Electrochemical nitrate reduction offers a sustainable route to produce ammonia while simultaneously remediating nitrate pollution.Here,we report a series of trimetallic catalysts derived from carbonized zeolitic imid...Electrochemical nitrate reduction offers a sustainable route to produce ammonia while simultaneously remediating nitrate pollution.Here,we report a series of trimetallic catalysts derived from carbonized zeolitic imidazolate frameworks(Czif),incorporating Zn and Cu into a Co-based metal-organic framework(MOF)scaffold.Among them,Czif-Zn_(3)Cu_(1)(zinc and copper precursors at a molar ratio of Zn:Cu=3:1)exhibits the highest Faradaic efficiency(>90%)and NH_(3) yield rate across a broad current density range(100-500 mA/cm^(2)),outperforming both undoped and bimetallic counterparts.Structural characterization reveals the preservation of MOF morphology,with uniformly dispersed Co,Zn,and Cu sites embedded in a porous N-doped carbon matrix.The optimized Zn:Cu ratio enhances intermediate stabilization and suppresses competing hydrogen evolution,supported by a comprehensive set of analyses.Operando flowcell tests confirm the catalyst’s energy efficiency,nitrate tolerance(10-1000 mM),and long-term durability over 100 h.Density functional theory(DFT)calculations confirm that the trimetallic synergy of Czif-Zn_(3)Cu_(1) lowers the overall energy barrier and underpins its enhanced activity.This work highlights the importance of rational trimetallic design and MOFderived architectures in achieving high-performance electrocatalysts for selective and scalable nitrate-to-ammonia conversion.展开更多
In response to growing energy and environmental concerns associated with fossil fuels,renewable energypowered fuel cells have gained significant attention as sustainable alternatives.Especially,ammonia offers high ene...In response to growing energy and environmental concerns associated with fossil fuels,renewable energypowered fuel cells have gained significant attention as sustainable alternatives.Especially,ammonia offers high energy density as well as superior storage and transport properties,thus attracting increasing attention as a promising alternative to hydrogen and rendering direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.While platinum-based catalysts currently dominate the anodic ammonia oxidation reaction(AOR)applications,their scarcity and high cost substantially hinder DAFC commercialization.In this context,developing non-platinumbased electrocatalysts for the AOR represents the efforts towards the more economical use of ammonia energy.This review comprehensively introduces recent progress in non-platinum-based AOR electrocatalysts for low-temperature DAFC applications.Beginning with introductory section highlighting historical context and catalytic breakthroughs,fundamental understanding of DAFC system and the anodic AOR are systematically presented.Subsequently,it outlines the advancements in typical non-platinum-based catalysts,highlighting material innovations and performance enhancements.The analysis concludes by identifying critical research challenges and future directions,offering strategic insights to accelerate the development of high-efficiency DAFC systems.展开更多
Poor tumor penetration is a significant challenge for using nanoliposomebased chemotherapy for triple-negative breast cancer(TNBC).Recently,a milieu of biological cues downregulating tumor stroma has been associated w...Poor tumor penetration is a significant challenge for using nanoliposomebased chemotherapy for triple-negative breast cancer(TNBC).Recently,a milieu of biological cues downregulating tumor stroma has been associated with biological metal ions,primarily such as Mn2+.Inspired by this,we hypothesized that Mn2+could serve as a functional component in designing an alternative modulator for the tumor stroma microenvironment by reducing its extracellular matrix,further decreasing its stromal density.Herein,we presented a novel extracellular matrix(ECM)depleter within a tumor involving manganese-based mineralization materials that primed inhibition of the extracellular matrix of cancer cells,demonstrating a facile strategy for improving drug penetration,delivery and therapy efficiency of the doxorubicin-loaded liposome nanoparticles(Dox-LNP).As a result,the manganese mimetic mineralization material,manganese phosphate(MnP),demonstrated controlled biodegradation and biocompatibility within tumor microenvironments.The release of Mn^(2+)from MnP within the cell lysosome or tumor microenvironment inhibited TGF-β expression and its downstream profibrotic signaling pathways,thereby reducing the tumor stroma density by suppressing the expression of α-smooth actin(α-SMA)and collagen I(COL-I),and inducing tumor stromal disruption both in vitro and in vivo.The typical nanomedicines,Dox-LNP,were subsequently used to check their penetration.The MnP pretreated tumor could significantly improve tumor penetration and accumulation of Dox-LNP,which demonstrated a significant improvement in the treatment of TNBC.These achievements proposed a successful tumor stromal regulation material involving manganese mineralization for priming tumor stromal depletion in situ by inhibiting the TGF-β and associated proteins,representing an alternative materials strategy to substitute biotechnology for stromal reduction,which may further represent a great potential of nanomedicine-based cancer therapy.展开更多
Transition metal phosphides(TMPs)hold promise as effective bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries(RZABs),yet their practical application is hindered by inadequate durability and sluggis...Transition metal phosphides(TMPs)hold promise as effective bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries(RZABs),yet their practical application is hindered by inadequate durability and sluggish kinetics.Herein,we design a heterophosphate composite comprising Fe_(2)P-FeCoP heterojunctions anchored on onedimensional(1D)hollow N,P-doped carbon nanotubes(Fe_(2)PFeCoP@HNPC)through controlled metal modulation of anilinephytate nanorods.Critically,the interfacial electronic coupling between Fe_(2)P and FeCoP induces a cross-interfacial electronbridge network,which drives charge redistribution to accelerate interfacial electron transfer and refines the d band adsorption energetics for optimized oxygen intermediate binding.Coupled with its hollow architecture,Fe_(2)P-FeCoP@HNPC enables synergistic mass/charge transfer enhancement.The synergistic electronic-structural effects endow Fe_(2)P-FeCoP@HNPC with exceptional bifunctional activity,achieving a high oxygen reduction reaction(ORR)half-wave potential(0.83 V vs.reversible hydrogen electrode(RHE))and low oxygen evolution reaction(OER)overpotential(1.53 V@10 mA·cm^(-2)),attributed to the stabilized electron-bridge effect and hierarchical mass/charge transfer dynamics.Fe_(2)P-FeCoP@HNPC assembled RZAB achieves a peak power density of 145 mW·cm^(-2) and ultralong cycling stability(>1240 h)with negligible decay.This work demonstrates a universal strategy to harmonize electronic and structural engineering in TMPs for high-performance electrochemical energy systems.展开更多
Liquid-phase adsorption is a critical technology for environmental sustainability,resource management,and the advancement of biotechnology and materials science.The development of materials capable of efficient and hi...Liquid-phase adsorption is a critical technology for environmental sustainability,resource management,and the advancement of biotechnology and materials science.The development of materials capable of efficient and highly selective adsorption from aqueous media is essential.In this study,we investigate the adsorption of phenolic compounds(guaiacol,creosol,and homocresol)from aqueous solutions using a stable hydrophobic metal-organic framework(MOF),namely MIL-140C.Synthesized via fast microwave-assisted hydrothermal conditions within 40 min,MIL-140C exhibits high efficiency in liquid-phase separations,achieving full recovery of these compounds upon complete pore occupancy.Our results highlight that the adsorbent with one-dimensional(1D)channels featuring parallel benzene rings is superior;the micropore filling degree of the adsorbent directly affects the recovery efficiency of the adsorbate.Theoretical calculations and Fourier transform infrared spectroscopy(FTIR)analysis further confirm the adsorption with minimal chemical bonding.This study underscores the potential of MOFs of benzene rings parallel to the 1D channel for sustainable phenolic recovery and efficient separations of aromatic containing molecules,reflecting the decisive importance of micropore occupancy in determining recovery efficiency.展开更多
The dynamic evolution of surface electrochemical potential of the electrolyte plays a key role in the performance of solid-state electrochemical devices,while its real-time characterization remains challenging.Here,we...The dynamic evolution of surface electrochemical potential of the electrolyte plays a key role in the performance of solid-state electrochemical devices,while its real-time characterization remains challenging.Here,we visualize the dynamic evolution of the surface electrochemical potential on yttria-stabilized zirconia(YSZ)in a planar Au|YSZ|Au model cell,using spatially resolved photoelectron-based techniques including photoemission electron microscopy(PEEM)and micro-region X-ray photoelectron spectroscopy(μ-XPS).PEEM reveals two sequential reaction fronts in YSZ under cathodic polarization,corresponding to the evolution of the chemical potential of oxygen ions,with a faster propagation speed on the top surface and a slower one in the near-surface region.XPS measurements quantitatively reveal the time-dependent electric potential distribution across YSZ surface.COMSOL simulations confirm the presence of a stronger electric field at the top surface,particularly at the advancing reaction fronts,compared to the near-surface region.The critical role of the electric field in driving surface reactions is further supported by the enhanced reactions observed at the tips of the zigzag-shaped electrode edges.This work offers mechanistic insights into the coupling between electrochemical potential dynamics and electrolyte reactions.展开更多
Vanadium-ceria catalysts have become promising bifunctional catalysts for simultaneously removing nitrogen oxides(NO_(x))and chlorobenzene(CB).However,limited selectivity toward inorganic chlorine species and the accu...Vanadium-ceria catalysts have become promising bifunctional catalysts for simultaneously removing nitrogen oxides(NO_(x))and chlorobenzene(CB).However,limited selectivity toward inorganic chlorine species and the accumulation of chlorine species remain critical challenges.In this study,a Ru-modified(VO_(x))_(n)/CeO_(2) catalyst was synthesized via a pre-loading strategy.The pre-loaded Ru species not only created highly active redox sites favorable for deep CB oxidation through strong interactions with the CeO_(2) support but also enhanced the polymerization of V species and modulated the electronic environment of V=O species,enhancing the selective catalytic reduction(SCR)activity and the ability to cleave C-Cl bonds.Importantly,the Ru pre-loading preserved Brønsted acid site concentrations while decreasing Lewis acid site density,thereby reducing Cl deposition and improving catalyst stability.As a result,the optimized catalyst demonstrated superior performance,achieving over 90%NO_(x) and CB conversion in the 330-400℃ temperature range.The selectivities towards inorganic chlorine species(IC)and CO_(x) are both maintained above 90%.展开更多
Two-dimensional(2D)Bi_(2)O_(2)Se nanosheets,as an emerging ternary layered semiconductor,exhibit promising potential for photodetection owing to their moderate bandgap,high carrier mobility,and excellent environmental...Two-dimensional(2D)Bi_(2)O_(2)Se nanosheets,as an emerging ternary layered semiconductor,exhibit promising potential for photodetection owing to their moderate bandgap,high carrier mobility,and excellent environmental stability.However,their intrinsically high carrier concentration typically results in elevated dark currents and sluggish response speeds,thereby limiting further performance enhancement.To synergistically optimize both the response speed and sensitivity,we fabricated n-type Bi_(2)O_(2)Se nanosheets via chemical vapor deposition(CVD)and integrated them into a Bi_(2)O_(2)Se/InSe semivertical heterojunction photodetector featuring a single-sided depletion region.Benefitting from the type-II band alignment and the graphene bottom electrode,photogenerated carriers are efficiently separated and rapidly extracted.This design simultaneously shortens the carrier transit time and suppresses recombination,enabling the device to achieve high sensitivity(responsivity R of 0.47 A/W,detectivity D^(*) f 3.21×10^(12) Jones,external quantum efficiency(EQE)of 166.09%)while maintaining ultrafast response characteristics(rise/fall times of 48.5/41.7μs).The photodetector exhibits broadband selfpowered operation across ultraviolet(UV)to near-infrared wavelengths(300-1050 nm).These results highlight the significant potential of Bi_(2)O_(2)Se/InSe semi-vertical heterojunctions for high-performance,low-power,self-powered broadband photodetectors spanning the UV-visible-near infrared ray(UV-Vis-NIR)spectrum.展开更多
Twisted multilayers of two-dimensional materials attract widespread research interest due to their intriguing electronic and optical properties related to their chiral symmetry breaking and moiréeffects.The two-d...Twisted multilayers of two-dimensional materials attract widespread research interest due to their intriguing electronic and optical properties related to their chiral symmetry breaking and moiréeffects.The two-dimensional transition metal dichalcogenide MoSe_(2) is a particularly promising material for twisted multilayers,capable of sustaining moiréexcitons.Here,we report on a rational bottomup synthesis approach for twisted MoSe_(2) flakes by chemical vapor transport(CVT).Screw dislocation-driven growth was forced by surface-fused SiO_(2)nanoparticles on the substrates that serve as potential nucleation points in low supersaturation condition.Thus,crystal growth by in-situ CVT under addition of MoCl_(5) leads to bulk 2H-MoSe_(2) in a temperature gradient from 900 to 820℃ with a dwell time of 96 h.Hexagonally shaped 2H-MoSe_(2) flakes were grown from 710 to 685℃ with a dwell time of 30 min on SiO_(2)@Al_(2)O_(3)(0001)substrates.Electron backscatter diffraction as well as electron microscopy reveals the screw dislocation-driven growth of triangular 3R-MoSe_(2) with individual step heights between 0.9 and 2.9 nm on SiO_(2)@Si(100)under the same conditions.Finally,twisted MoSe_(2) flakes exhibiting a twist angle of 19°with respect to the[010]zone axis could be synthesized.展开更多
Multisensory integration allows biological organisms to merge information from various sensory modalities,enhancing perception,decision-making,and adaptability in complex environments.This process,involving specialize...Multisensory integration allows biological organisms to merge information from various sensory modalities,enhancing perception,decision-making,and adaptability in complex environments.This process,involving specialized cortical and subcortical areas,reduces uncertainty,speeds up responses,enriches perception,and supports adaptive behaviors.Recent findings reveal that even primary sensory cortices contribute to multisensory processing,further boosting adaptability and decisionmaking.Inspired by these natural capabilities,researchers aim to develop artificial systems replicating biological sensory integration to address challenges in robotics,artificial intelligence,and big data.Current artificial systems,often reliant on single-modal perception,struggle in dynamic environments due to their limited adaptability.Advances in materials,device architectures,and neuromorphic technologies,such as memristor-and transistor-based neurons,are enabling the development of multimodal systems with enhanced efficiency,flexibility,and functionality.This review explores strategies to overcome single-modal limitations,focusing on synchronization,fusion,and deep interpretation of sensory data.Future directions emphasize improving integration density,novel device designs,and adaptable mechanisms.Multimodal systems hold promise to revolutionize artificial perception,narrowing the gap between biological systems and intelligent technologies.展开更多
Epilepsy is a complex neurological disorder aggravated by chronic neuroinflammation largely driven by reactive astrocytes.These cells promote epileptogenesis through persistent cytokine secretion and glial scar format...Epilepsy is a complex neurological disorder aggravated by chronic neuroinflammation largely driven by reactive astrocytes.These cells promote epileptogenesis through persistent cytokine secretion and glial scar formation.Current antiepileptic drugs remain ineffective in targeting these mechanisms due to limited blood-brain barrier(BBB)permeability and poor astrocytic specificity.A transferrin-functionalized biomimetic nanotherapeutic loaded with resveratrol(RN@RTA)was developed to regulate astrocyte-mediated inflammation by activating sirtuin 1(SIRT1)and suppressing the mitogen-activated protein kinase/nuclear factor Kappalight-chain-enhancer of activated B cells(MAPK/NF-κB)axis.Using in vitro BBB models,primary astrocytes,and a pilocarpine-induced chronic epilepsy mouse model,we evaluated the capacity of RN@RTA to cross the BBB,inhibit inflammatory signaling,and reduce seizure activity.Mechanistic assays included immunoprecipitation of NF-κB complexes,cytokine quantification,RNA sequencing,and histopathological assessments of glial and synaptic markers.RN@RTA achieved 82%uptake by hippocampal astrocytes and significantly reduced Il6,Tnf-α,and Nlrp3 expression.SIRT1 activation disrupted the NF-κB p65/p300 complex,leading to transcriptional repression of inflammatory genes and enhancement of autophagy.In vivo,seizure frequency decreased by 67%,synaptic structure was preserved,and astrogliosis was markedly alleviated.The findings demonstrate a dual regulatory mechanism in which RN@RTA suppresses neuroinflammatory signaling and restores neural homeostasis,offering a promising molecularly targeted approach for refractory epilepsy.展开更多
Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy a...Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy and renewable electricity.As a key component,efficient oxygen electrocatalyst for promoting sluggish reaction kinetics of oxygen reduction and evolution reaction(ORR and OER)under harsh operation conditions severely limited progress of these devices.Among various candidates,Ptgroup(Pt,Ir,and Ru)-based electrocatalysts are still the most active ORR/OER catalysts.However,the scarcity,high cost,and questionable stability restrict the widespread applications and the commercialization of PEMWE/PEMFC.Progresses in synthesizing atomically dispersed single/multiple-atom catalysts(SACs/MACs)offer new opportunities to Pt-group ORR/OER catalysts owing to nearly 100% metal utilization and high catalytic activities.Extensive efforts have been continuously devoted to optimizing the local structure of Pt-group OER/ORR catalysts at atom-level for further enhancing stability and activity.In this review,universal synthesis methods to prepare Ptgroup SACs are discussed first,highlighting crucial factors which affect the structure and catalytic performance.Afterward,advanced characterization techniques for directly confirming atomic dispersed metal atoms were introduced,including aberration-corrected high-angle-annular-dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy.Importantly,considerations for rational catalyst design and typical Pt-group SACs/MACs are summarized regarding the regulation strategy of atomically dispersed metal sites and various supports,and effects of metal-support interaction on the catalytic performance.Finally,key challenges and proposed perspectives for future development of atomically dispersed Pt-group oxygen electrocatalysts for fuel cell and electrolyzer are briefly discussed.展开更多
Fe-N-C catalysts,as promising non-precious metal alternatives for the oxygen reduction reaction(ORR),still suffer from severe mass transport limitations in proton exchange membrane fuel cells(PEMFCs)due to water flood...Fe-N-C catalysts,as promising non-precious metal alternatives for the oxygen reduction reaction(ORR),still suffer from severe mass transport limitations in proton exchange membrane fuel cells(PEMFCs)due to water flooding of active sites embedded in micropores.Although pore engineering through a selected template is a general strategy,the structural features of an ideal template,particularly those governing the exposure of active sites and thus affecting mass transport,remain elusive.Here,we demonstrate that low-porosity carbon templates maximize the ratio of active sites distributed at or near the surface,thereby enhancing their exposure and accessibility while reducing mass transport resistance during the ORR process.The C_(lp-1)@PPy and C_(lp-2)@PPy(PPy=polypyrrole)catalysts,derived from low-porosity carbon templates,achieve peak power densities of 0.96 and 1.03 W·cm^(-2) under H_(2)/O_(2)and 0.50 and 0.52 W·cm^(-2) under H_(2)/air,demonstrating excellent performance in PEMFC tests.Structural and electrochemical characterizations reveal that the enhanced surface exposure of active sites effectively mitigates mass transport resistance during the ORR,thereby offering a general design principle for overcoming mass transport limitations in Fe-N-C catalysts for PEMFC applications.展开更多
Electromagnetic interference(EMI)shielding materials principally attain shielding by reflecting electromagnetic waves through impedance mismatch caused by high conductivity,which inevitably leads to secondary electrom...Electromagnetic interference(EMI)shielding materials principally attain shielding by reflecting electromagnetic waves through impedance mismatch caused by high conductivity,which inevitably leads to secondary electromagnetic wave pollution.Consequently,the development of multifunctional,low-reflection electromagnetic shielding materials remains a significant challenge.Materials that are lightweight,possess high mechanical strength,exhibit excellent electromagnetic shielding absorption,and demonstrate low reflectivity have historically been the focus of significant interest.Natural silk,lightweight and strong,is an ideal composite matrix.Regenerated silk fibroin(RSF)synthesized via a bottom-up approach and cross-linked with polyvinyl alcohol(PVA)forms an aerogel matrix with remarkable compressive strength.In accordance with the principle of integrating functional design with structural design,spherical NiFe_(2)O_(4)particles were grown on the MXene surface via electrostatic self-assembly and combined with RSF/PVA as the aerogel absorptive layer,while RSF/PVA/MXene served as the reflective layer.A vertically oriented structure of Janus aerogel was prepared through sequential directed freezing.The resulting aerogel with 0.058 g/cm^(3) reveals the high compression strength(3.52 MPa).Reasonable functional and structural design enables aerogel to effectively dissipate incident electromagnetic waves through absorption,reflection,and reabsorption processes,achieving an average SET value of 48.05±1.75 dB and reaching a minimum reflection coefficient of 0.19.Furthermore,the aerogel displays remarkable infrared stealth capabilities.This lightweight,rigid,multifunctional aerogel is poised to play a significant role in the field of next-generation electronic devices.展开更多
Oxygen reduction reaction(ORR)is crucial for Znair batteries,while also serves as a core electrochemical process in oxygen depolarized cathodes(ODCs)for chlor-alkali electrolysis.The lack of cost-effective,highly acti...Oxygen reduction reaction(ORR)is crucial for Znair batteries,while also serves as a core electrochemical process in oxygen depolarized cathodes(ODCs)for chlor-alkali electrolysis.The lack of cost-effective,highly active ORR electrocatalysts with superior kinetics hinders progress in this field.Herein,we report the Fe/Ni dual single-atomic sites anchored by commercial carbon black(Fe/Ni-N/CB)using rigid ligand confined and high-temperature shock(HTS)strategy in less than 0.5 s.Theoretical calculation reveals that singleatomic Fe is the real active site.Single-atomic Fe and Ni species in Fe/Ni-N/CB synergistically accelerate the kinetics of ORR by reducing the energy barrier of the rate-determining step.A large half-wave potential(E_(1/2))of 0.907 V is achieved in 0.1 M KOH aqueous solution.The assembled aqueous Zn-air battery(A-ZAB)with Fe/Ni-N/CB cathode presents remarkable charge-discharge cycling stability for over 650 h without voltage gap degradation.The quasi-solid-state Zn-air battery(QSS-ZAB)exhibits excellent reversibility over a 150-h operation at 0.5 mA·cm^(-2) with negligible energy conversion efficiency recession.Impressively,Fe/Ni-N/CB||RuO_(2)chloralkali flow cell exhibits a low cell voltage of 1.60 V at a large current density of 300 mA·cm^(-2) at 80℃,and demonstrates exceptional durability with 7% current density decay over 150 h of continuous operation at 100 mA·cm^(-2).Fe/Ni-N/CB||RuO_(2)achieves near-ideal caustic current efficiency(~97.2%)at the current density of 300 mA·cm^(-2).This work provides a rapid and economical synthesis technique for the synthesis of catalysts at the atomic scale while demonstrating significant potential for application in energy-saving chlor-alkali electrolyzer.展开更多
The magnetic proximity effect enables interfacial modulation of excitonic and spin-valley properties in transition metal dichalcogenides(TMDs),offering a versatile route toward next-generation spintronic and valleytro...The magnetic proximity effect enables interfacial modulation of excitonic and spin-valley properties in transition metal dichalcogenides(TMDs),offering a versatile route toward next-generation spintronic and valleytronic devices.However,the inherently weak photoluminescence(PL)of bright excitons—suppressed by proximity-induced darkening mechanisms—hinders the optical detection of magnetic interactions.Here,we demonstrate substantial exciton emission enhancement in CrOCl/WSe_(2)(HS)and twisted 90°-CrOCl/CrOCl/WSe_(2)(THS)heterostructures by employing plasmonic Au nanopillar arrays to activate surface plasmon polariton(SPP)coupling.The neutral exciton emission intensity is enhanced by factors of 5 and 18 for HS/Au and THS/Au,respectively,with enhancements persisting under high magnetic fields and elevated temperatures(~10-fold in THS/Au).Enabled by this amplification,we observe pronounced Zeeman splitting and modified intervalley relaxation pathways,indicating significant magnetic proximity interactions.Finite-element simulations and first-principles calculations reveal that the enhancement arises from local electromagnetic field concentration and layer-dependent interfacial coupling.Our results establish SPP-assisted PL enhancement as an effective strategy for probing weak magneto-optical signatures,paving the way for detailed exploration of exciton-magnon coupling and interface-driven quantum phenomena in twodimensional(2D)magnetic heterostructures.展开更多
Myelosuppression is a common and severe side effect of cancer chemotherapy,with current treatments hindered by limitations such as depletion of hematopoietic reserves,poor patient compliance,delayed therapeutic onset,...Myelosuppression is a common and severe side effect of cancer chemotherapy,with current treatments hindered by limitations such as depletion of hematopoietic reserves,poor patient compliance,delayed therapeutic onset,and high cost.To overcome these challenges,we developed Epimedium-derived nanovesicles(ENVs)from the traditional Chinese medicinal herb Epimedium,addressing the solubility and bioavailability issues associated with conventional extracts.ENVs encapsulate bioactive constituents,including icariin and hematopoiesis-promoting ceramides.In a cyclophosphamide(CTX)-induced myelosuppression mouse model,prophylactic and therapeutic oral administration of ENVs effectively alleviated hematopoietic suppression,significantly outperforming the Epimedium-based herbal extract“Joungal”(Shengbai Formula)despite equivalent icariin content.Notably,ENVs promoted hematopoietic stem cell(HSC)proliferation—an outcome rarely achieved with existing therapies.Mechanistically,ENVs modulated the gut microbiota,enriching lactobacillus species and enhancing lactate production.This microbiota-driven lactate signaling stimulated LepR+mesenchymal stem cells(MSCs)in the bone marrow niche to secrete stromal cellderived factor-1(SDF-1)and stem cell factor(SCF),thereby supporting HSC expansion and restoring hematopoietic function.In vivo safety evaluations confirmed the excellent biocompatibility of ENVs.Our findings uncover a gut-lactate-bone marrow axis through which ENVs enhance hematopoiesis and promote HSC regeneration.This work introduces a cost-effective,scalable,and orally administrable biomaterial platform with strong translational potential for the prevention and treatment of chemotherapy-induced myelosuppression.展开更多
Water,salt solution,and many conventional organic solvents exhibit melting temperatures nearly or well below zero degree,and functional phase change composites based on these components will be useful in energy and en...Water,salt solution,and many conventional organic solvents exhibit melting temperatures nearly or well below zero degree,and functional phase change composites based on these components will be useful in energy and environmental areas.Here,we report the design and fabrication of a series of composite hydrogels and organogels consisting of water,NaCl/water eutectic solution,n-undecane,and n-heptanol held by a built-in carbon nanotube(CNT)-polymer skeleton,respectively.We adopt an initially uniform yet transformable CNT network to mix with gel precursors and obtain densified CNT-reinforced pore walls by in situgelation.These composite gels realized solid-liquid phase transition in temperatures ranging from−10 to−36℃,with reduced supercooling,large enthalpy(120 to 200 J/g),enhanced structural stability and anti-leakage property,and the effects of CNTs on thermal and mechanical properties are investigated systematically.We demonstrate that by wrapping the composite gels around pipe models with cold liquid flow,the temperature increase process could be substantially prolonged,owing to efficient latent heat release during phase change.Our CNT-reinforced hydrogels and organogels,made by a general,facile approach,have many potential applications as cold energy storage and transformation media in liquefied natural gas industry,food,and biomedical fields.展开更多
Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying ther...Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying therapies.Inspired by natural enzymatic cascades,we developed a bioinspired nanocomposite hydrogel,N,S-doped Mn-Nb(C-CeO),that mimics endogenous antioxidant pathways to reprogram the OA microenvironment.This system combines N,Sdoped Mn-Nb_(2)C MXene nanosheets with CeO_(2)nanozymes within a boronate ester-crosslinked hydrogel,forming an“immuno-redox circuitry”with four synergistic functions:(1)cascade reactive oxygen species(ROS)scavenging via superoxide dismutase-like Mn-Nb_(2)C and catalase-like CeO_(2),amplified by photothermal enhancement under near-infrared irradiation;(2)broad reactive nitrogen species clearance,removing peroxynitrite(ONOO^(-)),nitric oxide(NO),and nitroxyl(NO^(-))to mitigate inflammation;(3)immunomodulation through Mn^(2+)-activated cGAS-STING signaling,which promoted macrophage polarization toward the M2 phenotype,concomitantly reducing the levels of pro-inflammatory cytokines such as interleukin-1 beta(IL-1β)and tumor necrosis factor-alpha(TNF-α);(4)cartilage regeneration via pH/ROS-responsive simvastatin(SIM)release and nanocatalysis,upregulating SRY-box transcription factor 9(SOX9)and Col2a1 while inhibiting matrix metalloproteinase-13(MMP-13)and a disintegrin and metalloproteinase with thrombospondin motifs 5(ADAMTS5).In a murine OA model,the system reduced synovitis by 60%,restored 80% of cartilage thickness,and suppressed osteophyte formation,outperforming singlecomponent treatments.This strategy pioneers a“self-healing cartilage”approach by integrating nanocatalysis with immunoengineering for transformative OA therapy.展开更多
Metal-semiconductor plasmonic metasurfaces enable precise optical field manipulation at the subwavelength scale;however,most existing designs rely on external fields and exhibit only binary responses,thereby restricti...Metal-semiconductor plasmonic metasurfaces enable precise optical field manipulation at the subwavelength scale;however,most existing designs rely on external fields and exhibit only binary responses,thereby restricting the realization of multistate logic operations.Here,we present an in-situ polarization-controlled approach based on an Au-indium tin oxide(ITO)bilayer nanocrescent with a Schottky heterojunction for achieving polarization-dependent tristate optical modulation.Polarization-selective excitation of distinct localized plasmon modes facilitates directional hot-electron injection across the Au-ITO interface,thereby producing three distinct programmable states—positive,zero,and negative—at a single detection wavelength.This symmetric bilayer design is applicable to other metal-semiconductor composites and offers generalizable design principles for ternary logic,multistate optical encoding,and ultrafast photonic information processing.The proposed concept is validated through both experimental measurements and numerical simulations.展开更多
基金supported by the National Natural Science Foundation of China(No.22406049)China Postdoctoral Science Foundation(No.GZC20240432).
文摘Electrochemical nitrate reduction offers a sustainable route to produce ammonia while simultaneously remediating nitrate pollution.Here,we report a series of trimetallic catalysts derived from carbonized zeolitic imidazolate frameworks(Czif),incorporating Zn and Cu into a Co-based metal-organic framework(MOF)scaffold.Among them,Czif-Zn_(3)Cu_(1)(zinc and copper precursors at a molar ratio of Zn:Cu=3:1)exhibits the highest Faradaic efficiency(>90%)and NH_(3) yield rate across a broad current density range(100-500 mA/cm^(2)),outperforming both undoped and bimetallic counterparts.Structural characterization reveals the preservation of MOF morphology,with uniformly dispersed Co,Zn,and Cu sites embedded in a porous N-doped carbon matrix.The optimized Zn:Cu ratio enhances intermediate stabilization and suppresses competing hydrogen evolution,supported by a comprehensive set of analyses.Operando flowcell tests confirm the catalyst’s energy efficiency,nitrate tolerance(10-1000 mM),and long-term durability over 100 h.Density functional theory(DFT)calculations confirm that the trimetallic synergy of Czif-Zn_(3)Cu_(1) lowers the overall energy barrier and underpins its enhanced activity.This work highlights the importance of rational trimetallic design and MOFderived architectures in achieving high-performance electrocatalysts for selective and scalable nitrate-to-ammonia conversion.
基金supported by the National Natural Science Foundation of China(No.52401284)the Natural Science Foundation of Jiangsu Province(No.BK20240957).
文摘In response to growing energy and environmental concerns associated with fossil fuels,renewable energypowered fuel cells have gained significant attention as sustainable alternatives.Especially,ammonia offers high energy density as well as superior storage and transport properties,thus attracting increasing attention as a promising alternative to hydrogen and rendering direct ammonia fuel cells(DAFCs)distinct safety advantages over hydrogen-based systems.While platinum-based catalysts currently dominate the anodic ammonia oxidation reaction(AOR)applications,their scarcity and high cost substantially hinder DAFC commercialization.In this context,developing non-platinumbased electrocatalysts for the AOR represents the efforts towards the more economical use of ammonia energy.This review comprehensively introduces recent progress in non-platinum-based AOR electrocatalysts for low-temperature DAFC applications.Beginning with introductory section highlighting historical context and catalytic breakthroughs,fundamental understanding of DAFC system and the anodic AOR are systematically presented.Subsequently,it outlines the advancements in typical non-platinum-based catalysts,highlighting material innovations and performance enhancements.The analysis concludes by identifying critical research challenges and future directions,offering strategic insights to accelerate the development of high-efficiency DAFC systems.
基金financially supported by the National Natural Science Foundation of China(Nos.32471400 and 51902289)the key project of the Natural Science Foundation of Zhejiang Province(No.LZ24E020002)+1 种基金the Key Research&Development Program of Zhejiang Province(No.2024C03019,2024C03075,2021C01180,and 2019C04020)the Interdisciplinary Construction Funding of Biomedical Materials in ZSTU.
文摘Poor tumor penetration is a significant challenge for using nanoliposomebased chemotherapy for triple-negative breast cancer(TNBC).Recently,a milieu of biological cues downregulating tumor stroma has been associated with biological metal ions,primarily such as Mn2+.Inspired by this,we hypothesized that Mn2+could serve as a functional component in designing an alternative modulator for the tumor stroma microenvironment by reducing its extracellular matrix,further decreasing its stromal density.Herein,we presented a novel extracellular matrix(ECM)depleter within a tumor involving manganese-based mineralization materials that primed inhibition of the extracellular matrix of cancer cells,demonstrating a facile strategy for improving drug penetration,delivery and therapy efficiency of the doxorubicin-loaded liposome nanoparticles(Dox-LNP).As a result,the manganese mimetic mineralization material,manganese phosphate(MnP),demonstrated controlled biodegradation and biocompatibility within tumor microenvironments.The release of Mn^(2+)from MnP within the cell lysosome or tumor microenvironment inhibited TGF-β expression and its downstream profibrotic signaling pathways,thereby reducing the tumor stroma density by suppressing the expression of α-smooth actin(α-SMA)and collagen I(COL-I),and inducing tumor stromal disruption both in vitro and in vivo.The typical nanomedicines,Dox-LNP,were subsequently used to check their penetration.The MnP pretreated tumor could significantly improve tumor penetration and accumulation of Dox-LNP,which demonstrated a significant improvement in the treatment of TNBC.These achievements proposed a successful tumor stromal regulation material involving manganese mineralization for priming tumor stromal depletion in situ by inhibiting the TGF-β and associated proteins,representing an alternative materials strategy to substitute biotechnology for stromal reduction,which may further represent a great potential of nanomedicine-based cancer therapy.
基金supported by the National Natural Science Foundation of China(Nos.22075072 and 52301272)the Research Project of Hubei Provincial Department of Education(No.D20242502)+1 种基金the Natural Science Foundation of Hubei Province(No.2023AFB1010)Undergraduate Innovation and Entrepreneurship Training Program Project(Nos.202510513014 and S202510513078).
文摘Transition metal phosphides(TMPs)hold promise as effective bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries(RZABs),yet their practical application is hindered by inadequate durability and sluggish kinetics.Herein,we design a heterophosphate composite comprising Fe_(2)P-FeCoP heterojunctions anchored on onedimensional(1D)hollow N,P-doped carbon nanotubes(Fe_(2)PFeCoP@HNPC)through controlled metal modulation of anilinephytate nanorods.Critically,the interfacial electronic coupling between Fe_(2)P and FeCoP induces a cross-interfacial electronbridge network,which drives charge redistribution to accelerate interfacial electron transfer and refines the d band adsorption energetics for optimized oxygen intermediate binding.Coupled with its hollow architecture,Fe_(2)P-FeCoP@HNPC enables synergistic mass/charge transfer enhancement.The synergistic electronic-structural effects endow Fe_(2)P-FeCoP@HNPC with exceptional bifunctional activity,achieving a high oxygen reduction reaction(ORR)half-wave potential(0.83 V vs.reversible hydrogen electrode(RHE))and low oxygen evolution reaction(OER)overpotential(1.53 V@10 mA·cm^(-2)),attributed to the stabilized electron-bridge effect and hierarchical mass/charge transfer dynamics.Fe_(2)P-FeCoP@HNPC assembled RZAB achieves a peak power density of 145 mW·cm^(-2) and ultralong cycling stability(>1240 h)with negligible decay.This work demonstrates a universal strategy to harmonize electronic and structural engineering in TMPs for high-performance electrochemical energy systems.
基金supported by the National Natural Science Foundation of China(Nos.22471027,22101039,22311530679,and 22171035)the State Key Laboratory of Catalysis(2024SKL-A-006,N-23-01)+3 种基金the Foundation of State Key Laboratory of Coal Conversion(No.J24-25-611)the Fundamental Research Funds for the Central Universities(Nos.DUT24LK004 and DUT25Z2501)Liaoning Provincial Science and Technology Programme Joint Programme(Nos.2025JH2/101900044 and 2024-MSLH-068)the Open Research Fund of Guangdong Advanced Carbon Materials Co.,Ltd(No.Kargen-2024A0102).
文摘Liquid-phase adsorption is a critical technology for environmental sustainability,resource management,and the advancement of biotechnology and materials science.The development of materials capable of efficient and highly selective adsorption from aqueous media is essential.In this study,we investigate the adsorption of phenolic compounds(guaiacol,creosol,and homocresol)from aqueous solutions using a stable hydrophobic metal-organic framework(MOF),namely MIL-140C.Synthesized via fast microwave-assisted hydrothermal conditions within 40 min,MIL-140C exhibits high efficiency in liquid-phase separations,achieving full recovery of these compounds upon complete pore occupancy.Our results highlight that the adsorbent with one-dimensional(1D)channels featuring parallel benzene rings is superior;the micropore filling degree of the adsorbent directly affects the recovery efficiency of the adsorbate.Theoretical calculations and Fourier transform infrared spectroscopy(FTIR)analysis further confirm the adsorption with minimal chemical bonding.This study underscores the potential of MOFs of benzene rings parallel to the 1D channel for sustainable phenolic recovery and efficient separations of aromatic containing molecules,reflecting the decisive importance of micropore occupancy in determining recovery efficiency.
基金financially supported by the National Key R&D Program of China(Nos.2022YFA1504500 and 2021YFA1502800)the National Natural Science Foundation of China(Nos.22372158,22332006,and 22288201)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0600300)iChEM and Photon Science Center for Carbon Neutrality.
文摘The dynamic evolution of surface electrochemical potential of the electrolyte plays a key role in the performance of solid-state electrochemical devices,while its real-time characterization remains challenging.Here,we visualize the dynamic evolution of the surface electrochemical potential on yttria-stabilized zirconia(YSZ)in a planar Au|YSZ|Au model cell,using spatially resolved photoelectron-based techniques including photoemission electron microscopy(PEEM)and micro-region X-ray photoelectron spectroscopy(μ-XPS).PEEM reveals two sequential reaction fronts in YSZ under cathodic polarization,corresponding to the evolution of the chemical potential of oxygen ions,with a faster propagation speed on the top surface and a slower one in the near-surface region.XPS measurements quantitatively reveal the time-dependent electric potential distribution across YSZ surface.COMSOL simulations confirm the presence of a stronger electric field at the top surface,particularly at the advancing reaction fronts,compared to the near-surface region.The critical role of the electric field in driving surface reactions is further supported by the enhanced reactions observed at the tips of the zigzag-shaped electrode edges.This work offers mechanistic insights into the coupling between electrochemical potential dynamics and electrolyte reactions.
基金support provided by the National Natural Science Foundation of China(Nos.22376178,22322606,and 22276105)Beijing Natural Science Foundation(No.8222054).
文摘Vanadium-ceria catalysts have become promising bifunctional catalysts for simultaneously removing nitrogen oxides(NO_(x))and chlorobenzene(CB).However,limited selectivity toward inorganic chlorine species and the accumulation of chlorine species remain critical challenges.In this study,a Ru-modified(VO_(x))_(n)/CeO_(2) catalyst was synthesized via a pre-loading strategy.The pre-loaded Ru species not only created highly active redox sites favorable for deep CB oxidation through strong interactions with the CeO_(2) support but also enhanced the polymerization of V species and modulated the electronic environment of V=O species,enhancing the selective catalytic reduction(SCR)activity and the ability to cleave C-Cl bonds.Importantly,the Ru pre-loading preserved Brønsted acid site concentrations while decreasing Lewis acid site density,thereby reducing Cl deposition and improving catalyst stability.As a result,the optimized catalyst demonstrated superior performance,achieving over 90%NO_(x) and CB conversion in the 330-400℃ temperature range.The selectivities towards inorganic chlorine species(IC)and CO_(x) are both maintained above 90%.
基金the Beijing Outstanding Young Scientist Program(No.JWZ020240101014).
文摘Two-dimensional(2D)Bi_(2)O_(2)Se nanosheets,as an emerging ternary layered semiconductor,exhibit promising potential for photodetection owing to their moderate bandgap,high carrier mobility,and excellent environmental stability.However,their intrinsically high carrier concentration typically results in elevated dark currents and sluggish response speeds,thereby limiting further performance enhancement.To synergistically optimize both the response speed and sensitivity,we fabricated n-type Bi_(2)O_(2)Se nanosheets via chemical vapor deposition(CVD)and integrated them into a Bi_(2)O_(2)Se/InSe semivertical heterojunction photodetector featuring a single-sided depletion region.Benefitting from the type-II band alignment and the graphene bottom electrode,photogenerated carriers are efficiently separated and rapidly extracted.This design simultaneously shortens the carrier transit time and suppresses recombination,enabling the device to achieve high sensitivity(responsivity R of 0.47 A/W,detectivity D^(*) f 3.21×10^(12) Jones,external quantum efficiency(EQE)of 166.09%)while maintaining ultrafast response characteristics(rise/fall times of 48.5/41.7μs).The photodetector exhibits broadband selfpowered operation across ultraviolet(UV)to near-infrared wavelengths(300-1050 nm).These results highlight the significant potential of Bi_(2)O_(2)Se/InSe semi-vertical heterojunctions for high-performance,low-power,self-powered broadband photodetectors spanning the UV-visible-near infrared ray(UV-Vis-NIR)spectrum.
基金funding from SFB 1415 subproject B04(Deutsche Forschungsgemeinschaft,No.417590517)supported by the Deutsche Forschungsgemeinschaft through the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter-ct.qmat(EXC 2147,No.390858490)the support provided by the DRESDEN-concept alliance of research institutions.
文摘Twisted multilayers of two-dimensional materials attract widespread research interest due to their intriguing electronic and optical properties related to their chiral symmetry breaking and moiréeffects.The two-dimensional transition metal dichalcogenide MoSe_(2) is a particularly promising material for twisted multilayers,capable of sustaining moiréexcitons.Here,we report on a rational bottomup synthesis approach for twisted MoSe_(2) flakes by chemical vapor transport(CVT).Screw dislocation-driven growth was forced by surface-fused SiO_(2)nanoparticles on the substrates that serve as potential nucleation points in low supersaturation condition.Thus,crystal growth by in-situ CVT under addition of MoCl_(5) leads to bulk 2H-MoSe_(2) in a temperature gradient from 900 to 820℃ with a dwell time of 96 h.Hexagonally shaped 2H-MoSe_(2) flakes were grown from 710 to 685℃ with a dwell time of 30 min on SiO_(2)@Al_(2)O_(3)(0001)substrates.Electron backscatter diffraction as well as electron microscopy reveals the screw dislocation-driven growth of triangular 3R-MoSe_(2) with individual step heights between 0.9 and 2.9 nm on SiO_(2)@Si(100)under the same conditions.Finally,twisted MoSe_(2) flakes exhibiting a twist angle of 19°with respect to the[010]zone axis could be synthesized.
基金the Hong Kong Research Grants Council,Young Collaborative Research Grant(No.C5001-24)Research Institute for Smart Energy(No.UCDC9)+10 种基金Guangdong Provincial Department of Science and Technology(No.2024B1515040002)RSC Sustainable Laboratories Grant(No.L24-8215098370)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515012479)the Science and Technology Innovation Commission of Shenzhen(No.JCYJ20220818100206013)RSC Researcher Collaborations Grant(No.C23-2422436283)State Key Laboratory of Radio Frequency Heterogeneous Integration(Independent Scientific Research Program No.2024010)NTUT-SZU Joint Research Programsupported by the National Natural Science Foundation of China(No.52373248)Guangdong Provincial Department of Science and Technology(Nos.2024A1515010006 and 2024A1515011718)Guangdong Basic and Applied Basic Research Foundation(Nos.2023A1515012479 and 2025A1515011274)the Science and Technology Innovation Commission of Shenzhen(Nos.JCYJ20230808105900001,JCYJ20220531102214032,20231123155543001,and JCYJ20240813141813018).
文摘Multisensory integration allows biological organisms to merge information from various sensory modalities,enhancing perception,decision-making,and adaptability in complex environments.This process,involving specialized cortical and subcortical areas,reduces uncertainty,speeds up responses,enriches perception,and supports adaptive behaviors.Recent findings reveal that even primary sensory cortices contribute to multisensory processing,further boosting adaptability and decisionmaking.Inspired by these natural capabilities,researchers aim to develop artificial systems replicating biological sensory integration to address challenges in robotics,artificial intelligence,and big data.Current artificial systems,often reliant on single-modal perception,struggle in dynamic environments due to their limited adaptability.Advances in materials,device architectures,and neuromorphic technologies,such as memristor-and transistor-based neurons,are enabling the development of multimodal systems with enhanced efficiency,flexibility,and functionality.This review explores strategies to overcome single-modal limitations,focusing on synchronization,fusion,and deep interpretation of sensory data.Future directions emphasize improving integration density,novel device designs,and adaptable mechanisms.Multimodal systems hold promise to revolutionize artificial perception,narrowing the gap between biological systems and intelligent technologies.
基金supported by the Health Commission of Hubei Province scientific research project(No.WJ2021M143)the Fundamental Research Funds for the Central Universities(No.413000714)+2 种基金the Research Fund of Anhui Institute of translational medicine(No.2023zhyx-C61)the Research Fund Project of Anhui Medical University(No.2022xkj148)Hubei Society of Pathology General Project(No.2025HBAP013).
文摘Epilepsy is a complex neurological disorder aggravated by chronic neuroinflammation largely driven by reactive astrocytes.These cells promote epileptogenesis through persistent cytokine secretion and glial scar formation.Current antiepileptic drugs remain ineffective in targeting these mechanisms due to limited blood-brain barrier(BBB)permeability and poor astrocytic specificity.A transferrin-functionalized biomimetic nanotherapeutic loaded with resveratrol(RN@RTA)was developed to regulate astrocyte-mediated inflammation by activating sirtuin 1(SIRT1)and suppressing the mitogen-activated protein kinase/nuclear factor Kappalight-chain-enhancer of activated B cells(MAPK/NF-κB)axis.Using in vitro BBB models,primary astrocytes,and a pilocarpine-induced chronic epilepsy mouse model,we evaluated the capacity of RN@RTA to cross the BBB,inhibit inflammatory signaling,and reduce seizure activity.Mechanistic assays included immunoprecipitation of NF-κB complexes,cytokine quantification,RNA sequencing,and histopathological assessments of glial and synaptic markers.RN@RTA achieved 82%uptake by hippocampal astrocytes and significantly reduced Il6,Tnf-α,and Nlrp3 expression.SIRT1 activation disrupted the NF-κB p65/p300 complex,leading to transcriptional repression of inflammatory genes and enhancement of autophagy.In vivo,seizure frequency decreased by 67%,synaptic structure was preserved,and astrogliosis was markedly alleviated.The findings demonstrate a dual regulatory mechanism in which RN@RTA suppresses neuroinflammatory signaling and restores neural homeostasis,offering a promising molecularly targeted approach for refractory epilepsy.
基金supported by the National Key Research and Development Program of China(No.2021YFB4000603)the National Natural Science Foundation of China(Nos.52273277 and U24A2062)+2 种基金Jilin Province Science and Technology Development Plan Funding Project(No.SKL202302039)Youth Innovation Promotion Association CAS(No.2021223)funding from National Natural Science Foundation of China Outstanding Youth Science Foundation of China(Overseas).
文摘Proton-exchange membrane fuel cell and water electrolyzer(PEMFC and PEMWE)with high conversion efficiency and zero-carbon emission stand out as an attractive strategy for efficient conversion between hydrogen energy and renewable electricity.As a key component,efficient oxygen electrocatalyst for promoting sluggish reaction kinetics of oxygen reduction and evolution reaction(ORR and OER)under harsh operation conditions severely limited progress of these devices.Among various candidates,Ptgroup(Pt,Ir,and Ru)-based electrocatalysts are still the most active ORR/OER catalysts.However,the scarcity,high cost,and questionable stability restrict the widespread applications and the commercialization of PEMWE/PEMFC.Progresses in synthesizing atomically dispersed single/multiple-atom catalysts(SACs/MACs)offer new opportunities to Pt-group ORR/OER catalysts owing to nearly 100% metal utilization and high catalytic activities.Extensive efforts have been continuously devoted to optimizing the local structure of Pt-group OER/ORR catalysts at atom-level for further enhancing stability and activity.In this review,universal synthesis methods to prepare Ptgroup SACs are discussed first,highlighting crucial factors which affect the structure and catalytic performance.Afterward,advanced characterization techniques for directly confirming atomic dispersed metal atoms were introduced,including aberration-corrected high-angle-annular-dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy.Importantly,considerations for rational catalyst design and typical Pt-group SACs/MACs are summarized regarding the regulation strategy of atomically dispersed metal sites and various supports,and effects of metal-support interaction on the catalytic performance.Finally,key challenges and proposed perspectives for future development of atomically dispersed Pt-group oxygen electrocatalysts for fuel cell and electrolyzer are briefly discussed.
基金the National Key R&D Program of China(No.2024YFA1509500)the National Natural Science Foundation of China(No.22479010)+5 种基金the financial support from the Chongqing Municipal Natural Science Foundation(No.CSTB2024NSCQJQX0034)Shenzhen Science and Technology Program(No.KJZD20240903101359020)the financial support from the National Natural Science Foundation of China(No.22372004)the support from the Experimental Center of Advanced Materials of the Beijing Institute of Technologythe technical support from Biological and Medical Engineering Core Facilities of Beijing Institute of Technologythe Analysis and Testing Center of Beijing Institute of Technology.
文摘Fe-N-C catalysts,as promising non-precious metal alternatives for the oxygen reduction reaction(ORR),still suffer from severe mass transport limitations in proton exchange membrane fuel cells(PEMFCs)due to water flooding of active sites embedded in micropores.Although pore engineering through a selected template is a general strategy,the structural features of an ideal template,particularly those governing the exposure of active sites and thus affecting mass transport,remain elusive.Here,we demonstrate that low-porosity carbon templates maximize the ratio of active sites distributed at or near the surface,thereby enhancing their exposure and accessibility while reducing mass transport resistance during the ORR process.The C_(lp-1)@PPy and C_(lp-2)@PPy(PPy=polypyrrole)catalysts,derived from low-porosity carbon templates,achieve peak power densities of 0.96 and 1.03 W·cm^(-2) under H_(2)/O_(2)and 0.50 and 0.52 W·cm^(-2) under H_(2)/air,demonstrating excellent performance in PEMFC tests.Structural and electrochemical characterizations reveal that the enhanced surface exposure of active sites effectively mitigates mass transport resistance during the ORR,thereby offering a general design principle for overcoming mass transport limitations in Fe-N-C catalysts for PEMFC applications.
基金supported by Key R&D Program of Shandong Province,China(No.2025CXGC010407).
文摘Electromagnetic interference(EMI)shielding materials principally attain shielding by reflecting electromagnetic waves through impedance mismatch caused by high conductivity,which inevitably leads to secondary electromagnetic wave pollution.Consequently,the development of multifunctional,low-reflection electromagnetic shielding materials remains a significant challenge.Materials that are lightweight,possess high mechanical strength,exhibit excellent electromagnetic shielding absorption,and demonstrate low reflectivity have historically been the focus of significant interest.Natural silk,lightweight and strong,is an ideal composite matrix.Regenerated silk fibroin(RSF)synthesized via a bottom-up approach and cross-linked with polyvinyl alcohol(PVA)forms an aerogel matrix with remarkable compressive strength.In accordance with the principle of integrating functional design with structural design,spherical NiFe_(2)O_(4)particles were grown on the MXene surface via electrostatic self-assembly and combined with RSF/PVA as the aerogel absorptive layer,while RSF/PVA/MXene served as the reflective layer.A vertically oriented structure of Janus aerogel was prepared through sequential directed freezing.The resulting aerogel with 0.058 g/cm^(3) reveals the high compression strength(3.52 MPa).Reasonable functional and structural design enables aerogel to effectively dissipate incident electromagnetic waves through absorption,reflection,and reabsorption processes,achieving an average SET value of 48.05±1.75 dB and reaching a minimum reflection coefficient of 0.19.Furthermore,the aerogel displays remarkable infrared stealth capabilities.This lightweight,rigid,multifunctional aerogel is poised to play a significant role in the field of next-generation electronic devices.
基金supported financially by the National Natural Science Foundation of China(No.52172208)Taishan Scholar Young Talent Program(No.tsqn202306216)Shandong Excellent Young Scientists Fund Program(Overseas,2023HWYQ‑091).
文摘Oxygen reduction reaction(ORR)is crucial for Znair batteries,while also serves as a core electrochemical process in oxygen depolarized cathodes(ODCs)for chlor-alkali electrolysis.The lack of cost-effective,highly active ORR electrocatalysts with superior kinetics hinders progress in this field.Herein,we report the Fe/Ni dual single-atomic sites anchored by commercial carbon black(Fe/Ni-N/CB)using rigid ligand confined and high-temperature shock(HTS)strategy in less than 0.5 s.Theoretical calculation reveals that singleatomic Fe is the real active site.Single-atomic Fe and Ni species in Fe/Ni-N/CB synergistically accelerate the kinetics of ORR by reducing the energy barrier of the rate-determining step.A large half-wave potential(E_(1/2))of 0.907 V is achieved in 0.1 M KOH aqueous solution.The assembled aqueous Zn-air battery(A-ZAB)with Fe/Ni-N/CB cathode presents remarkable charge-discharge cycling stability for over 650 h without voltage gap degradation.The quasi-solid-state Zn-air battery(QSS-ZAB)exhibits excellent reversibility over a 150-h operation at 0.5 mA·cm^(-2) with negligible energy conversion efficiency recession.Impressively,Fe/Ni-N/CB||RuO_(2)chloralkali flow cell exhibits a low cell voltage of 1.60 V at a large current density of 300 mA·cm^(-2) at 80℃,and demonstrates exceptional durability with 7% current density decay over 150 h of continuous operation at 100 mA·cm^(-2).Fe/Ni-N/CB||RuO_(2)achieves near-ideal caustic current efficiency(~97.2%)at the current density of 300 mA·cm^(-2).This work provides a rapid and economical synthesis technique for the synthesis of catalysts at the atomic scale while demonstrating significant potential for application in energy-saving chlor-alkali electrolyzer.
基金the National Natural Science Foundation of China(No.52373311)the Innovation Program for Quantum Science and Technology(No.2021ZD0301605)+3 种基金provided by the National Natural Science Foundation of China(Nos.92263202 and 12374020)the National Key Research and Development Program of China(No.2020YFA0711502)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB33000000)support from the Australian Research Council(ARC Discovery Project,No.DP180102976).
文摘The magnetic proximity effect enables interfacial modulation of excitonic and spin-valley properties in transition metal dichalcogenides(TMDs),offering a versatile route toward next-generation spintronic and valleytronic devices.However,the inherently weak photoluminescence(PL)of bright excitons—suppressed by proximity-induced darkening mechanisms—hinders the optical detection of magnetic interactions.Here,we demonstrate substantial exciton emission enhancement in CrOCl/WSe_(2)(HS)and twisted 90°-CrOCl/CrOCl/WSe_(2)(THS)heterostructures by employing plasmonic Au nanopillar arrays to activate surface plasmon polariton(SPP)coupling.The neutral exciton emission intensity is enhanced by factors of 5 and 18 for HS/Au and THS/Au,respectively,with enhancements persisting under high magnetic fields and elevated temperatures(~10-fold in THS/Au).Enabled by this amplification,we observe pronounced Zeeman splitting and modified intervalley relaxation pathways,indicating significant magnetic proximity interactions.Finite-element simulations and first-principles calculations reveal that the enhancement arises from local electromagnetic field concentration and layer-dependent interfacial coupling.Our results establish SPP-assisted PL enhancement as an effective strategy for probing weak magneto-optical signatures,paving the way for detailed exploration of exciton-magnon coupling and interface-driven quantum phenomena in twodimensional(2D)magnetic heterostructures.
基金supported by National Natural Science Foundation of China(Nos.82104445 and 82470182]Basic Scientific Research Funds of Department of Education of Zhejiang Province(No.KYZD2024013)+2 种基金The Startup Foundation of Zhejiang Provincial People’s Hospital(Nos.C-2023-QDJJ12 and C-2024-ZZJJ05)Science and Technology Plan Project of Traditional Chinese Medicine in Zhejiang Province(No.2025ZR007)The National Administration of Traditional Chinese Medicine(No.GZY-ZJ-KJ-24044).
文摘Myelosuppression is a common and severe side effect of cancer chemotherapy,with current treatments hindered by limitations such as depletion of hematopoietic reserves,poor patient compliance,delayed therapeutic onset,and high cost.To overcome these challenges,we developed Epimedium-derived nanovesicles(ENVs)from the traditional Chinese medicinal herb Epimedium,addressing the solubility and bioavailability issues associated with conventional extracts.ENVs encapsulate bioactive constituents,including icariin and hematopoiesis-promoting ceramides.In a cyclophosphamide(CTX)-induced myelosuppression mouse model,prophylactic and therapeutic oral administration of ENVs effectively alleviated hematopoietic suppression,significantly outperforming the Epimedium-based herbal extract“Joungal”(Shengbai Formula)despite equivalent icariin content.Notably,ENVs promoted hematopoietic stem cell(HSC)proliferation—an outcome rarely achieved with existing therapies.Mechanistically,ENVs modulated the gut microbiota,enriching lactobacillus species and enhancing lactate production.This microbiota-driven lactate signaling stimulated LepR+mesenchymal stem cells(MSCs)in the bone marrow niche to secrete stromal cellderived factor-1(SDF-1)and stem cell factor(SCF),thereby supporting HSC expansion and restoring hematopoietic function.In vivo safety evaluations confirmed the excellent biocompatibility of ENVs.Our findings uncover a gut-lactate-bone marrow axis through which ENVs enhance hematopoiesis and promote HSC regeneration.This work introduces a cost-effective,scalable,and orally administrable biomaterial platform with strong translational potential for the prevention and treatment of chemotherapy-induced myelosuppression.
基金the National Natural Science Foundation of China(No.52472084).
文摘Water,salt solution,and many conventional organic solvents exhibit melting temperatures nearly or well below zero degree,and functional phase change composites based on these components will be useful in energy and environmental areas.Here,we report the design and fabrication of a series of composite hydrogels and organogels consisting of water,NaCl/water eutectic solution,n-undecane,and n-heptanol held by a built-in carbon nanotube(CNT)-polymer skeleton,respectively.We adopt an initially uniform yet transformable CNT network to mix with gel precursors and obtain densified CNT-reinforced pore walls by in situgelation.These composite gels realized solid-liquid phase transition in temperatures ranging from−10 to−36℃,with reduced supercooling,large enthalpy(120 to 200 J/g),enhanced structural stability and anti-leakage property,and the effects of CNTs on thermal and mechanical properties are investigated systematically.We demonstrate that by wrapping the composite gels around pipe models with cold liquid flow,the temperature increase process could be substantially prolonged,owing to efficient latent heat release during phase change.Our CNT-reinforced hydrogels and organogels,made by a general,facile approach,have many potential applications as cold energy storage and transformation media in liquefied natural gas industry,food,and biomedical fields.
基金supported by the National Natural Science Foundation of China(Nos.82101647 and 82203446)Natural Science Fund of Zhejiang Province(Nos.LY24H250001,LQN25H060003,and LY23H060011)+2 种基金the Postdoctoral Fellowship Program of CPSF(No.188020-170257701/136)the Regional Innovation and Development Joint Fund of the National Natural Science Foundation of China(No.U22A20282)the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515220225).
文摘Osteoarthritis(OA),a debilitating joint disorder affecting millions worldwide,is characterized by persistent inflammation,oxidative stress,and irreversible cartilage breakdown,yet remains without diseasemodifying therapies.Inspired by natural enzymatic cascades,we developed a bioinspired nanocomposite hydrogel,N,S-doped Mn-Nb(C-CeO),that mimics endogenous antioxidant pathways to reprogram the OA microenvironment.This system combines N,Sdoped Mn-Nb_(2)C MXene nanosheets with CeO_(2)nanozymes within a boronate ester-crosslinked hydrogel,forming an“immuno-redox circuitry”with four synergistic functions:(1)cascade reactive oxygen species(ROS)scavenging via superoxide dismutase-like Mn-Nb_(2)C and catalase-like CeO_(2),amplified by photothermal enhancement under near-infrared irradiation;(2)broad reactive nitrogen species clearance,removing peroxynitrite(ONOO^(-)),nitric oxide(NO),and nitroxyl(NO^(-))to mitigate inflammation;(3)immunomodulation through Mn^(2+)-activated cGAS-STING signaling,which promoted macrophage polarization toward the M2 phenotype,concomitantly reducing the levels of pro-inflammatory cytokines such as interleukin-1 beta(IL-1β)and tumor necrosis factor-alpha(TNF-α);(4)cartilage regeneration via pH/ROS-responsive simvastatin(SIM)release and nanocatalysis,upregulating SRY-box transcription factor 9(SOX9)and Col2a1 while inhibiting matrix metalloproteinase-13(MMP-13)and a disintegrin and metalloproteinase with thrombospondin motifs 5(ADAMTS5).In a murine OA model,the system reduced synovitis by 60%,restored 80% of cartilage thickness,and suppressed osteophyte formation,outperforming singlecomponent treatments.This strategy pioneers a“self-healing cartilage”approach by integrating nanocatalysis with immunoengineering for transformative OA therapy.
基金supported by the National Natural Science Foundation of China(Nos.12374345,U24A20103,12404358,and 12304309)the Natural Science Foundation of Zhejiang Province(Nos.LZ26E010002 and LQN25A040010)+2 种基金the Key R&D Project of Zhejiang Province(No.2024C03258)the Fundamental Research Funds for the Provincial Universities of Zhejiang(No.GK259909299001-310)the Hong Kong Joint Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province(No.2023B1212120011).
文摘Metal-semiconductor plasmonic metasurfaces enable precise optical field manipulation at the subwavelength scale;however,most existing designs rely on external fields and exhibit only binary responses,thereby restricting the realization of multistate logic operations.Here,we present an in-situ polarization-controlled approach based on an Au-indium tin oxide(ITO)bilayer nanocrescent with a Schottky heterojunction for achieving polarization-dependent tristate optical modulation.Polarization-selective excitation of distinct localized plasmon modes facilitates directional hot-electron injection across the Au-ITO interface,thereby producing three distinct programmable states—positive,zero,and negative—at a single detection wavelength.This symmetric bilayer design is applicable to other metal-semiconductor composites and offers generalizable design principles for ternary logic,multistate optical encoding,and ultrafast photonic information processing.The proposed concept is validated through both experimental measurements and numerical simulations.
