial role in the catalyst which could serve as electron transferring bridge to strengthen electron delocalization, thus facilitating the single electron transfer from photosensitizer to substrates, and making it an efficient ⋅O 2 - generator. While PS-III without alkynyl units tends to produce 1 O 2 . Therefore, these molecules can serve as efficient catalysts for different kinds of visible-light-induced aerobic organic reactions. More importantly, the simply structured molecule is insoluble and stable in various solvents, and thus could be recycled as heterogeneous catalyst for many rounds with slight catalytic activity degradation. Besides, large scale (1 mol) reaction of benzylamine coupling proceeded smoothly under the standard conditions., (© 2022 Wiley-VCH GmbH.)