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Chemically powered colloidal motors are self-propelled tiny machines capable of converting chemical energy into mechanical work or kinetic energy. A wide variety of organic or inorganic substrates are selectively utilized as consumable fuels that would allow the creation of a gradient of chemical concentration via catalytic reactions for driving controllable transport in various complex liquid environments, unlocking the potential of chemically powered colloidal motors in a large range of applications. Recently, combinations of synthetic chemistry and nanotechnology have been exploited to design and construct degradable polymer-fueled artificial colloidal motors whose chemically powered propulsion relies on a rapid degradation of stimuli-responsive polymers with labile units in the nanostructured smart colloidal systems under the activation of various physical or chemical stimuli. This review highlights the most recent advances in artificial colloidal motors powered by degradable polymer fuels. It explores the general fabrication approaches to degradable polymer-fueled colloidal motors with asymmetric morphologies and the powering mechanisms of physical or chemical stimuli-responsive polymer degradation toward the self-propelled motion in liquid media and biological microenvironments. The distinct application performance of degradable polymer-fueled colloidal motors developed so far is reviewed. A future perspective on the development of degradable polymer-fueled colloidal motors is also proposed., (© 2025 Wiley‐VCH GmbH.)

Quantum dots (QDs) with multiple exciton generation are identified as one of the most competitive candidates for highly efficient solar-to-chemical energy conversion, yet not well recognized in excellent CO 2 photoreduction activity due to the agglomeration and exciton effect. Here, taking Zn 0.5 Cd 0.5 S QDs (ZCS QDs) as an example, ferroelectric BaTiO 3 (BTO) with high-energy state polarization charges is introduced to dynamically tune the properties of interfacial charges, achieving self-adaptive electrostatic adsorption of QDs and intensive photogenerated charge separation. Meanwhile, in synergy with the Z-scheme ZCS QDs/BTO heterojunction, carrier recombination is further inhibited. Such a subtle charge modulation exhibits an exceptional improvement in CO 2 photoreduction, reaching CO yields that are 15.06 times and 2.13 times those of the pure BTO and ZCS QDs, respectively. Notably, there is a remarkable 8.67 times further increase in CO yield for external polarization. The validity of the polarization charges modulating strategy for boosting CO yield is further demonstrated using the double-layer capacitance (C dl ) and in situ Fourier transform infrared spectroscopy. This study shows great promise for ferroelectric materials in CO 2 photoreduction., (© 2025 Wiley‐VCH GmbH.)

Engineering nanomaterials at single-atomic sites can enable unprecedented catalytic properties for broad applications, yet it remains challenging to do so on RuO 2 -based electrocatalysts for proton exchange membrane water electrolyzer (PEMWE). Herein, the rational design and construction of Bi-RuO 2 single-atom alloy oxide (SAAO) are presented to boost acidic oxygen evolution reaction (OER), via phase engineering a novel hexagonal close packed (hcp) RuBi single-atom alloy. This Bi-RuO 2 SAAO electrocatalyst exhibits a low overpotential of 192 mV and superb stability over 650 h at 10 mA cm -2 , enabling a practical PEMWE that needs only 1.59 V to reach 1.0 A cm -2 under industrial conditions. Operando differential electrochemical mass spectroscopy analysis, coupled with density functional theory studies, confirmed the adsorbate-evolving mechanism on Bi-RuO 2 SAAO and that the incorporation of Bi 1 improves the activity by electronic density optimization and the stability by hindering surface Ru demetallation. This work not only introduces a new strategy to fabricate high-performance electrocatalysts at atomic-level, but also demonstrates their potential use in industrial electrolyzers., (© 2025 Wiley‐VCH GmbH.)

The confining effect is essential to regulate the activity and stability of single-atom catalysts (SACs), but the universal fabrication of confined SACs is still a great challenge. Here, various lattice-confined Pt SACs supported by different carriers are constructed by a universal co-reduction approach. Notably, Pt single atoms confined in the lattice of Ni(OH) 2 (Pt 1 /Ni(OH) 2 ) with a high electron-deficient state exhibit excellent activity for basic hydrogen evolution reaction (HER). Specifically, Pt 1 /Ni(OH) 2 just requires 15 mV to get 10 mA cm -2 and the mass activity of Pt 1 /Ni(OH) 2 is 15 times of commercial Pt/C. Moreover, Pt 1 /Ni(OH) 2 assembled in an alkaline water electrolyzer shows 1030 h durability under the industrial current density of 800 mA cm -2 . In situ spectroscopy techniques reveal Pt─H and "free" OH radical can be directly observed for Pt 1 /Ni(OH) 2 , confirming the lattice-confined Pt single atoms play a key role during HER. Further density functional theory uncovers the Pt 3d orbital strongly hybridizes with O 2p and Ni 3d orbitals in Ni(OH) 2 , which quickly optimizes the electronic state of the Pt site, thus largely reducing the energy barrier of the rate-determining step to 0.16 eV for HER. Finally, this synthesis method is extended to construct other 9 lattice-confined SACs., (© 2025 Wiley‐VCH GmbH.)

Photoelectrochemical (PEC) water splitting is a top green tech for renewable energy, turning solar power into storable hydrogen. The efficiency of PEC water splitting is constrained by charge separation and surface reactions. While traditional material modifications like heterojunction design and defect regulation have enhanced efficiency, they are limited by material properties. The ferroelectric material provides a novel strategy to address these limitations in PEC water splitting. Ferroelectric materials, with their spontaneous polarization, can enhance charge separation and regulate surface reactions in PEC water splitting via internal electric fields. This paper summarizes the mechanism of ferroelectric polarization and its role in PEC, especially how ferroelectric polarization promotes bulk charge separation and surface reactions. It also reviews the research progress made in recent years regarding the enhancement of PEC performance through ferroelectric polarization. This includes applications in two main aspects: charge separation, which involves pure ferroelectrics, ferroelectric-semiconductor heterojunctions, and ferroelectric-plasmonic structures; and surface reactions, which cover electronic structure modification, pH regulation, and nanostructures. Studies have shown that ferroelectric polarization can significantly improve the charge separation efficiency and optimize the surface reaction kinetics by regulating the interfacial energy band structure. Finally, the future development of this promising research field is prospected., (© 2025 Wiley‐VCH GmbH.)

Chiral macrocycles have recently emerged as promising materials for enantioselective recognition, asymmetric catalysis, and circularly polarized luminescence (CPL) due to their terminal-free structure, preorganized chiral cavities, and unique host-guest and self-assembly properties. This review summarizes recent advances in the design and synthesis of chiral macrocycles with central, axial, helical, and planar chirality, each imparting distinct structural and chiroptical characteristics. We highlight key strategies for constructing these macrocycles and their applications in optoelectronic and catalytic systems. Emphasis is placed on the balance between rigidity and flexibility in macrocycle design, essential for effective molecular recognition, adaptable catalysis, and CPL. We conclude with perspectives on future opportunities, anticipating ongoing developments in chiral macrocycle research., (© 2025 Wiley-VCH GmbH.)

Lithium batteries, favored for their high energy density and long lifespan, are staples in electric vehicles, portable electronics, and aerospace. A key component, Li salts, aids lithium ion migration and electrode protection, significantly impacting battery performance. Developing an ideal Li salt, balancing stability, solubility, dissociation, solvation, and eco-friendliness, remains challenging. Given the scarcity of relevant reviews, it is endeavored here to present a novel perspective on Li salt chemistry, offering a concise roadmap for future designs and innovations. It is delved into the trends, opportunities, design principles, and evaluation methodologies related to Li salt chemistry, with a particular emphasis on organic anionic compositions. Furthermore, the latest and most representative organic Li salts from their intrinsic structure and coordination chemistry, highlighting their unique features and contributions are organized and presented. Finally, a visionary outlook is articulated for this field, exploring avenues, such as customizing Li salts for specific applications, synthesizing Li salts on demand, and discussing the potential of F-free Li salts alongside with their electrochemical window challenges. Here it is served as a strategic compass, addressing the shortcomings of existing reviews and guiding the design of functionalized Li salts., (© 2025 Wiley‐VCH GmbH.)

Ribonucleoprotein (RNP)-based CRISPR/Cas9 genome editing holds great potential for the treatment of choroidal neovascularization (CNV), which however, is challenged by the lack of efficient cytosolic protein delivery tools. Herein, reversibly-phosphorylated pro-proteins (P-proteins) with conjugated adenosine triphosphate (ATP) tags are engineered and coupled with a membrane-penetrating, guanidine-enriched, α-helical polypeptide ( L GP) to mediate robust and universal cytosolic delivery. L GP forms salt-stable nanocomplexes (NCs) with P-proteins via electrostatic interaction and salt bridging, and the helix-assisted, strong membrane activities of L GP enabled efficient cellular internalization and endolysosomal escape of NCs. Therefore, this approach allows efficient cytosolic delivery of a wide range of protein cargoes and maintains their bioactivities due to endolysosomal acidity-triggered traceless restoration of P-proteins. Notably, intravitreally delivered L GP/P-RNP NCs targeting hypoxia-inducible factor-1α (HIF-1α) induce pronounced gene disruption to downregulate pro-angiogenic factors and alleviate subretinal fibrosis, ultimately provoking robust therapeutic efficacy in CNV mice. Such a facile and versatile platform provides a powerful tool for cytosolic protein delivery and genome editing, and it holds promising potential for the treatment of CNV-associated diseases, such as age-related macular degeneration., (© 2024 Wiley‐VCH GmbH.)

With the depletion of fossil fuels and increasing pollution problems, green and sustainable energy supply attracts worldwide attention. Hydrogen is a green and high-density energy substance, and photocatalytic hydrogen generation is an effective and sustainable method. Therefore, developing high-performance photocatalysts plays a crucial role in practical application. Porous frameworks with large surface areas and diversified structures are considered promising candidates for photocatalysts. This review summarizes the recent progress on porous frameworks and their derivatives through fine-tuning structural components in terms of building monomers, functional groups, and metal hybridization for photocatalytic production of hydrogen. A detailed correlation is conducted between the structural features of porous frameworks and photocatalysis capability. In addition, we summarized the advantages of porous materials for photocatalytic hydrogen production and future development., (© 2024 Wiley-VCH GmbH.)

The application of sodium metal battery is hampered by the large volume change and uncontrollable top growth of Na metal. Herein, a dual strategy including constructing a three-dimensional gradient ZnO/Fe 0.7 Co 0.3 (ZFC) framework of decreasing sodiophilic capability from bottom to top, and imposing magnetic fields based on magnetohydrodynamic (MHD) effect, is proposed to regulate the sodium deposition/stripping behavior and realize the bottom-up deposition of Na. Therefore, the ZFC framework under a magnetic field of 200 mT exhibits high electrochemical reversibility with a Coulombic efficiency of 99.77 % at 1 mA cm -2 and 1 mAh cm -2 . Meanwhile, the ZFC composite anode (ZFC@Na) with the magnetic field of 200 mT delivers a small polarization voltage of approximately10 mV and long cycle life of more than 2500 h at 5 mA cm -2 and 5 mAh cm -2 in symmetric cells, along with good cycle stability in ZFC@Na||Na 3 V 2 (PO 4 ) 3 full cells (200 cycles at 1 C with a high capacity retention of 98 %). Accordingly, the novel strategy of combining magnetic fields and sodiophilic gradient frameworks provides a perspective to solve the issues of sodium dendrite growth., (© 2024 Wiley-VCH GmbH.)

Skull base foramen invasion (SBFI) indicates poor prognosis in nasopharyngeal carcinoma (NPC). However, only a few studies systematically assessed the role of SBFIin staging and treatment of NPC. To investigate the prognostic value of SBFI in NPC, a total of 1,752 patients with nonmetastatic NPC from two hospitals (1,320 and 432) between January 2010 and March 2014 are enrolled. The primary endpoint is overall survival (OS). Heatmap/cluster and network analyses are used to provide subclassification indication. Univariate and multivariate analyses with Kaplan-Meier method are performed to compare survival outcomes. SBFIs are classified into slight (only foramen lacerum and/or pterygopalatine fossa invasion) and severe (other SBFIs). The severe SBFI is an unfavorable prognosticator for OS in both the entire cohort and the T3 group. OS is similar between T3 with severe SBFI and T4 patients. Reclassifying T3 with severe SBFI as the T4 category yields an improved T category discrimination. Additionally, patients in the severe SBFI group gain significant survival benefits from induction chemotherapy ((IC). Therefore, T3 NPC with severe SBFI is an independent negative predictor for OS and is classified into the T4 category. T category adjustment enables better prognostic stratification. Severe SBFI benefits from IC in long-term OS., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Free-standing micro-supercapacitor (MSC) devices without substrate or current collectors are promising for practical applications. However, it is still difficult to prepare high-performance free-standing MSC devices because of the requirement of optimized active sites, conductivity, ion diffusion, controlled patterns, moisture susceptibility, etc. Here, it is proposed that the optimization of oxygen level on graphene is promising to solve these requirements because of the balance of sp 2 and sp 3 hybridization. Using the medium-oxidized graphene, the flexible, conductive, hydro-stable, easy-processing film can be facilely obtained, which facilitates the preparation of free-standing MSC electrodes. After constructing with gel electrolyte, the free-standing MSC device shows a high capacitance of 898.4 mF cm -2 using aqueous-gel electrolyte and 383.6 mF cm -2 using ion-gel electrolyte with mass loading of ca. 10 mg cm -2 . Correspondingly, the MSC device can achieve a landmark energy density of 42.6 µWh cm -2 at 0.85 mW cm -2 (7.1 mWh cm -3 at 141.7 mW cm -3 ). The advantages of high performance, facile preparation, and low inactive components make the free-standing MSC device promising for practical applications., (© 2024 Wiley‐VCH GmbH.)

Strain engineering is an effective strategy for manipulating the electronic structure of active sites and altering the binding strength toward adsorbates during the hydrogen evolution reaction (HER). However, the effects of weak and strong strain engineering on the HER catalytic activity have not been fully explored. Herein, the core-shell PdPt alloys with two-layer Pt shells (PdPt 2L ) and multi-layer Pt shells (PdPt ML ) is constructed, which exhibit distinct lattice strains. Notably, PdPt 2L with weak strain effect just requires a low overpotential of 18 mV to reach 10 mA cm -2 for the HER and shows the superior long-term stability for 510 h with negligible activity degradation in 0.5 M H 2 SO 4 . The intrinsic activity of PdPt 2L is 6.2 and 24.5 times higher than that of PdPt ML and commercial Pt/C, respectively. Furthermore, PdPt 2L ||IrO 2 exhibits superior activity over Pt/C||IrO 2 in proton exchange membrane water electrolyzers and maintains stable operation for 100 h at large current density of 500 mA cm -2 . In situ/operando measurements verify that PdPt 2L exhibits lower apparent activation energy and accelerated ad-/desorption kinetics, benefiting from the weak strain effect. Density functional theory calculations also reveal that PdPt 2L displays weaker H * adsorption energy compared to PdPt ML , favoring for H * desorption and promoting H 2 generation., (© 2024 Wiley‐VCH GmbH.)

Zinc-air batteries employing non-Pt cathodes hold significant promise for advancing cathodic oxygen reduction reaction (ORR). However, poor intrinsic electrical conductivity and aggregation tendency hinder the application of metal-organic frameworks (MOFs) as active ORR cathodes. Conductive MOFs possess various atomically dispersed metal centers and well-aligned inherent topologies, eliminating the additional carbonization processes for achieving high conductivity. Here, a novel room-temperature electrochemical cathodic electrodeposition method is introduced for fabricating uniform and continuous layered 2D bimetallic conductive MOF films cathodes without polymeric binders, employing the organic ligand 2,3,6,7,10,11-hexaiminotriphenylene (HITP) and varying the Ni/Cu ratio. The influence of metal centers on modulating the ORR performance is investigated by density functional theory (DFT), demonstrating the performance of bimetallic conductive MOFs can be effectively tuned by the unpaired 3d electrons and the Jahn-Teller effect in the doped Cu. The resulting bimetallic Ni 2.1 Cu 0.9 (HITP) 2 exhibits superior ORR performance, boasting a high onset potential of 0.93 V. Moreover, the assembled aqueous zinc-air battery demonstrates high specific capacity of 706.2 mA h g -1 , and exceptional long-term charge/discharge stability exceeding 1250 cycles., (© 2024 Wiley‐VCH GmbH.)

The seawater electrolysis to produce hydrogen is a significant topic on alleviating the energy crisis. Here, the Fe, Nb-Ni 3 S 2 catalyst is prepared by metal-doping strategy, and it shows high oxygen evolution reaction (OER) activity in alkaline medium, and only needs 1.491 V to deliver a current density of 100 mA cm -2 in simulated seawater. Using Fe, Nb-Ni 3 S 2 as a bifunctional catalyst, the two-electrode electrolyzer only requires a voltage of 1.751 V (without impedance compensation) to drive the current density of 50 mA cm -2 , and can run over 150 h stably in the simulated seawater. Importantly, In situ Raman test demonstrates that the outstanding performance of Fe, Nb-Ni 3 S 2 in simulated seawater is ascribed to the in situ formed sulfate protective layer induced by Nb doping, which can effectively inhibit the corrosion of chloride ion, while the protective layer is absent for Fe-Ni 3 S 2 . The stable operation of simulated seawater electrolysis under industrial current density further confirms the stability improvement mechanism of forming protective layer. In short, this study provides a new strategy of using Nb dopants inducing the formation of protective layer to enhance the stability of seawater electrolysis., (© 2024 Wiley‐VCH GmbH.)

Developing efficient and earth-abundant alkaline HER electrocatalysts is pivotal for sustainable energy, but co-regulating its intricate multi-step process, encompassing water dissociation, OH - desorption, and hydrogen generation, is still a great challenge. Herein, we tackle these obstacles by fabricating a vertically integrated electrode featuring a nanosheet array with prominent dual-nitride metallic heterostructures characterized by impeccable lattice matching and excellent conductivity, functioning as a multi-purpose catalyst to fine-tune the bonding affinity with alkaline HER intermediates. Detailed structural characterization and theoretical calculation elucidate that charge redistribution at the heterointerface reduces the O p-W d and H s-W d interactions vs. single nitride, thereby enhancing OH - transfer and H 2 release. As anticipated, the resulting WN-NiN/CFP catalyst demonstrates a gratifying low overpotential of 36.8 mV at 10 mA/cm 2 for alkaline HER, while concurrently maintaining operational stability for 1300 h at 100 mA/cm 2 for overall water splitting. This work presents an effective approach to meticulously optimize multiple site-intermediate interactions in alkaline HER, laying the foundation for efficient energy conversion., (© 2024 Wiley-VCH GmbH.)

Dual-atom catalysts (DACs) with atomically dispersed dual-sites, as an extension of single-atom catalysts (SACs), have recently become a new hot topic in heterogeneous catalysis due to their maximized atom efficiency and dual-site diverse synergy, because the synergistic diversity of dual-sites achieved by asymmetric microenvironment tailoring can efficiently boost the catalytic activity by optimizing the electronic structure of DACs. Here, this work first summarizes the frequently-used experimental synthesis and characterization methods of DACs. Then, four synergistic catalytic mechanisms (cascade mechanism, assistance mechanism, co-adsorption mechanism and bifunction mechanism) and four key modulating methods (active site asymmetric strategy, transverse/axial-modification engineering, distance engineering and strain engineering) are elaborated comprehensively. The emphasis is placed on the effects of asymmetric microenvironment of DACs on oxygen/carbon dioxide reduction reaction. Finally, some perspectives and outlooks are also addressed. In short, the review summarizes a useful asymmetric microenvironment tailoring strategy to speed up synthesis of high-performance electrocatalysts for different reactions., (© 2024 Wiley‐VCH GmbH.)

Decoration of an axial coordination ligand (ACL) on the active metal site is a highly effective and versatile strategy to tune activity of single-atom catalysts (SACs). However, the regulation mechanism of ACLs on SACs is still incompletely known. Herein, we investigate diversified combinations of ACL-SACs, including all 3d-5d transition metals and ten prototype ACLs. We identify that ACLs can weaken the adsorption capability of the metal atom (M) by raising the bonding energy levels of the M-O bond while enhancing dispersity of the d orbital of M. Through examination of various local configurations and intrinsic parameters of ACL-SACs, a general structure descriptor σ is constructed to quantify the structure-activity relationship of ACL-SACs which solely based on a few key intrinsic features. Importantly, we also identified the axial ligand descriptor σ ACL , as a part of σ, which can serve as a potential descriptor to determine the rate-limiting steps (RLS) of ACL-SACs in experiment. And we predicted several ACL-SACs, namely, CrN 4 -, FeN 4 -, CoN 4 -, RuN 4 -, RhN 4 -, OsN 4 -, IrN 4 - and PtN 4 -ACLs, that entail markedly higher activities than the benchmark catalysts of Pt and IrO 2 for oxygen reduction reaction and oxygen evolution reaction, respectively, thereby supporting that the general descriptor σ can provide a simple and cost-effective method to assess efficient electrocatalysts., (© 2024 Wiley-VCH GmbH.)

The existing electronic waste (e-waste) and leaching solutions generated by industries accumulate significant amounts of gold (Au), even in excess of those in natural minerals. Therefore, the recycling of Au is extremely significant for the potential sustainability of chemical industry. By designing ionic covalent organic frameworks (COFs), here we synthesize a series of Ionic-COF-X (X=Cl - , Br - , AcO - , and SO 4 2- ) by anion regulation strategy and further explore their adsorption performance towards Au recovery. All these ionic COFs exhibit ultrahigh gold adsorption efficiency and excellent regeneration. Moreover, anion regulation could indeed affect the Au capture performance. In particular, when Cl - ions serve as counter ions, the Au capacity of Ionic-COF-Cl could reach 1270.8 mg g -1 . Moreover, in the actual CPU leaching solution test, the selectivity of Ionic-COF-Cl towards Au 3+ ion hits 39000 and 4600 times higher than that of Cu 2+ and Ni 2+ ions, respectively, suggesting that the Ionic-COF-Cl is a promising material for highly selective recovering gold from actual e-waste. DFT calculations further reveal that counter ions can regulate the adsorption affinity of ionic COF framework toward Au. In short, this work provides a useful anion regulation strategy to design ionic COFs as a promising platform for gold selective recovery from actual e-waste., (© 2024 Wiley-VCH GmbH.)

Developing efficient electrocatalysts for water splitting is of great significance for realizing sustainable energy conversion. In this work, Ru sub-nanoclusters anchored on cobalt-nickel bimetallic phosphides (Ru-CoP/Ni 2 P) are constructed by an interfacial confinement strategy. Remarkably, Ru-CoP/Ni 2 P with low noble metal loading (33.1 µg cm -2 ) shows superior activity for hydrogen evolution reaction (HER) in all pH values, whose turnover frequency (TOF) is 8.7, 15.3, and 124.7 times higher than that of Pt/C in acidic, alkaline, and neutral conditions, respectively. Meanwhile, it only requires the overpotential of 171 mV@10 mA cm -2 for oxygen evolution reaction (OER) and corresponding TOF is 20.3 times higher than that of RuO 2 . More importantly, the Ru-CoP/Ni 2 P||Ru-CoP/Ni 2 P displays superior mass activity of 4017 mA mg noble metal -1 at 2.0 V in flowing alkaline water electrolyzer, which is 105.1 times higher than that of Pt/C||IrO 2 . In situ Raman spectroscopy demonstrates that the Ru sites in Ru-CoP/Ni 2 P play a key role for water splitting and follow the adsorption evolution mechanism toward OER. Further mechanism studies disclose the confined Ru atom contributes to the desorption of H 2 during HER and the formation of O-O bond during OER, leading to fast reaction kinetics. This study emphasizes the importance of interface confinement for enhancing electrocatalytic activity., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Periodontitis is the leading cause of adult tooth missing. Thorny bacterial biofilm and high reactive oxygen species (ROS) levels in tissue are key elements for the periodontitis process. It is meaningful to develop an advanced therapeutic system with sequential antibacterial/ antioxidant ability to meet the overall goals of periodontitis therapy. Herein, a dual-polymer functionalized melanin-AgNPs (P/D-MNP-Ag) with biofilm penetration, hydroxyapatite binding, and sequentially treatment ability are fabricated. Polymer enriched with 2-(Dimethylamino)ethyl methacrylate (D), can be protonated in an acid environment with enhanced positive charge, promoting penetration in biofilm. The other polymer is rich in phosphate group (P) and can chelate Ca 2+ , promoting the polymer to adhere to the hydroxyapatite surface. Melanin has good ROS scavenging and photothermal abilities, after in situ reduction Ag, melanin-AgNPs composite has sequentially transitioned between antibacterial and antioxidative ability due to heat and acid accelerated Ag + release. The released Ag + and heat have synergistic antibacterial effects for bacterial killing. With Ag + consumption, the antioxidant ability of MNP recovers to scavenge ROS in the inflammatory area. When applied in the periodontitis model, P/D-MNP-Ag has good therapeutical effects to ablate biofilm, relieve inflammation state, and reduce alveolar bone loss. P/D-MNP-Ag with sequential treatment ability provides a reference for developing advanced oral biofilm eradication systems., (© 2024 Wiley‐VCH GmbH.)

Parasitic side reactions and dendrites formation hinder the application of aqueous zinc ion batteries due to inferior cycling life and low reversibility. Against this background, N-methyl formamide (NMF), a multi-function electrolyte additive is applied to enhance the electrochemical performance. Studied via advanced synchrotron radiation spectroscopy and DFT calculations, the NMF additive simultaneously modifies the Zn 2+ solvation structure and ensures uniform zinc deposition, thus suppressing both parasitic side reactions and dendrite formation. More importantly, an ultralong cycling life of 3115 h in the Zn||Zn symmetric cell at a current density of 0.5 mA cm -2 is achieved with the NMF additive. Practically, the Zn||PANI full cell utilizing NMF electrolyte shows better rate and cycling performance compared to the pristine ZnSO 4 aqueous electrolyte. This work provides useful insights for the development of high-performance aqueous metal batteries., (© 2024 Wiley‐VCH GmbH.)

Self-assembling peptides have numerous applications in medicine, food chemistry, and nanotechnology. However, their discovery has traditionally been serendipitous rather than driven by rational design. Here, HydrogelFinder, a foundation model is developed for the rational design of self-assembling peptides from scratch. This model explores the self-assembly properties by molecular structure, leveraging 1,377 self-assembling non-peptidal small molecules to navigate chemical space and improve structural diversity. Utilizing HydrogelFinder, 111 peptide candidates are generated and synthesized 17 peptides, subsequently experimentally validating the self-assembly and biophysical characteristics of nine peptides ranging from 1-10 amino acids-all achieved within a 19-day workflow. Notably, the two de novo-designed self-assembling peptides demonstrated low cytotoxicity and biocompatibility, as confirmed by live/dead assays. This work highlights the capacity of HydrogelFinder to diversify the design of self-assembling peptides through non-peptidal small molecules, offering a powerful toolkit and paradigm for future peptide discovery endeavors., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Modulating the chemical composition and structure has been considered as one of the most promising strategies for developing high-efficient water splitting catalysts. Here, a single-atom Ru doped Ni 2 P/Fe 3 P catalyst is synthesized by introducing the dispersed Ru atoms to adjust Ni 2 P/Fe 3 P heterostructure. Single atom Ru provides effective hydrogen evolution reaction (HER) active sites for boosting catalytic activities. The catalyst with only 0.2 wt.% content of Ru exhibits an overpotential of 19.3 mV at 10 mA cm -2 , which is obviously lower than 146.1 mV of Ni 2 P/Fe 3 P. Notably, an alkaline overall water electrolyzer based on Ru-Ni 2 P/Fe 3 P catalysts achieves a cell voltage of 1.47 V and operates over 600 h at 10 mA cm -2 , which is superior to that of benchmark RuO 2 //Pt/C (1.61 V). The theoretical calculations further confirm that Ru single atom doping can effectively optimize the hydrogen/water adsorption free energy of the active site and therefore improve the HER activity of heterostructure. This work provides a valuable reference to design high-activity and durability catalyst for water splitting through the double modulation of interface-effect and atomic doping., (© 2024 Wiley‐VCH GmbH.)

The poor bulk-phase and interphase stability, attributable to adverse internal stress, impede the cycling performance of silicon microparticles (µSi) anodes and the commercial application for high-energy-density lithium-ion batteries. In this work, a groundbreaking gradient-hierarchically ordered conductive (GHOC) network structure, ingeniously engineered to enhance the stability of both bulk-phase and the solid electrolyte interphase (SEI) configurations of µSi, is proposed. Within the GHOC network architecture, two-dimensional (2D) transition metal carbides (Ti 3 C 2 T x ) act as a conductive "brick", establishing a highly conductive inner layer on µSi, while the porous outer layer, composed of one-dimensional (1D) Tempo-oxidized cellulose nanofibers (TCNF) and polyacrylic acid (PAA) macromolecule, functions akin to structural "rebar" and "concrete", effectively preserves the tightly interconnected conductive framework through multiple bonding mechanisms, including covalent and hydrogen bonds. Additionally, Ti 3 C 2 T x enhances the development of a LiF-enriched SEI. Consequently, the µSi-MTCNF-PAA anode presents a high discharge capacity of 1413.7 mAh g -1 even after 500 cycles at 1.0 C. Moreover, a full cell, integrating LiNi 0.8 Mn 0.1 Co 0.1 O 2 with µSi-MTCNF-PAA, exhibits a capacity retention rate of 92.0% following 50 cycles. This GHOC network structure can offer an efficacious pathway for stabilizing both the bulk-phase and interphase structure of anode materials with high volumetric strain., (© 2024 Wiley‐VCH GmbH.)

Developing efficient metal-free catalysts to directly synthesize hydrogen peroxide (H 2 O 2 ) through a 2-electron (2e) oxygen reduction reaction (ORR) is crucial for substituting the traditional energy-intensive anthraquinone process. Here, in-plane topological defects enriched graphene with pentagon-S and pyrrolic-N coordination (SNC) is synthesized via the process of hydrothermal and nitridation. In SNC, pentagon-S and pyrrolic-N originating from thiourea precursor are covalently grafted onto the basal plane of the graphene framework, building unsymmetrical dumbbell-like S─C─N motifs, which effectively modulates atomic and electronic structures of graphene. The SNC catalyst delivers ultrahigh H 2 O 2 productivity of 8.1, 7.3, and 3.9 mol g catalyst -1  h -1 in alkaline, neutral, and acidic electrolytes, respectively, together with long-term operational stability in pH-universal electrolytes, outperforming most reported carbon catalysts. Theoretical calculations further unveil that defective S─C─N motifs efficiently optimize the binding strength to OOH * intermediate and substantially diminish the kinetic barrier for reducing O 2 to H 2 O 2 , thereby promoting the intrinsic activity of 2e-ORR., (© 2024 Wiley‐VCH GmbH.)

Covalent organic frameworks (COFs) have recently shown great potential for photocatalytic hydrogen production. Currently almost all reports are focused on two-dimensional (2D) COFs, while the 3D counterparts are rarely explored due to their non-conjugated frameworks derived from the sp 3 carbon based tetrahedral building blocks. Here, we rationally designed and synthesized a series of fully conjugated 3D COFs by using the saddle-shaped cyclooctatetrathiophene derivative as the building block. Through molecular engineering strategies, we thoroughly discussed the influences of key factors including the donor-acceptor structure, hydrophilicity, specific surface areas, as well as the conjugated/non-conjugated structures on their photocatalytic hydrogen evolution properties. The as-synthesized fully conjugated 3D COFs could generate the hydrogen up to 40.36 mmol h -1  g -1 . This is the first report on intrinsic metal-free 3D COFs in photocatalytic hydrogen evolution application. Our work provides insight on the structure design of 3D COFs for highly-efficient photocatalysis, and also reveals that the semiconducting fully conjugated 3D COFs could be a useful platform in clear energy-related fields., (© 2024 Wiley-VCH GmbH.)

Layered Li-rich oxide cathode materials are capable of offering high energy density due to their cumulative cationic and anionic redox mechanism during (de)lithiation process. However, the structural instability of the layered Li-rich oxide cathode materials, especially in the deeply delitiated state, results in severe capacity and voltage degradation. Considering the minimal isotropic structural evolution of disordered rock salt oxide cathode during cycling, cation-disordered nano-domains have been controllably introduced into layered Li-rich oxides by co-doping of d 0 -TM and alkali ions. Combining electrochemical and synchrotron-based advanced characterizations, the incorporation of the phase-compatible cation-disordered domains can not only hinder the oxygen framework collapse along the c axis of layered Li-rich cathode under high operation voltage but also promote the Mn and anionic activities as well as Li + (de)intercalation kinetics, leading to remarkable improvement in rate capability and mitigation of capacity and voltage decay. With this unique layered/rocksalt intergrown structure, the intergrown cathode yields an ultrahigh capacity of 288.4 mAh g -1 at 0.1 C, and outstanding capacity retention of ≈90.0% with obviously suppressed voltage decay after 100 cycles at 0.5, 1, and 2 C rate. This work provides a new direction toward advanced cathode materials for next-generation Li-ion batteries., (© 2024 Wiley‐VCH GmbH.)

The rechargeable aqueous Zn||MnO 2 chemistry has been extensively explored, but its electrochemical reaction mechanisms, especially in the context of MnO 2 /Mn 2+ conversion and Zn 2+ /H + intercalation chemistry, remain not fully understood. Here, we designed an amphiphilic hydrogel electrolyte, which distinguished the MnO 2 /Mn 2+ conversion, Zn 2+ intercalation, and H + intercalation and conversion processes at three distinct discharge plateaus of an aqueous Zn||MnO 2 battery. The amphiphilic hydrogel electrolyte is featured with an extended electrochemical stability window up to 3.0 V, high ionic conductivity, Zn 2+ -selective ion tunnels, and hydrophobic associations with cathode materials. This specifically designed electrolyte allows the MnO 2 /Mn 2+ conversion reaction at a discharge plateau of 1.75 V. More interesting, the discharge plateaus of ~1.33 V, previously assigned as the co-intercalation of Zn 2+ and H + ions in the MnO 2 cathode, are specified as the exclusive intercalation of Zn 2+ ions, leading to an ultra-flat voltage plateau. Furthermore, with a distinct three-step electrochemical energy storage process, a high areal capacity of 1.8 mAh cm -2 and high specific energy of 0.858 Wh cm -2 , even at a low MnO 2 loading mass of 0.5 mg cm -2 are achieved. To our knowledge, this is the first report to fully distinguish different mechanisms at different potentials in aqueous Zn||MnO 2 batteries., (© 2024 Wiley-VCH GmbH.)

Rigid three-dimensional (3D) polycyclic propellanes have garnered interest due to their unique conformational spaces, which display great potential use in selectivity, separation and as models to study through-space electronic interactions. Herein we report the synthesis of a novel rigid propellane, trinaphtho[3.3.3]propellane triimide, which comprises three imide groups embedded on a trinaphtho[3.3.3]propellane. This propellane triimide exhibits large bathochromic shift, amplified molar absorptivity, enhanced fluorescence, and lower reduction potential when compared to the subunits. Computational and experimental studies reveal that the effective through-space π-orbitals interacting (homoconjugation) occurs between the subunits. Single-crystal XRD analysis reveals that the propellane triimide has a highly quasi-D 3h symmetric skeleton and readily crystallizes into different superstructures by changing alkyl chains at the imide positions. In particular, the porous 3D superstructure with S-shaped channels is promising for taking up ethane (C 2 H 6 ) with very good selectivity over ethylene (C 2 H 4 ), which can purify C 2 H 4 from C 2 H 6 /C 2 H 4 in a single separation step. This work showcases a new class of rare 3D polycyclic propellane with intriguing electronic and supramolecular properties., (© 2024 Wiley‐VCH GmbH.)

Constructing structural defects is a promising way to enhance the catalytic activity toward the hydrogen evolution reaction (HER). However, the relationship between defect density and HER activity has rarely been discussed. In this study, a series of Pt/WO x nanocrystals are fabricated with controlled morphologies and structural defect densities using a facile one-step wet chemical method. Remarkably, compared with polygonal and star structures, the dendritic Pt/WO x (d-Pt/WO x ) exhibited a richer structural defect density, including stepped surfaces and atomic defects. Notably, the d-Pt/WO x catalyst required 4 and 16 mV to reach 10 mA cm -2 , and its turnover frequency (TOF) values are 11.6 and 22.8 times higher than that of Pt/C under acidic and alkaline conditions, respectively. In addition, d-Pt/WO x //IrO 2 displayed a mass activity of 5158 mA mg Pt -1 system. Further mechanistic studies suggested that the d-Pt/WO 2 system. Further mechanistic studies suggested that the d-Pt/WO x exhibited reduced number of antibonding bands and the lowest dz 2 -band center of d-Pt/WO 2 -band center of d-Pt/WO x facilitated the adsorption of hydrogen from water molecules and water dissociation in alkaline medium. This work emphasizes the key role of the defect density in improving the HER activity of electrocatalysts., (© 2023 Wiley‐VCH GmbH.)

Designing robust bifunctional catalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction in all-pH conditions for overall water splitting (OWS) is an effective way to achieve sustainable development. Herein, a composite Ru-VO 2 containing Ru-doped VO 2 and Ru nanoparticles (NPs) is synthesized, and it shows a high OWS performance in full-pH range due to their synergist effect. In particular, the OER mass activities of Ru-VO 2 at 1.53 V (vs RHE) in acidic, alkaline, and PBS solutions are ≈65, 36, and 235 times of commercial RuO 2 in the same conditions. The "Ru-VO 2 || Ru-VO 2 " two-electrode electrolyzer only needs a voltage of 1.515 V (at 10 mA cm -2 ) in acidic water splitting, which can operate stably for 125 h at 10 mA cm -2 without significant voltage decay. In situ Raman spectra and in situ differential electrochemical mass spectrometry prove that the OER of Ru-VO 2 in acid follows the adsorption evolution mechanism. Density functional theory calculations further reveal the synergistic effect between Ru NP and Ru-doped VO 2 , which breaks the hydrogen bond network formed by *OH adsorbed on the Ru single-atom site, and thereby significantly enhances the OER activity. This work provides new insights into the design of novel bifunctional pH-universal catalysts for OWS., (© 2023 Wiley-VCH GmbH.)

The pursuit of high-performance batteries has propelled the investigation into advanced materials and design methodologies. Herein, the yolk-shell MnSe/ZnSe heterojunction encapsulated in hollow carbontubes (MnSe/ZnSe@HCTs) is prepared as a prospective electrode material for sodium/potassium batteries. The band structure in the heterojunction is methodically adjusted and regulated by intentionally utilizing Mn with unpaired electrons in the 3d orbital. The ZnSe shell confer effectively mitigates volumetric expansion challenges inherent in ions insertion/extraction processes and 1D carbontubular conductive substrate avert the aggregation of MnSe/ZnSe nanoparticles. Concurrently, the heterojunctions implantation induces sublattice distortion and charge redistribution, enriching active sites and regulating band structure. The selenium vacancies within these heterojunctions contribute to the provision of abundant active sites, thereby promoting efficient ions insertion/extraction. In sodium-ion batteries (SIBs), MnSe/ZnSe@HCTs present a superior capacity of 475 mA hg -1 at 0.1 A g -1 and sustains a capacity of 408.5 mAh g -1 even after 1000 cycles. In potassium-ion batteries (KIBs), MnSe/ZnSe@HCTs deliver a higher specific capacity of 422 mAh g -1 at a current density of 0.1 A g -1 and maintain a high coulombic efficiency of 99% after 1000 cycles. The yolk-shell structured MnSe/ZnSe heterojunction demonstrates excellent electrode properties for high-performance sodium/potassium batteries, holding significant promise for future energy storage applications., (© 2023 Wiley-VCH GmbH.)

Epidermal dry electrodes with high skin-compliant stretchability, low bioelectric interfacial impedance, and long-term reliability are crucial for biopotential signal recording and human-machine interaction. However, incorporating these essential characteristics into dry electrodes remains a challenge. Here, a skin-conformal dry electrode is developed by encapsulating kirigami-structured poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)/polyvinyl alcohol (PVA)/silver nanowires (Ag NWs) film with ultrathin polyurethane (PU) tape. This Kirigami-structured PEDOT:PSS/PVA/Ag NWs/PU epidermal electrode exhibits a low sheet resistance (≈3.9 Ω sq -1 ), large skin-compliant stretchability (>100%), low interfacial impedance (≈27.41 kΩ at 100 Hz and ≈59.76 kΩ at 10 Hz), and sufficient mechanoelectrical stability. This enhanced performance is attributed to the synergistic effects of ionic/electronic current from PEDOT:PSS/Ag NWs dual conductive network, Kirigami structure, and unique encapsulation. Compared with the existing dry electrodes or standard gel electrodes, the as-prepared electrodes possess lower interfacial impedance and noise in various conditions (e.g., sweat, wet, and movement), indicating superior water/motion-interference resistance. Moreover, they can acquire high-quality biopotential signals even after water rinsing and ultrasonic cleaning. These outstanding advantages enable the Kirigami-structured PEDOT:PSS/PVA/Ag NWs/PU electrodes to effectively monitor human motions in real-time and record epidermal biopotential signals, such as electrocardiogram, electromyogram, and electrooculogram under various conditions, and control external electronics, thereby facilitating human-machine interactions., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

The semiconducting properties and applications of three dimensional (3D) covalent organic frameworks (COFs) are greatly hampered because of their long-ranged non-conjugated skeletons and relatively unstable linkages. Here, a robust imidazole-linked fully conjugated 3D covalent organic framework (BUCT-COF-7) is synthesized through the one-pot multicomponent Debus-Radziszewski reaction of the saddle-shaped aldehyde-substituted cyclooctatetrathiophene, pyrene-4,5,9,10-tetraone, and ammonium acetate. The semiconducting BUCT-COF-7, as a metal-free catalyst, shows excellent two electron oxygen reduction reaction (ORR) activity in alkaline medium with high hydrogen peroxide (H 2 O 2 ) selectivity of 83.4 %. When the BUCT-COF-7 as cathode catalyst is assembled into the electrolyzer, the devices showed high electrochemical production rate of H 2 O 2 up to 326.9 mmol g -1 h -1 . The accumulative amount of H 2 O 2 could totally degrade the dye methylene blue via Fenton reaction for wastewater treatment. This is the first report about intrinsic 3D COFs for efficient electrochemical synthesis of H 2 O 2 , revealing the promising applications of fully conjugated 3D COFs in the environment-related field., (© 2023 Wiley-VCH GmbH.)

Van der Waals (vdW) metal-semiconductor junctions (MSJs) exhibit huge potential to reduce the contact resistance and suppress the Fermi-level pinning (FLP) for improving the device performance, but they are limited by optional (2D) metals with a wide range of work functions. Here a new class of vdW MSJs entirely composed of atomically thin MXenes is reported. Using high-throughput first-principles calculations, highly stable 80 metals and 13 semiconductors are screened from 2256 MXene structures. The selected MXenes cover a broad range of work functions (1.8-7.4 eV) and bandgaps (0.8-3 eV), providing a versatile material platform for constructing all-MXene vdW MSJs. The contact type of 1040 all-MXene vdW MSJs based on Schottky barrier heights (SBHs) is identified. Unlike conventional 2D vdW MSJs, the formation of all-MXene vdW MSJs leads to interfacial polarization, which is responsible for the FLP and deviation of SBHs from the prediction of Schottky-Mott rule. Based on a set of screening criteria, six Schottky-barrier-free MSJs with weak FLP and high carrier tunneling probability (>50%) are identified. This work offers a new way to realize vdW contacts for the development of high-performance electronic and optoelectronic devices., (© 2023 Wiley-VCH GmbH.)

The limited availability of effective agents for removing actinides from the lungs significantly restricts the effectiveness of medical treatments for nuclear emergencies. Inhalation is the primary route of internal contamination in 44.3% of actinide-related accidents, leading to the accumulation of radionuclides in the lungs and resulting in infections and potential tumor formation (tumorigenesis). This study focuses on the synthesis of a nanometal-organic framework (nMOF) material called ZIF-71-COOH, which is achieved by post-synthetic carboxyl functionalization of ZIF-71. The material demonstrates high and selective adsorption of uranyl, while also exhibiting increased particle size (≈2100 nm) when it aggregates in the blood, enabling passive targeting of the lungs through mechanical filtration. This unique property facilitates the rapid enrichment and selective recognition of uranyl, making nano ZIF-71-COOH highly effective in removing uranyl from the lungs. The findings of this study highlight the potential of self-aggregated nMOFs as a promising drug delivery system for targeted uranium decorporation in the lungs., (© 2023 Wiley-VCH GmbH.)

High-capacity silicon has been regarded as one of the most promising anodes for high-energy lithium-ion batteries. However, it suffers from severe volume expansion, particle pulverization, and repeated solid electrolyte interphase (SEI) growth, which leads to rapid electrochemical failure, while the particle size also plays key role here and its effects remain elusive. In this paper, through multiple-physical, chemical, and synchrotron-based characterizations, the evolutions of the composition, structure, morphology, and surface chemistry of silicon anodes with the particle size ranging from 50 to 5 µm upon cycling are benchmarked, which greatly link to their electrochemical failure discrepancies. It is found that the nano- and micro-silicon anodes undergo similar crystal to amorphous phase transition, but quite different composition transition upon de-/lithiation; at the same time, the nano- and 1 µm-silicon samples present obviously different mechanochemical behaviors from the 5 µm-silicon sample, such as electrode crack, particle pulverization/crack as well as volume expansion; in addition, the micro-silicon samples possess much thinner SEI layer than the nano-silicon samples upon cycling, and also differences in SEI compositions. It is hoped this comprehensive study and understanding should offer critical insights into the exclusive and customized modification strategies to diverse silicon anodes ranging from nano to microscale., (© 2023 Wiley-VCH GmbH.)

Electrocatalytic oxidation of urea (UOR) is a potential energy-saving hydrogen production technology that can replace oxygen evolution reaction (OER). Therefore, CoSeP/CoP interface catalyst is synthesized on nickel foam using hydrothermal, solvothermal, and in situ template methods. The strong interaction of tailored CoSeP/CoP interface promotes the hydrogen production performance of electrolytic urea. During the hydrogen evolution reaction (HER), the overpotential can reach 33.7 mV at 10 mA cm -2 . The cell voltage can reach 1.36 V at 10 mA cm -2 in the overall urea electrolytic process. Notably, the overall urine electrolysis performance of the catalyst in the human urine medium can reach 1.40 V at 10 mA cm -2 and can exhibit durable cycle stability at 100 mA cm -2 . Density functional theory (DFT) proves that the CoSeP/CoP interface catalyst can better adsorb and stabilize reaction intermediates CO* and NH* on its surface through a strong synergistic effect, thus enhancing the catalytic activity., (© 2023 Wiley-VCH GmbH.)

As post-lithium ion batteries, both sodium-ion batteries (SIBs) and potassium ion batteries (PIBs) possess great potential for large scale energy storage. However, the application of both SIBs and PIBs are hindered by the lack of suitable electrode materials. Here, we synthesized the sulfur decorated Ti 3 C 2 T x (S-T 3 C 2 T x ) MXene as electrode material for SIBs and PIBs. Thanks to the sulfur functional group and the formation of Ti-S bond, which facilitates the sodium in-/desertion and strengthens the potassium ion adsorption ability, as well as enhances ion reaction kinetics and improved structure stability, the S-T 3 C 2 T x exhibit excellent sodium/potassium storage performance, high reversible capacities of 151 and 101 mAh g -1 at 0.1 mA g -1 were achieved for SIBs and PIBs, respectively. Moreover, the S-T 3 C 2 T x exhibits remarkable long-term capacity stability at a high density of 500 mA g -1 , providing an impressive storage of 88 mAh g -1 for SIBs and 41 mAh g -1 for PIBs even after 2000 cycles. This work could give a deep comprehension of the heteroatom modification influence on the MXene-based framework and promote the application of MXene electrodes., (© 2023 Wiley-VCH GmbH.)

The ability to extend the polymerizations of thiyl radical propagation to be regulated by existing controlled methods would be highly desirable, yet remained very challenging to achieve because the thiyl radicals still cannot be reversibly controlled by these methods. In this article, we reported a novel strategy that could enable the radical ring-opening polymerization of macrocyclic allylic sulfides, wherein propagating specie is thiyl radical, to be controlled by reversible addition-fragmentation chain transfer (RAFT) agents. The key to the success of this strategy is the propagating thiyl radical can undergo desulfurization with isocyanide and generate a stabilized alkyl radical for reversible control. Systematic optimization of the reaction conditions allowed good control over the polymerization, leading to the formation of polymers with well-defined architectures, exemplified by the radical block copolymerization of macrocyclic allylic sulfides and vinyl monomers and the incorporation of sequence-defined segments into the polymer backbone. This work represents a significant step toward directly enabling the polymerizations of heteroatom-centered radical propagation to be regulated by existing reversible-deactivation radical polymerization techniques., (© 2023 Wiley-VCH GmbH.)

Zn 2+ -induced β-amyloid protein (Aβ) aggregation and microglia activation are the predominant contributors in Alzheimer's disease (AD). Regulating intracephalic excessive Zn 2+ is a promising therapeutic strategy for AD treatment. However, only inhibition of Zn 2+ is hardly to repair continuous damages caused by activated microglia. Herein, an intelligent resveratrol-loaded supramolecular vesicles (RES-loaded vesicles) with zinc ion chelation function and responsive release capability are constructed to alleviate Aβ fibrillation, oxidative stress, and microglial dysfunction. The resveratrol encapsulation efficiency and drug loading efficiency are calculated to be 49.67% and 7.87%, respectively. In vitro studies demonstrate that the RES-loaded vesicles can modulate Zn 2+ -dependent Aβ aggregation. More importantly, the cargoes will be released in zinc environment and further reprograms microglia from proinflammatory M1 phenotype toward anti-inflammatory M2 phenotype, which prevents spontaneous neuroinflammation and alleviates cytotoxicity of cultured cells from 29% to 12%. With the stereotactic or intranasal administration, RES-loaded vesicles can overcome the blood brain barrier, alleviate neuronal apoptosis, neuroinflammation, and ultimately ameliorate cognitive impairment in two AD mouse models. This work provides a new sight for taking advantage of Zn 2+ to treat CNS disorders., (© 2023 Wiley-VCH GmbH.)

Organic polymers have been considered reliable candidates for lithium storage due to their high capacity and lack of volume expansion. Compared with other organic polymers, polyimide has become a very promising electrode material for lithium-ion batteries (LIBs) because of its easy synthesis, customizable structure and structural stability. A large number of studies have confirmed that the benzene ring structure of polyimide has strong lithium storage capacity as an anode material. Hence, we designed and synthesized polyimide organic polymer (PBPAQ) for the first time. The unique spherical flower structure of this material enhances the interaction between the electrode material and the electrolyte by increasing the contact area. The PBPAQ anode has a specific discharge capacity of 738 mAh g -1 after 100 cycles at 0.1 A g -1 . The excellent lithium storage performance of this material laid a foundation for the research of the anode of LIBs in the future., (© 2023 Wiley-VCH Verlag GmbH.)

Fabricating heterogeneous interfaces is an effective approach to improve the intrinsic activity of noble-metal-free catalysts for water splitting. Herein, 3D copper-nickel selenide (CuNi@NiSe) nanodendrites with abundant heterointerfaces are constructed by a precise multi-step wet chemistry method. Notably, CuNi@NiSe only needs 293 and 41 mV at 10 mA cm -2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively. Moreover, the assembled CuNi@NiSe system just requires 2.2 V at 1000 mA cm -2 in anion exchange membrane (AEM) electrolyzer, which is 2.0 times better than Pt/C//IrO 2 . Mechanism studies reveal Cu defects on the Cu 2-x Se surface boost the electron transfer between Cu atoms and Se atoms of Ni 3 Se 4 via Cu 2-x Se/Ni 3 Se 4 interface, largely lowering the reaction barrier of rate-determining step for HER. Besides, the intrinsic activity of Ni atoms for in situ generated NiOOH is largely enhanced during OER because of the electron-modulating effect of Se atoms at Ni 3 Se 4 /NiOOH interface. The unique 3D structure also promotes the mass transfer during catalysis process. This work emphasizes the essential role of interfacial engineering for practical water splitting., (© 2023 Wiley-VCH GmbH.)

Colloidal motors with multimode propulsion have attracted considerable attention because of enhanced transportability. It is a great challenge to fabricate colloidal motors powered by a single engine for multimode synergistic propulsion. Herein, we report on Janus versatile polymer nanoplatforms integrating various functionalities via tetrazole linkages for light-regulated multimode synergistic propulsion in the liquid. The presence of tetrazole linkages in the polymers endows the nanoparticles with various photoresponsive capabilities. A sole energy source (ultraviolet or visible light) simultaneously activates photocatalytic N 2 release and photothermal conversion within the tetrazole-containing polymer phase at one side of asymmetric nanoparticles for converting light energy into photothermal/photocatalytic propulsion independent of the surrounding chemical medium. The photoactivated locomotion using tetrazoles as light-triggered fuels highly corresponds to light wavelengths, light powers and tetrazole contents. The tetrazole linkages capable of incorporating various functionalities to the polymer nanoparticles allow on-demand customizing of the colloidal motors, showing great potential in bio-applications., (© 2023 Wiley-VCH GmbH.)

Phenytoin (PHT) is a first-line antiepileptic drug in clinics, which could decrease neuronal bioelectric activity by blocking the voltage-operated sodium channels. However, the intrinsically low blood-brain-barrier (BBB)-crossing capability of PHT and upregulated expression level of the efflux transporter p-glycoprotein (P-gp) coded by the gene Abcb1 in epileptic neurons limit its efficacy in vivo. Herein, a nanointegrated strategy to overcome PHT resistance mechanisms for enhanced antiepileptic efficacy is reported. Specifically, PHT is first incorporated into calcium phosphate (CaP) nanoparticles through biomineralization, followed by the surface modification of the PEGylated BBB-penetrating TAT peptide. The CaP@PHT-PEG-TAT nanoformulation could effectively cross the BBB to be taken in by epileptic neurons. Afterward, the acidic lysosomal environment would trigger their complete degradation to release Ca 2+ and PHT into the cytosol. Ca 2+ ions would inhibit mitochondrial oxidative phosphorylation to reverse cellular hypoxia to block hypoxia-inducible factor-1α (Hif1α)-Abcb1-axis, as well as disrupt adenosine triphosphate generation, leading to simultaneous suppression of the expression and drug efflux capacity of P-gp to enhance PHT retention. This study offers an approach for effective therapeutic intervention against drug-resistant epilepsy., (© 2023 Wiley-VCH GmbH.)

The importance of catalysts today as workhorses in most modern industrial fields cannot be downplayed. As a result, rational design and engineering of targeted catalysts have emerged as key objectives and are dependent on in-depth understanding of complex catalytic dynamics. Synchrotron radiation (SR) light sources with rich advanced experimental methods are being recognized as a comprehensive characterization platform, which can draw a full picture on such multiparameter-involved catalysis under actual working conditions. Herein, the recent progress of catalytic dynamics process studied by the means of various SR techniques is summarized. In particular, SR-based spectroscopic, scattering, and imaging investigations on true catalysts are first introduced with the potential of in situ and operando characterizations. Apparently, the limitations from single SR technique naturally prompt a simple combination of SR techniques to better understand the whole catalysis process. Moreover, the discrepancies among various online testing facilities and batches of samples, along with random/systematic errors introduced by traditional intermittent/asynchronous measurement make it imperative to develop more prolific systems, complementary of multiple SR techniques for deep probing of dynamic catalytic processes. It is believed that the booming new light sources can further enrich the current multiple SR techniques, and thus may realize the true visualization on future catalytic dynamic processes., (© 2023 Wiley-VCH GmbH.)

To relieve the overwhelming pressure on fossil energy, aqueous magnesium ion batteries attracted tremendous attention owing to their low cost and high safety. However, the cathode materials are apt to occur lattice distortion because of the electrostatic interaction between magnesium ions and crystal. The 2×2 manganese octahedral molecular sieve with potassium ions and water located in the tunnels (K-OMS-2), utilized as a cathode material for chargeable magnesium ions batteries, is exposed to irreversible Mg 2+ intercalation/deintercalation due to lattice distortion, which heavily damages the electrochemical properties and declines the capacity. Herein, we carry out an ion doping strategy to overcome the above issues, leading to an enhanced Mg Mg 2+ storage behavior. The Nb or V cation is successfully doped into K-OMS-2 by a facile reflux method under room temperature. The specific surface area is enlarged by the addition of cations, which promise a large electrode-electrolyte contact area. The Nb and V doped K-OMS-2 present a capacity of 252.6 and 265.9 mAh/g at 20 mA/g, respectively. This work demonstrates an ion doping approach toward exploiting the stable and high-capacity Mg-ion battery cathode and provides potential cathode materials for a large-scale aqueous Mg-ion-based energy storage system., (© 2023 Wiley-VCH GmbH.)

MoS 2 , as a classical 2D material, becomes a capable anode candidate for sodium-ion batteries. However, MoS 2 presents a disparate electrochemical performance in the ether-based and ester-based electrolyte with unclear mechanism. Herein, tiny MoS 2 nanosheets embedded in nitrogen/sulfur-codoped carbon (MoS 2 @NSC) networks are designed and fabricated through an uncomplicated solvothermal method. Thanks to the ether-based electrolyte, the MoS 2 @NSC shows a unique capacity growth in the original stage of cycling. But in the ester-based electrolyte, MoS 2 @NSC shows a usual capacity decay. The increasing capacity puts down to the gradual transformation from MoS 2 to MoS 3 with the structure reconstruction. Based on the above mechanism, MoS 2 @NSC demonstrates an excellent recyclability and the specific capacity keeps around 286 mAh g -1 at 5 A g -1 after 5000 cycles with an ultralow capacity fading rate of only 0.0034% per cycle. In addition, a MoS 2 @NSC‖Na 3 V 2 (PO 4 ) 3 full cell with ether-based electrolyte is assembled and demonstrates a capacity of 71 mAh g -1 , suggesting the potential application of MoS 2 @NSC. Here the electrochemical conversion mechanism of MoS 2 is revealed in the ether-based electrolyte and significance of the electrolyte design on the promoting Na ion storage behavior is highlighted., (© 2023 Wiley-VCH GmbH.)

Highly flexible and robust self-standing covalent organic framework (COF) membranes with rapid preparation are important but technically challenging for achieving precise separation. Herein , a novel imine-based 2D soft covalent organic framework (SCOF) membrane with a large area of 226.9 cm 2 , via ingeniously selecting an aldehyde flexible linker and a trigonal building block, is reported. The soft 2D covalent organic framework membrane is rapidly formed (≈5 min) based on the sodium dodecyl sulfate (SDS) molecular channel constructed at the water/dichloromethane (DCM) interface, which is the record-fast SCOF membrane formation and 72 times faster than that in the reported literature. MD simulation and DFT calculation elucidate that the dynamic, self-assembled SDS molecular channel facilitates faster and more homogeneous transfer of amine monomers in the bulk, thereby forming a soft 2D self-standing COF membrane with more uniform pores. The formed SCOF membrane exhibits superb sieving capability for small molecules, robustness in strong alkaline (5 mol L -1 NaOH), acid (0.1 mol L -1 HCl), and various organic solutions, and sufficient flexibility with a large curvature of 2000 m -1 for membrane-based separation science and technology., (© 2023 Wiley-VCH GmbH.)