To solve the slow dynamics of catalytic oxygen reaction energy devices,a facile method was developed for the synthesis of methylene alcohol terminated poly(1,4-phenyldiimine)porphyrin cobalt(MPImPorCo),which was synth...To solve the slow dynamics of catalytic oxygen reaction energy devices,a facile method was developed for the synthesis of methylene alcohol terminated poly(1,4-phenyldiimine)porphyrin cobalt(MPImPorCo),which was synthesized by RuCl3 catalyzed redox reaction of meso-5,10,15,20-tetra(4-nitrophenyl)porphyrin cobalt(TNO2PorCo)and 1,4-phenyldimethanol.M-PImPorCo is a fully conjugated covalent organic framework(COF)with high thermal and chemical stability.COFs with different edge groups were synthesized to compare the effect of different groups(–CH_(2)–OH and–NO_(2))on catalytic bifunctional oxygen reaction activity.C=N as nitrogen-rich environment of M-PImPorCo leads to the protonation process of oxygen catalysis and reduces the energy barrier of adsorption in the oxygen intermediate.C=N and–CH_(2)–OH form an“electron pump”structure to deliver electrons to the Co–N4 site in M-PImPorCo,and theπ–πinteraction between M-PImPorCo and three-dimensional graphene(3D-G)can further enrich the electron cloud density of Co–N4 sites.M-PImPorCo/3D-G has remarkable oxygen catalytic performance,with a half-wave potential(E_(1/2))of 0.91 V vs.reversible hydrogen electrode(RHE).M-PImPorCo/3D-G has low potential(Ej=10 is 1.49 V vs.RHE)at a current density of 10 mA·cm^(-2).It exhibits a good bifunctional catalytic performance(potential difference(ΔE)=0.58 V).The smaller charge–discharge band gap of zinc-air batteries(ZABs)and flexible ZABs(F-ZABs)equipped with M-PImPorCo/3D-G suggests the potential for catalytic oxygen reaction bifunctional applications.This work provides a new idea for the synthesis of Schiff-base porphyrin-based COF catalyst and its potential application to oxygen reaction catalytic energy storage devices.展开更多
With the popularization of fifth-generation(5G)technology,even the next generation-6G and portable electronic products,electromagnetic wave pollution poses a serious threat to human physical and mental health and the ...With the popularization of fifth-generation(5G)technology,even the next generation-6G and portable electronic products,electromagnetic wave pollution poses a serious threat to human physical and mental health and the normal operation of devices.The rapid development of display screens,medical equipment,and aerospace equipment has led to a surge in demand for highperformance transparent electromagnetic shielding materials to reduce electromagnetic interference(EMI)while ensuring optical clarity.This review systematically examines the latest developments in transparent EMI shielding materials,with a focus on their mechanisms,key material categories,and strategies for balancing shielding effectiveness(SE)and transmittance.The shielding mechanism(reflection,absorption,and multiple reflections)was analyzed through transmission line theory.This work reviews transparent EMI shielding materials based on transparent conductive oxides(TCOs),metal networks(MNs),carbonbased materials(CBMs),MXene,and other materials(OMs).The future development prospects and challenges of transparent EMI shielding materials were discussed.The review aims to promote the development of next-generation materials with high EMI shielding,optical transparency,and adaptability to complex environments.展开更多
The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of m...The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of metal phosphates,their precipitation in aqueous solution becomes too fast to control,making it a significant challenge to ensure a heterogeneous growth process towards surface coatings.Herein,we report a solution-based synthetic process to achieve conformal metal phosphate coating through coordination-assisted precipitation,which involved the reaction between phytic acid(PA),urea,and metal ions,particularly Nb^(5+),in ethanol solution to achieve a well-tamed coating effect.The use of PA,a plant-derived compound known as inositol hexaphosphoric acid,was facile to form soluble phytate-metal complex,which precipitated with urea to form metal-phosphate-containing coatings with thickness controlled at high precision.This proposed synthetic protocol was applied for the surface coating of high-voltage cathode materials in the form of LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),leading to significantly enhanced structural and electrochemical stability for its working at 5 V.Notably,after 300 cycles,the modified LNMO was able to achieve capacity retention of 85.1%for its working at 45℃ at a current density of 1 C as compared to only 29.9%of the pristine sample.Our findings highlight the potential of solution-based processes in building conformal coatings for the stabilization of high-energy cathode materials in their LIBs application.展开更多
Triboelectric nanogenerators(TENGs)represent a promising technology for next generation human–computer interaction.The effective enhancement of induced charges are critical factors that determine the recognition accu...Triboelectric nanogenerators(TENGs)represent a promising technology for next generation human–computer interaction.The effective enhancement of induced charges are critical factors that determine the recognition accuracy of TENGbased tactile sensors.Here,we propose a magnetic fieldassisted TENG device utilizing waveform feature enrichment strategies to significantly enhance the tactile recognition accuracy in natural environments.An elastic micro-nano structure was fabricated on a polydimethylsiloxane(PDMS)film via a facile templating method.Leveraging the inherent hydrophobicity and microscale surface roughness of PDMS,our device demonstrates stable and distinct waveform characteristics under natural operating conditions.Importantly,the introduction of a magnetic field generates a Lorentz force,which effectively modulates induced charges within the electrode,yet minimally affects triboelectric charges at the PDMS interface.This selective modulation induces an asymmetric charge distribution inside the electrode,substantially increasing the induced charge density,consequently,subtle waveform features are markedly enhanced.These enriched signal features play a crucial role in elevating material recognition accuracy.As a result,the sensor achieves a remarkable recognition accuracy of 99%when distinguishing among ten different materials under magnetic field assistance.This work provides valuable guidelines for advancing the performance and accuracy of TENG-based tactile sensing systems.展开更多
Anisotropic two-dimensional(2D)semiconductors have emerged as promising candidates for polarization-resolved photodetection due to their intrinsic in-plane optical anisotropies and linear dichroisms.However,their prac...Anisotropic two-dimensional(2D)semiconductors have emerged as promising candidates for polarization-resolved photodetection due to their intrinsic in-plane optical anisotropies and linear dichroisms.However,their practical applications are often constrained by limited spectral response and low anisotropy ratios.In this work,we report a broadband polarization-sensitive photodetector based on a type-II p-GaTe/n-PdSe_(2) van der Waals heterostructure,where interfacial band engineering—through the combined effect of the builtin p–n junction field and Schottky barrier—enables efficient carrier separation and unconventional reverse rectification.The device exhibits a high reverse rectification ratio(>10^(2))and an ultra-low forward dark current(~10^(-11) A).Owing to the engineered band alignment,it achieves broadband photodetection from 365 to 940 nm,with a high photoswitching ratio(>10^(3)),responsivity(~10^(3) A/W),detectivity(~10^(13) Jones),and external quantum efficiency(~10^(4)%).Furthermore,strong polarization sensitivity is demonstrated,with polarization ratios of 5.39,4.71,and 4.60 at the wavelengths of 365,520,and 940 nm,respectively,highlighting the potential of this heterostructure for high-performance and polarization-resolved optoelectronic applications.展开更多
Fabricating organic solar cells(OSCs)in open-air and room-temperature environments is essential for cost-effective roll-to-roll printing,but its performance is limited by non-ideal block and surface morphology of acti...Fabricating organic solar cells(OSCs)in open-air and room-temperature environments is essential for cost-effective roll-to-roll printing,but its performance is limited by non-ideal block and surface morphology of active layer.Herein,we demonstrate a record power conversion efficiency(PCE)of 19.72%in open-air and as-cast processed devices by using a lowcost terpolymer donor(PTQ20-5)to optimize the block and surface morphology.Compared with the counterpart PTQ10,PTQ20-5 shows increased hydrophobicity,which can better prevent the intrusion of H2O molecules in the film formation process in open-air environment,giving excellent humidity tolerance of corresponding devices.Moreover,the enhanced dielectric constant results in reduced exciton binding energy and improved charge transport of PTQ20-5,leading to improved charge separation and transfer,and suppressed carrier recombination in the devices.Besides,the PTQ20-5-based film has more appropriate block morphological features of balanced molecular self-assembly and phase separation,which simultaneously promotes the charge carrier transport and inhibits the carrier recombination at the donor/acceptor interface.This work is of great significance for promoting the industrialization of OSCs.展开更多
Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhan...Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhancing their optical performance remains greatly challenging.In this work,an effective strategy is employed to achieve highperformance OLETs by constructing a two-dimensional molecular-scale passivation layer at the dielectric/channel interface using a promising solution-processed small-molecule material,tetratetracontane(TTC).By controlling the microscopic flows driven by intermolecular interactions near the solution meniscus,molecular self-assembly dynamics are effectively regulated,contributing to a significant transformation in molecular layer stacking mode and enabling the formation of large-area TTC thin films with two-dimensional molecular-scale surface structure and uniform morphology.The introduction of high-quality TTC passivation layer film into the dielectric/channel interface optimizes the film morphologies of overlying channel layer,effectively shields the electrostatic dipole effects at dielectric/channel interface,leading to the synergistic optoelectronic regulation and enhanced optical properties of OLETs.Consequently,high brightness of 10,077.3 cd·m^(-2),high external quantum efficiency(EQE)of 20.46%,and low voltage of 15 V are achieved in the lateral OLET.This work presents a promising approach for two-dimensional molecular-scale small molecule interfaces,and provides an effective strategy for achieving high-performance OLET devices.展开更多
Second window near-infrared(NIR-II)light is preferred for photothermal therapy due to its deeper tissue penetration,reduced scattering,and improved imaging guidance compared to NIR(I)light.However,NIR-II–absorbing go...Second window near-infrared(NIR-II)light is preferred for photothermal therapy due to its deeper tissue penetration,reduced scattering,and improved imaging guidance compared to NIR(I)light.However,NIR-II–absorbing gold nanomaterials with low cytotoxicity,well-defined structural stability,controllable size,and excellent dispersibility have been rarely reported.Compared with nanospheres and nanorods,gold nanostars have lower cytotoxicity,lower oxidative stress damage,higher intracellular enrichment in tumor cells,and maintain their labeling activity after circulation in vivo.Here,we reported a well-defined and easily synthesized gold nanotetrapods(AuNTPs)material absorbing NIR(II).This material not only meets the requirements for localized tumor hyperthermia but also reprograms the tumor microenvironment by enhancing tumor cell antigen presentation,converting"cold"tumors into"hot"tumors.Additionally,AuNTPs-based photothermal therapy induced by NIR-II irradiation enhances the antitumor functions of dendritic cells,T cells,and NK cells in the systemic immune response,inducing a sustained antitumor immune effect.The tumor microenvironment modulation properties exhibited by these AuNTPs may provide new avenues for exploring precise,non-invasive optical modulation nano anti-cancer therapy platforms within the NIR(II)window.展开更多
Gemcitabine(Gem)is the gold-standard chemotherapeutic drug for pancreatic cancer therapy in clinic.However,intratumoral bacteria can metabolize Gem into an inactive form,leading to Gem resistance.To address this chall...Gemcitabine(Gem)is the gold-standard chemotherapeutic drug for pancreatic cancer therapy in clinic.However,intratumoral bacteria can metabolize Gem into an inactive form,leading to Gem resistance.To address this challenge,Zn^(2+)-containing nanoparticles(ZGP NPs)are used to eliminate intracellular bacteria to enhance the therapeutic efficacy of Gem in pancreatic therapy.ZGP NPs are prepared via a facile one-pot method using Zn2+,epigallocatechin gallate(EGCG),and polyethylene glycol(PEG),which prevents metal ion chelation by proteins and ensures antibacterial activity.Leveraging the pH-responsive disassembly of metal-phenolic networks,ZGP NPs can be degraded in acidic lysosomes after cellular uptake,releasing Zn^(2+)to eliminate intracellular bacteria and thereby protecting Gem from bacteria-mediated inactivation.Moreover,the elimination of intratumoral bacteria enhances immunotherapy.The delivery of Zn^(2+)via ZGP NPs presents a promising strategy to eliminate intratumoral bacteria to overcome Gem resistance in pancreatic cancer therapy.展开更多
Metabolic-associated fatty liver disease(MAFLD),a global health burden with limited therapeutic options beyond lifestyle changes,urgently needs novel strategies.We engineered exosome-like nanovesicles(HNVs)from dried ...Metabolic-associated fatty liver disease(MAFLD),a global health burden with limited therapeutic options beyond lifestyle changes,urgently needs novel strategies.We engineered exosome-like nanovesicles(HNVs)from dried honeysuckle(Lonicera japonica),exhibiting significantly more uniform size distribution than conventional herbal extracts and characteristic nanovesicle morphology.Orally delivered HNVs,enriched with bioactive metabolites,dramatically inhibited increased fat vacuoles,lipid droplet deposition,and collagen fibrosis in the livers of mice with MAFLD induced by high-fat diet(HFD).Mechanistically,HNVs orchestrate a dual gut-liver intervention:(1)restoring gut barrier integrity,slashing serum LPS by 1.58-fold and quelling hepatic inflammation;(2)remodeling gut microbiota to suppress bile salt hydrolase(BSH),elevating taurochenodeoxycholic acid(TCDCA)2.07-fold.This microbial shift reprograms enterohepatic signaling by inhibiting the FXR-FGF15-FGFR4 axis,thereby boosting hepatic cholesterol catabolism via bile acid synthases.Critically,efficacy is strictly microbiotadependent:abolished by antibiotics and fully transferable via fecal microbiota transplantation(FMT)from HNV-treated donors.Presenting the first natural nanovesicle platform that concurrently targets gut barrier repair and metabolic reprogramming,HNVs establish a pioneering,multi-targeted therapeutic paradigm for MAFLD,directly linking gut microbial ecology to hepatic pathophysiology with high translational potential.展开更多
Supported single-atom catalysts(SACs)demonstrate exceptional catalytic performance,atom efficiency,and selectivity,as a result,they are the potential candidates used in oxygen evolution reaction(OER).However,stabilizi...Supported single-atom catalysts(SACs)demonstrate exceptional catalytic performance,atom efficiency,and selectivity,as a result,they are the potential candidates used in oxygen evolution reaction(OER).However,stabilizing monodispersed noblemetal atoms is challenging.This is especially true for two-dimensional(2D)layered double hydroxide(LDH)nanostructures.Here,we report the successful stabilization of ruthenium(Ru)single atoms(SAs).These SAs are located within a defective NiFe LDH nanosheet grown on the nickel foam(NF).This material is named Ru SAs/D-NiFe LDH@NF and formed through the*OOH hydrothermal reaction followed by etching.The resulting catalyst exhibits outstanding OER performance in alkaline media,achieving an exceedingly low overpotential(206 mV)at 50 mA·cm^(-2),which remarkably decreases relative to the overpotential in pristine NiFe LDH(311 mV).Ru SAs regulate the electron distribution near defects,optimizing the Ru-NiFe hydroxide interaction and diminishing energy barrier for forming intermediates,as revealed by density functional theory(DFT)calculations.Moreover,the catalyst demonstrates remarkable stability in Zn-air batteries(ZABs),delivering the maximal power density(170 mW·cm^(-2)).Furthermore,it maintains stable operation for 350 h,highlighting its practical viability.This work provides a versatile strategy for integrating single-atom sites into NiFe LDH,paving the way for the design of next-generation SACs for energy conversion applications.展开更多
Appropriate non-metallic element doping is promising to improve the intrinsic electrocatalytic oxygen reduction reaction(ORR)performance of nitrogen-doped carbon candidates,yet challenges still remain to rationally de...Appropriate non-metallic element doping is promising to improve the intrinsic electrocatalytic oxygen reduction reaction(ORR)performance of nitrogen-doped carbon candidates,yet challenges still remain to rationally design of the catalyst configuration with kinetically favorable state.Herein,we propose the metalloid element to regulate the local electronic environment,and a novel metal-free electrocatalyst,namely,atomically dispersed Te-N_(2) on nitrogen-doped carbon frameworks was developed.Characterization and theoretical analyses demonstrate that the heteroatoms tellurium integrated with nitrogen-doped carbon substrate forms a Te-N covalent coordination as the active center that empowers both improved ORR kinetics and structural stability.As expected,the optimized composite of Te-N-C 900 delivers considerable electrocatalytic ORR activity in alkaline media(E_(1/2)=0.871 V,0.1 M KOH),along with encouraging durability(over 10,000 cycles with 13 mV decay),which is also responsible for Zn-air batteries operating with high uplifting peak power density and long lifespan.As a proof-of-concept,this work elucidates the key influence of heteroatom interaction of metalloid element,achieves the synthesis of Te-N_(2) metal-free ORR catalysts,and provides guidance for the development of high-performance metal-free ORR catalysts.展开更多
Uranium extraction from seawater(UES)is crucial for reducing nuclear fuel supply pressure and promoting the comprehensive utilization of marine resources.The successful implementations of UES engineering critically re...Uranium extraction from seawater(UES)is crucial for reducing nuclear fuel supply pressure and promoting the comprehensive utilization of marine resources.The successful implementations of UES engineering critically rely on the highly efficient sorbent materials with exceptional performance in binding uranyl ions.Herein,a universal and facile“organic ion building blocks self-assembly”strategy is established to realize a first class of carboxyl functionalized ionic single crystals,named BPTC-BPY-R(R=1–6,the R corresponds to alkyl chain length modifier,e.g.,R=1 corresponds to iodomethane derivatives,R=2 corresponds to bromoethane derivatives,etc.),derived from rationally designed viologen-derivatives with different alkyl chain lengths and polycarboxylic acid.This strategy effectively exploits the organic ion building block properties to achieve U(VI)adsorption based on the synergistic effects of anions(ligand interaction)and cations(electrostatic interaction).Notably,attributed to the special crystal stacking mode and higher specific surface area,the resulting BPTC-BPY-3 not only achieves ultrahigh selectivity for U(VI)adsorption with a partition coefficient of 3.998×10^(6) mL/g,but also possesses an ultrafast U(VI)adsorption kinetics and an uptake capacity of 686.8 mg/g within 2 min.More importantly,it realizes a U(VI)uptake capacity of 7.41 mg/g from natural seawater in 20 days.The designed material with ultra-selectivity,high capacity,ultrafast kinetics,and good recyclability exhibits a great promise for efficient U(VI)extraction from seawater.展开更多
Electromagnetic pollution is becoming significantly serious.Therefore,it is critical to prepare the advanced electromagnetic interference(EMI)shielding materials with thinness,flexibility and high mechanical strength....Electromagnetic pollution is becoming significantly serious.Therefore,it is critical to prepare the advanced electromagnetic interference(EMI)shielding materials with thinness,flexibility and high mechanical strength.Herein,the copperbased metal-organic framework(MOF-Cu)and polyethyleneiminemodified ammonium polyphosphate(PEI-APP)were successfully synthesized.The flame-retardant thermoplastic polyurethane(TPU)composite was successfully prepared by compounding MOF-Cu and PEI-APP.The Cotton@PDA@MXene composite was fabricated via a sequential loading process of polydopamine(PDA)and MXene onto cotton fabric.Then,the multilayer TPU composites were prepared by layer-by-layer hot-pressing.The TPU/9PAPP/1MOF/C-3PM composite exhibited exceptional EMI effectiveness of 20.5 dB in X-band and 23.0 dB in K-band,exceeding commercial standards.The TPU/9P-APP/1MOF/C-3PM composite also demonstrated significantly enhanced flame retardancy.Compared with pure TPU/Cotton sample,the peak heat release rate,total heat release and total smoke release of TPU/9PAPP/1MOF/C-3PM composite decreased by 40.7%,31.1%,and 33.3%,respectively.Furthermore,the thickness of the multilayer TPU composites was only 1 mm,demonstrating excellent flexibility.As the outer encapsulation material,TPU endowed the multilayer TPU composites outstanding durability and effectively addressed the common issues of fabric abrasion and conductive filler detachment.This study provides a novel strategy for preparing flexible electromagnetic interference shielding materials with superior flame retardancy.展开更多
To address postoperative melanoma issues of high recurrence and poor wound healing,we developed a nanocomposite hydrogel wound patch(M_(xNd/yCe)@M SAC)for cascade sequential therapy.Methotrexate(MTX)loaded Nd/Ce-doped...To address postoperative melanoma issues of high recurrence and poor wound healing,we developed a nanocomposite hydrogel wound patch(M_(xNd/yCe)@M SAC)for cascade sequential therapy.Methotrexate(MTX)loaded Nd/Ce-doped mesoporous bioactive glass was encapsulated in a sulfobetaine-polyacrylamide-carboxymethyl chitosan hydrogel via thermal polymerization.Under the acidic microenvironment of the residual tumor,the amide bonds in M_(xNd/yCe)@M SAC are broken,releasing M_(xNd/yCe)@M.M_(xNd/yCe)@M targets tumor cells,and the combined therapy of mild photothermal treatment and chemotherapy ablates tumor cells.Subsequently,the continuously released MTX downregulates the expression of pro-inflammatory factors and reshapes the immune microenvironment.Finally,M_(xNd/yCe)@M disintegrates,releasing Si^(4+),Ca^(2+),P^(5+)and Ce^(3+)ions,which can effectively promote angiogenesis and tissue repair.In the postoperative melanoma model,this method effectively cleared the residual tumors after surgery,shortened the inflammatory period,and promoted tissue regeneration.In conclusion,the nanocomposite hydrogel wound patch for cascade sequential treatment prepared in this study has excellent anti-tumor,immune regulation and tissue repair properties,providing prospective insights for the postoperative treatment of malignant melanoma.展开更多
The rising global burden of cancer necessitates innovative therapeutic strategies,with immunotherapy demonstrating remarkable potential.However,its clinical efficacy remains limited by low response rates and non-speci...The rising global burden of cancer necessitates innovative therapeutic strategies,with immunotherapy demonstrating remarkable potential.However,its clinical efficacy remains limited by low response rates and non-specific(off-target)delivery.This review highlights natural polymer-based hydrogels as emerging delivery platforms engineered to enhance the efficacy of cancer immunotherapy.These hydrogels exploit the biocompatibility and biodegradability of natural polymers,employing chemical or physical crosslinking to encapsulate and deliver immunotherapeutic agents.The versatility of these hydrogels is discussed in the context of oral,sprayable,injectable,and implantable formulations,which are adaptable to specific tumor sites.Their responsiveness to stimuli such as pH,temperature,and enzymatic activity enables controlled and sustained release of immunotherapeutic agents,including checkpoint inhibitors,cytokines,and Toll-like receptor agonists.These hydrogels can also modulate the tumor microenvironment by regulating pH,oxygen levels,and immune cell infiltration,thereby enhancing therapeutic efficacy.Moreover,immunotherapeutic hydrogels can act synergistically with chemotherapy,radiotherapy,and phototherapies to enhance antitumor immune responses.Despite their potential,challenges such as degradation kinetics,bioactivity retention,and regulatory hurdles must be addressed to ensure successful clinical translation.This review provides insights into the rational design,development and application of stimuli-responsive hydrogels as next-generation platforms for effective cancer immunotherapy.展开更多
Rational design of electrochemical sulfide oxidation reaction(SOR)catalysts is a prerequisite to fully recycling hydrogen(H_(2))and elemental sulfur(S0)resources,realizing the bridge between environment and energy fie...Rational design of electrochemical sulfide oxidation reaction(SOR)catalysts is a prerequisite to fully recycling hydrogen(H_(2))and elemental sulfur(S0)resources,realizing the bridge between environment and energy fields,as well as enlightening the optimization of metal‒sulfur battery applications.While transition metal catalysts often suffer from sulfur poisoning,single-atom catalysts(SACs)offer a promising solution,where the precise coordination environment of metal centers becomes a critical determinant of catalytic performance.Herein,for the first time,we develop a Ni single-atom catalyst for SOR with unique Ni-N_(3)O_(1) coordination anchored on hierarchically porous carbon(Ni1@HPC),which demonstrates remarkable advantages over conventional Ni-N_(4) or Ni-O4 configurations,exhibiting a superior SOR activity(0.37 V vs.RHE at 100 mA·cm^(-2))that surpasses reported carbon-based catalysts and is comparable to most metal-based catalysts.In situ Raman and density functional theory(DFT)results reveal that the HPC facilitates rapid product S0 desorption while the Ni-N3O1 coordination enables appropriate reactant sulfide(S^(2-))adsorption,striking a critical balance between activity and stability that other coordination geometries fail to achieve.Additionally,the practical application of coupling hydrogen evolution reaction(HER)and SOR is realized on Ni1@HPC with low power consumption,which is a promising alternative to the traditional overall water splitting(OWS)process.This work not only establishes a structure–activity relationship for single-atom catalysts in SOR but also provides a general strategy for optimizing metal coordination in electrocatalytic systems.展开更多
Metal-bio-oxygen batteries establish a paradigmshifting energy architecture for biomedical implants,endowing these devices with extended service life in continuous physiological surveillance and precision theranostic ...Metal-bio-oxygen batteries establish a paradigmshifting energy architecture for biomedical implants,endowing these devices with extended service life in continuous physiological surveillance and precision theranostic operations.However,the conventional electrolytes in these semi-opened batteries fail to meet the requirements in biocompatibility and bio-safety for in vivo applications.Herein,we report a bio-compatible composite gel electrolyte for implanted Zn-O_(2) battery(ZOB),while also sustainably powering a mechanical sensor in vivo.This electrolyte composes a poly(L-lactide-co-epsilon-caprolactone)(PLCL)framework with a gelatin methacryloyl(GelMA)modification layer,and the salt in body fluid serves as ion transport carriers in the electrolyte.It displays an O_(2) impermeable property and lower polarization potentials as electrolyte in Zn||Zn symmetric cell.In vitro assay results demonstrate that the battery components illustrate excellent biocompatibility with negligible cytotoxicity.In vivo histopathological and hematological analyses further verified the biosafety of ZOB during operation,while capillary regeneration around the cathode ensured adequate oxygen supply for sustained performance.The assembled ZOB delivers a power density of 1.96μW/cm^(2) at 0.98 V in vivo,which also successfully powers an integrated hydrogel mechanical sensor and monitors cardiac signals in rats.The unique two-electron transfer pathway of oxygen reduction in blood has also been elucidated.This work offers a new insight into bio-compatible electrolyte design for next-generation implantable power sources,enabling robust implantable devices for healthcare technologies.展开更多
The delicate balance of oral microbiota is frequently disrupted by exogenous discoloration and biofilm formation,thus requiring integrated antibacterial and whitening strategies.Conventional peroxide treatments often ...The delicate balance of oral microbiota is frequently disrupted by exogenous discoloration and biofilm formation,thus requiring integrated antibacterial and whitening strategies.Conventional peroxide treatments often damage the integrity of tooth enamel,while nanocatalysts pose cytotoxicity risks.In this work,we designed a biocompatible polydopamine-engineered barium titanate nanocomposite(BTO@PDA_(x)).By optimizing polydopamine(PDA)shell thickness,BTO@PDA_(0.5) exhibited superior excellent piezoelectric catalytic activity.Under ultrasound irradiation,PDA enhanced reactive oxygen species(ROS)generation by promoting charge carrier separation at the BTO interface,thereby accelerating chromogen degradation kinetics.Antibacterial assays and tooth whitening studies confirmed that BTO@PDA_(0.5) could effectively inhibit microorganisms and degrade pigments with extremely low cytotoxicity.This study designed a highly biocompatible organic-inorganic composite piezoelectric material,providing a new strategy for oral health care.展开更多
Conventional antibiotic treatment of bacterial infections associated with biofilms usually suffers from poor penetration and drug resistance.Ultrasound(US)-responsive antibacterial systems have shown great promise in ...Conventional antibiotic treatment of bacterial infections associated with biofilms usually suffers from poor penetration and drug resistance.Ultrasound(US)-responsive antibacterial systems have shown great promise in the elimination of bacterial biofilms,benefiting from their unique sonophysical and sonochemical effects.In this study,PFP@Lip-BNN6/Ce6 nanodroplets(PLBC NDs)were prepared by using perfluoropentane(PFP)to load chlorin e6(Ce6)and a nitric oxide(NO)precursor(BNN6)for treating Staphylococcus aureus(S.aureus)implant infection.PLBC NDs physically disrupt the biofilm structure by US-triggered PFP phase transition and cavitation to enhance the permeation of Ce6 and BNN6.Under US irradiation,Ce6 generates various reactive oxygen species(ROS),such as singlet oxygen(1O2)and superoxide anion(O_(2)^(•-));BNN6 releases NO and then reacts with O_(2)^(•-)to form peroxynitrite anion(ONOO^(-)),one of the long-lived reactive nitrogen species(RNS),thus realizing synergistic ROS/RNS antibacterial activity.In vitro experiments showed that PLBC NDs reduced the biofilm biomass of S.aureus in 96-well plates by 65.9%,with a bacterial inactivation rate of 4.4 log(99.995%),significantly surpassing single treatments.Transcriptomic analysis indicated that PLBC NDs can interfere with key pathways of S.aureus biosynthesis,metabolism,and oxidative stress.In a mouse titanium implant infection model,PLBC NDs reduced the number of viable bacteria in infected tissues by 3.5 log(99.97%)and promoted macrophage polarization towards an antiinflammatory phenotype(M2).Toxicity assessments demonstrated the favorable safety profile of PLBC NDs.This study presents a multifunctional US-responsive nanoplatform integrating sonophysical disruption and sonochemical killing for effective biofilm infection treatment.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22172093 and 21776167)the Natural Science Foundation of Shandong Province,China(No.ZR2023MB061).
文摘To solve the slow dynamics of catalytic oxygen reaction energy devices,a facile method was developed for the synthesis of methylene alcohol terminated poly(1,4-phenyldiimine)porphyrin cobalt(MPImPorCo),which was synthesized by RuCl3 catalyzed redox reaction of meso-5,10,15,20-tetra(4-nitrophenyl)porphyrin cobalt(TNO2PorCo)and 1,4-phenyldimethanol.M-PImPorCo is a fully conjugated covalent organic framework(COF)with high thermal and chemical stability.COFs with different edge groups were synthesized to compare the effect of different groups(–CH_(2)–OH and–NO_(2))on catalytic bifunctional oxygen reaction activity.C=N as nitrogen-rich environment of M-PImPorCo leads to the protonation process of oxygen catalysis and reduces the energy barrier of adsorption in the oxygen intermediate.C=N and–CH_(2)–OH form an“electron pump”structure to deliver electrons to the Co–N4 site in M-PImPorCo,and theπ–πinteraction between M-PImPorCo and three-dimensional graphene(3D-G)can further enrich the electron cloud density of Co–N4 sites.M-PImPorCo/3D-G has remarkable oxygen catalytic performance,with a half-wave potential(E_(1/2))of 0.91 V vs.reversible hydrogen electrode(RHE).M-PImPorCo/3D-G has low potential(Ej=10 is 1.49 V vs.RHE)at a current density of 10 mA·cm^(-2).It exhibits a good bifunctional catalytic performance(potential difference(ΔE)=0.58 V).The smaller charge–discharge band gap of zinc-air batteries(ZABs)and flexible ZABs(F-ZABs)equipped with M-PImPorCo/3D-G suggests the potential for catalytic oxygen reaction bifunctional applications.This work provides a new idea for the synthesis of Schiff-base porphyrin-based COF catalyst and its potential application to oxygen reaction catalytic energy storage devices.
文摘With the popularization of fifth-generation(5G)technology,even the next generation-6G and portable electronic products,electromagnetic wave pollution poses a serious threat to human physical and mental health and the normal operation of devices.The rapid development of display screens,medical equipment,and aerospace equipment has led to a surge in demand for highperformance transparent electromagnetic shielding materials to reduce electromagnetic interference(EMI)while ensuring optical clarity.This review systematically examines the latest developments in transparent EMI shielding materials,with a focus on their mechanisms,key material categories,and strategies for balancing shielding effectiveness(SE)and transmittance.The shielding mechanism(reflection,absorption,and multiple reflections)was analyzed through transmission line theory.This work reviews transparent EMI shielding materials based on transparent conductive oxides(TCOs),metal networks(MNs),carbonbased materials(CBMs),MXene,and other materials(OMs).The future development prospects and challenges of transparent EMI shielding materials were discussed.The review aims to promote the development of next-generation materials with high EMI shielding,optical transparency,and adaptability to complex environments.
基金supported by the National Key R&D Program of China(No.2022YFB2404402)the National Natural Science Foundation of China(Nos.22025507,22421001,and 22409200)the Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202010).
文摘The construction of metal phosphate coating layers has been widely recognized as an effective strategy for protecting high-energy cathode materials in lithium-ion batteries(LIBs).However,due to the low solubility of metal phosphates,their precipitation in aqueous solution becomes too fast to control,making it a significant challenge to ensure a heterogeneous growth process towards surface coatings.Herein,we report a solution-based synthetic process to achieve conformal metal phosphate coating through coordination-assisted precipitation,which involved the reaction between phytic acid(PA),urea,and metal ions,particularly Nb^(5+),in ethanol solution to achieve a well-tamed coating effect.The use of PA,a plant-derived compound known as inositol hexaphosphoric acid,was facile to form soluble phytate-metal complex,which precipitated with urea to form metal-phosphate-containing coatings with thickness controlled at high precision.This proposed synthetic protocol was applied for the surface coating of high-voltage cathode materials in the form of LiNi_(0.5)Mn_(1.5)O_(4)(LNMO),leading to significantly enhanced structural and electrochemical stability for its working at 5 V.Notably,after 300 cycles,the modified LNMO was able to achieve capacity retention of 85.1%for its working at 45℃ at a current density of 1 C as compared to only 29.9%of the pristine sample.Our findings highlight the potential of solution-based processes in building conformal coatings for the stabilization of high-energy cathode materials in their LIBs application.
基金supports by the Guangxi Science and Technology Base and Talent Special Project(No.AD25069020)Major project of scientific research in colleges and universities of Anhui Province(No.2024AH040211)+3 种基金Department of Education team project(No.2022AH010096)Anhui Province key research and development program(Nos.202423i08050016 and 202304a05020027)the National Natural Science Foundation of China(No.52472190)Beijing Nova Program(Nos.20220484036 and 20240484565).
文摘Triboelectric nanogenerators(TENGs)represent a promising technology for next generation human–computer interaction.The effective enhancement of induced charges are critical factors that determine the recognition accuracy of TENGbased tactile sensors.Here,we propose a magnetic fieldassisted TENG device utilizing waveform feature enrichment strategies to significantly enhance the tactile recognition accuracy in natural environments.An elastic micro-nano structure was fabricated on a polydimethylsiloxane(PDMS)film via a facile templating method.Leveraging the inherent hydrophobicity and microscale surface roughness of PDMS,our device demonstrates stable and distinct waveform characteristics under natural operating conditions.Importantly,the introduction of a magnetic field generates a Lorentz force,which effectively modulates induced charges within the electrode,yet minimally affects triboelectric charges at the PDMS interface.This selective modulation induces an asymmetric charge distribution inside the electrode,substantially increasing the induced charge density,consequently,subtle waveform features are markedly enhanced.These enriched signal features play a crucial role in elevating material recognition accuracy.As a result,the sensor achieves a remarkable recognition accuracy of 99%when distinguishing among ten different materials under magnetic field assistance.This work provides valuable guidelines for advancing the performance and accuracy of TENG-based tactile sensing systems.
基金supported by the National Natural Science Foundation of China(Nos.62404060 and 12464021)Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems(No.2023B1212010003)+3 种基金Construction of Key Technology Innovation Talent Team for Micro-Nano Information Devices and Integrated Circuits in Guizhou Province(No.BQW[2024]014)Functional Materials and Devices Technology Innovation Team of Guizhou Province University(No:Qian Jiaoji[2023]058)Guizhou Provincial Scientists Workstation of Photovoltaic Materials and Devices(No.KXJZ[2024]031)supported by Guizhou Provincial Science and Technology Foundation-ZK[2024]Youth 353 and MS-zk[2025]265,Funding for Doctoral Research Initiation Project in Natural Sciences at Guizhou Normal University(No.GZNUD[2024]02).
文摘Anisotropic two-dimensional(2D)semiconductors have emerged as promising candidates for polarization-resolved photodetection due to their intrinsic in-plane optical anisotropies and linear dichroisms.However,their practical applications are often constrained by limited spectral response and low anisotropy ratios.In this work,we report a broadband polarization-sensitive photodetector based on a type-II p-GaTe/n-PdSe_(2) van der Waals heterostructure,where interfacial band engineering—through the combined effect of the builtin p–n junction field and Schottky barrier—enables efficient carrier separation and unconventional reverse rectification.The device exhibits a high reverse rectification ratio(>10^(2))and an ultra-low forward dark current(~10^(-11) A).Owing to the engineered band alignment,it achieves broadband photodetection from 365 to 940 nm,with a high photoswitching ratio(>10^(3)),responsivity(~10^(3) A/W),detectivity(~10^(13) Jones),and external quantum efficiency(~10^(4)%).Furthermore,strong polarization sensitivity is demonstrated,with polarization ratios of 5.39,4.71,and 4.60 at the wavelengths of 365,520,and 940 nm,respectively,highlighting the potential of this heterostructure for high-performance and polarization-resolved optoelectronic applications.
基金supported by the National Natural Science Foundation of China(No.52103240)the Science and Technology Department of Henan Province(No.242301420056).
文摘Fabricating organic solar cells(OSCs)in open-air and room-temperature environments is essential for cost-effective roll-to-roll printing,but its performance is limited by non-ideal block and surface morphology of active layer.Herein,we demonstrate a record power conversion efficiency(PCE)of 19.72%in open-air and as-cast processed devices by using a lowcost terpolymer donor(PTQ20-5)to optimize the block and surface morphology.Compared with the counterpart PTQ10,PTQ20-5 shows increased hydrophobicity,which can better prevent the intrusion of H2O molecules in the film formation process in open-air environment,giving excellent humidity tolerance of corresponding devices.Moreover,the enhanced dielectric constant results in reduced exciton binding energy and improved charge transport of PTQ20-5,leading to improved charge separation and transfer,and suppressed carrier recombination in the devices.Besides,the PTQ20-5-based film has more appropriate block morphological features of balanced molecular self-assembly and phase separation,which simultaneously promotes the charge carrier transport and inhibits the carrier recombination at the donor/acceptor interface.This work is of great significance for promoting the industrialization of OSCs.
基金supported by the National Natural Science Foundation of China(Nos.62474011 and 62204006)Shenzhen Science and Technology Program(No.RCBS20231211090701006)+2 种基金Development and Reform Commission of Shenzhen Municipality(No.XMHT20220106002)Guangdong Key Laboratory of Flexible Optoelectronic Materials and Devices,Guangdong International Science Collaboration Base(No.2019A050505003)Shenzhen Key Laboratory of Organic Opto-electromagnetic Functional Materials of Shenzhen Science and Technology Plan(No.ZDSYS20140509094114164).
文摘Organic light-emitting transistors(OLETs)are gaining increasing attention as a promising candidate for nextgeneration display technology.However,due to the limited horizontal charge transport capability in OLETs,enhancing their optical performance remains greatly challenging.In this work,an effective strategy is employed to achieve highperformance OLETs by constructing a two-dimensional molecular-scale passivation layer at the dielectric/channel interface using a promising solution-processed small-molecule material,tetratetracontane(TTC).By controlling the microscopic flows driven by intermolecular interactions near the solution meniscus,molecular self-assembly dynamics are effectively regulated,contributing to a significant transformation in molecular layer stacking mode and enabling the formation of large-area TTC thin films with two-dimensional molecular-scale surface structure and uniform morphology.The introduction of high-quality TTC passivation layer film into the dielectric/channel interface optimizes the film morphologies of overlying channel layer,effectively shields the electrostatic dipole effects at dielectric/channel interface,leading to the synergistic optoelectronic regulation and enhanced optical properties of OLETs.Consequently,high brightness of 10,077.3 cd·m^(-2),high external quantum efficiency(EQE)of 20.46%,and low voltage of 15 V are achieved in the lateral OLET.This work presents a promising approach for two-dimensional molecular-scale small molecule interfaces,and provides an effective strategy for achieving high-performance OLET devices.
基金supported by Science and Technology Department Science and Technology Development Plan Project in Jilin Province(No.YDZJ202301ZYTS425 to L.B.)the National Natural Science Foundation of China(No.22225203 to K.L.and No.82303732 to L.B.)+2 种基金Program for Outstanding Young and Middle-Aged Talents in Jilin Province’s Medical and Health Workforce Development(No.JLSWSRCZX2025-109 to L.B.)Talent Reserve Program(TRP)at the First Hospital of Jilin University(No.JDYYCB-2023003 to L.B.)Tumor Immunotherapy Academic Special Zone Cultivation Project of the First Hospital of Jilin University.The animal study protocol was approved by the Institutional Animal Care and Use Committee at The First Hospital of Jilin University,China(No.2022-0647).
文摘Second window near-infrared(NIR-II)light is preferred for photothermal therapy due to its deeper tissue penetration,reduced scattering,and improved imaging guidance compared to NIR(I)light.However,NIR-II–absorbing gold nanomaterials with low cytotoxicity,well-defined structural stability,controllable size,and excellent dispersibility have been rarely reported.Compared with nanospheres and nanorods,gold nanostars have lower cytotoxicity,lower oxidative stress damage,higher intracellular enrichment in tumor cells,and maintain their labeling activity after circulation in vivo.Here,we reported a well-defined and easily synthesized gold nanotetrapods(AuNTPs)material absorbing NIR(II).This material not only meets the requirements for localized tumor hyperthermia but also reprograms the tumor microenvironment by enhancing tumor cell antigen presentation,converting"cold"tumors into"hot"tumors.Additionally,AuNTPs-based photothermal therapy induced by NIR-II irradiation enhances the antitumor functions of dendritic cells,T cells,and NK cells in the systemic immune response,inducing a sustained antitumor immune effect.The tumor microenvironment modulation properties exhibited by these AuNTPs may provide new avenues for exploring precise,non-invasive optical modulation nano anti-cancer therapy platforms within the NIR(II)window.
基金the National Natural Science Foundation of China(Nos.52473152,and 52273154)the Key Project of Natural Science Foundation of Zhejiang Province(No.LZ23B040002)is gratefully acknowledged.
文摘Gemcitabine(Gem)is the gold-standard chemotherapeutic drug for pancreatic cancer therapy in clinic.However,intratumoral bacteria can metabolize Gem into an inactive form,leading to Gem resistance.To address this challenge,Zn^(2+)-containing nanoparticles(ZGP NPs)are used to eliminate intracellular bacteria to enhance the therapeutic efficacy of Gem in pancreatic therapy.ZGP NPs are prepared via a facile one-pot method using Zn2+,epigallocatechin gallate(EGCG),and polyethylene glycol(PEG),which prevents metal ion chelation by proteins and ensures antibacterial activity.Leveraging the pH-responsive disassembly of metal-phenolic networks,ZGP NPs can be degraded in acidic lysosomes after cellular uptake,releasing Zn^(2+)to eliminate intracellular bacteria and thereby protecting Gem from bacteria-mediated inactivation.Moreover,the elimination of intratumoral bacteria enhances immunotherapy.The delivery of Zn^(2+)via ZGP NPs presents a promising strategy to eliminate intratumoral bacteria to overcome Gem resistance in pancreatic cancer therapy.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(No.KLZ25H280004 to X.Z.M.).
文摘Metabolic-associated fatty liver disease(MAFLD),a global health burden with limited therapeutic options beyond lifestyle changes,urgently needs novel strategies.We engineered exosome-like nanovesicles(HNVs)from dried honeysuckle(Lonicera japonica),exhibiting significantly more uniform size distribution than conventional herbal extracts and characteristic nanovesicle morphology.Orally delivered HNVs,enriched with bioactive metabolites,dramatically inhibited increased fat vacuoles,lipid droplet deposition,and collagen fibrosis in the livers of mice with MAFLD induced by high-fat diet(HFD).Mechanistically,HNVs orchestrate a dual gut-liver intervention:(1)restoring gut barrier integrity,slashing serum LPS by 1.58-fold and quelling hepatic inflammation;(2)remodeling gut microbiota to suppress bile salt hydrolase(BSH),elevating taurochenodeoxycholic acid(TCDCA)2.07-fold.This microbial shift reprograms enterohepatic signaling by inhibiting the FXR-FGF15-FGFR4 axis,thereby boosting hepatic cholesterol catabolism via bile acid synthases.Critically,efficacy is strictly microbiotadependent:abolished by antibiotics and fully transferable via fecal microbiota transplantation(FMT)from HNV-treated donors.Presenting the first natural nanovesicle platform that concurrently targets gut barrier repair and metabolic reprogramming,HNVs establish a pioneering,multi-targeted therapeutic paradigm for MAFLD,directly linking gut microbial ecology to hepatic pathophysiology with high translational potential.
基金supported by the National Natural Science Foundation of China(Nos.22309023,52301011,and 52231008)the China Postdoctoral Science Foundation(No.2022M720593)+2 种基金the project of Natural Science Foundation of Chongqing(No.CSTB2022NSCQ-MSX0270)the youth project of science and technology research program of Chongqing Municipal Education Commission of China(No.KJQN202501114)the special funding for research projects of Chongqing Human Resources and Social Security Bureau(No.2022CQBSHTB1023).
文摘Supported single-atom catalysts(SACs)demonstrate exceptional catalytic performance,atom efficiency,and selectivity,as a result,they are the potential candidates used in oxygen evolution reaction(OER).However,stabilizing monodispersed noblemetal atoms is challenging.This is especially true for two-dimensional(2D)layered double hydroxide(LDH)nanostructures.Here,we report the successful stabilization of ruthenium(Ru)single atoms(SAs).These SAs are located within a defective NiFe LDH nanosheet grown on the nickel foam(NF).This material is named Ru SAs/D-NiFe LDH@NF and formed through the*OOH hydrothermal reaction followed by etching.The resulting catalyst exhibits outstanding OER performance in alkaline media,achieving an exceedingly low overpotential(206 mV)at 50 mA·cm^(-2),which remarkably decreases relative to the overpotential in pristine NiFe LDH(311 mV).Ru SAs regulate the electron distribution near defects,optimizing the Ru-NiFe hydroxide interaction and diminishing energy barrier for forming intermediates,as revealed by density functional theory(DFT)calculations.Moreover,the catalyst demonstrates remarkable stability in Zn-air batteries(ZABs),delivering the maximal power density(170 mW·cm^(-2)).Furthermore,it maintains stable operation for 350 h,highlighting its practical viability.This work provides a versatile strategy for integrating single-atom sites into NiFe LDH,paving the way for the design of next-generation SACs for energy conversion applications.
基金supported by the National Natural Science Foundation of China(No.22278097)the Postdoctoral fellowship of Heilongjiang Province(No.LBH-Z23156)+3 种基金the Postdoctoral Fellowship Program of CPSF(No.GZC20233449)the Shandong Provincial Natural Science Foundation(No.ZR2024QB383)the Natural Science Foundation of Jiangsu Province(No.BK20230635)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.23KJB150002).
文摘Appropriate non-metallic element doping is promising to improve the intrinsic electrocatalytic oxygen reduction reaction(ORR)performance of nitrogen-doped carbon candidates,yet challenges still remain to rationally design of the catalyst configuration with kinetically favorable state.Herein,we propose the metalloid element to regulate the local electronic environment,and a novel metal-free electrocatalyst,namely,atomically dispersed Te-N_(2) on nitrogen-doped carbon frameworks was developed.Characterization and theoretical analyses demonstrate that the heteroatoms tellurium integrated with nitrogen-doped carbon substrate forms a Te-N covalent coordination as the active center that empowers both improved ORR kinetics and structural stability.As expected,the optimized composite of Te-N-C 900 delivers considerable electrocatalytic ORR activity in alkaline media(E_(1/2)=0.871 V,0.1 M KOH),along with encouraging durability(over 10,000 cycles with 13 mV decay),which is also responsible for Zn-air batteries operating with high uplifting peak power density and long lifespan.As a proof-of-concept,this work elucidates the key influence of heteroatom interaction of metalloid element,achieves the synthesis of Te-N_(2) metal-free ORR catalysts,and provides guidance for the development of high-performance metal-free ORR catalysts.
基金supported by the National Natural Science Foundation of China(No.22374159)the Youth Innovation Promotion Association CAS(No.2021420).
文摘Uranium extraction from seawater(UES)is crucial for reducing nuclear fuel supply pressure and promoting the comprehensive utilization of marine resources.The successful implementations of UES engineering critically rely on the highly efficient sorbent materials with exceptional performance in binding uranyl ions.Herein,a universal and facile“organic ion building blocks self-assembly”strategy is established to realize a first class of carboxyl functionalized ionic single crystals,named BPTC-BPY-R(R=1–6,the R corresponds to alkyl chain length modifier,e.g.,R=1 corresponds to iodomethane derivatives,R=2 corresponds to bromoethane derivatives,etc.),derived from rationally designed viologen-derivatives with different alkyl chain lengths and polycarboxylic acid.This strategy effectively exploits the organic ion building block properties to achieve U(VI)adsorption based on the synergistic effects of anions(ligand interaction)and cations(electrostatic interaction).Notably,attributed to the special crystal stacking mode and higher specific surface area,the resulting BPTC-BPY-3 not only achieves ultrahigh selectivity for U(VI)adsorption with a partition coefficient of 3.998×10^(6) mL/g,but also possesses an ultrafast U(VI)adsorption kinetics and an uptake capacity of 686.8 mg/g within 2 min.More importantly,it realizes a U(VI)uptake capacity of 7.41 mg/g from natural seawater in 20 days.The designed material with ultra-selectivity,high capacity,ultrafast kinetics,and good recyclability exhibits a great promise for efficient U(VI)extraction from seawater.
基金supported by the National Natural Science Foundation of China(No.52173070).
文摘Electromagnetic pollution is becoming significantly serious.Therefore,it is critical to prepare the advanced electromagnetic interference(EMI)shielding materials with thinness,flexibility and high mechanical strength.Herein,the copperbased metal-organic framework(MOF-Cu)and polyethyleneiminemodified ammonium polyphosphate(PEI-APP)were successfully synthesized.The flame-retardant thermoplastic polyurethane(TPU)composite was successfully prepared by compounding MOF-Cu and PEI-APP.The Cotton@PDA@MXene composite was fabricated via a sequential loading process of polydopamine(PDA)and MXene onto cotton fabric.Then,the multilayer TPU composites were prepared by layer-by-layer hot-pressing.The TPU/9PAPP/1MOF/C-3PM composite exhibited exceptional EMI effectiveness of 20.5 dB in X-band and 23.0 dB in K-band,exceeding commercial standards.The TPU/9P-APP/1MOF/C-3PM composite also demonstrated significantly enhanced flame retardancy.Compared with pure TPU/Cotton sample,the peak heat release rate,total heat release and total smoke release of TPU/9PAPP/1MOF/C-3PM composite decreased by 40.7%,31.1%,and 33.3%,respectively.Furthermore,the thickness of the multilayer TPU composites was only 1 mm,demonstrating excellent flexibility.As the outer encapsulation material,TPU endowed the multilayer TPU composites outstanding durability and effectively addressed the common issues of fabric abrasion and conductive filler detachment.This study provides a novel strategy for preparing flexible electromagnetic interference shielding materials with superior flame retardancy.
基金supported by the National Key Research and Development Program of China(No.2022YFC2106100)the National Natural Science Foundation of China(No.22078265).
文摘To address postoperative melanoma issues of high recurrence and poor wound healing,we developed a nanocomposite hydrogel wound patch(M_(xNd/yCe)@M SAC)for cascade sequential therapy.Methotrexate(MTX)loaded Nd/Ce-doped mesoporous bioactive glass was encapsulated in a sulfobetaine-polyacrylamide-carboxymethyl chitosan hydrogel via thermal polymerization.Under the acidic microenvironment of the residual tumor,the amide bonds in M_(xNd/yCe)@M SAC are broken,releasing M_(xNd/yCe)@M.M_(xNd/yCe)@M targets tumor cells,and the combined therapy of mild photothermal treatment and chemotherapy ablates tumor cells.Subsequently,the continuously released MTX downregulates the expression of pro-inflammatory factors and reshapes the immune microenvironment.Finally,M_(xNd/yCe)@M disintegrates,releasing Si^(4+),Ca^(2+),P^(5+)and Ce^(3+)ions,which can effectively promote angiogenesis and tissue repair.In the postoperative melanoma model,this method effectively cleared the residual tumors after surgery,shortened the inflammatory period,and promoted tissue regeneration.In conclusion,the nanocomposite hydrogel wound patch for cascade sequential treatment prepared in this study has excellent anti-tumor,immune regulation and tissue repair properties,providing prospective insights for the postoperative treatment of malignant melanoma.
基金funded by the Zhejiang Provincial Natural Science Foundation of China(No.LD22H310004)the National Natural Science Foundation of China(No.82473894)Zhejiang Sci-Tech University Research Start-up Fund(No.24042190-Y).
文摘The rising global burden of cancer necessitates innovative therapeutic strategies,with immunotherapy demonstrating remarkable potential.However,its clinical efficacy remains limited by low response rates and non-specific(off-target)delivery.This review highlights natural polymer-based hydrogels as emerging delivery platforms engineered to enhance the efficacy of cancer immunotherapy.These hydrogels exploit the biocompatibility and biodegradability of natural polymers,employing chemical or physical crosslinking to encapsulate and deliver immunotherapeutic agents.The versatility of these hydrogels is discussed in the context of oral,sprayable,injectable,and implantable formulations,which are adaptable to specific tumor sites.Their responsiveness to stimuli such as pH,temperature,and enzymatic activity enables controlled and sustained release of immunotherapeutic agents,including checkpoint inhibitors,cytokines,and Toll-like receptor agonists.These hydrogels can also modulate the tumor microenvironment by regulating pH,oxygen levels,and immune cell infiltration,thereby enhancing therapeutic efficacy.Moreover,immunotherapeutic hydrogels can act synergistically with chemotherapy,radiotherapy,and phototherapies to enhance antitumor immune responses.Despite their potential,challenges such as degradation kinetics,bioactivity retention,and regulatory hurdles must be addressed to ensure successful clinical translation.This review provides insights into the rational design,development and application of stimuli-responsive hydrogels as next-generation platforms for effective cancer immunotherapy.
基金supported by the National Key Technologies R&D Program of China(Nos.2018YFA0209301 and 2018YFA0209303)the National Natural Science Foundation of China(Nos.22272027,U21A20326,U1905214,21425309,21761132002,21961142019,and 21861130353)+1 种基金the Chang Jiang Scholars Program of China(No.T2016147)the 111 Project(No.D16008).
文摘Rational design of electrochemical sulfide oxidation reaction(SOR)catalysts is a prerequisite to fully recycling hydrogen(H_(2))and elemental sulfur(S0)resources,realizing the bridge between environment and energy fields,as well as enlightening the optimization of metal‒sulfur battery applications.While transition metal catalysts often suffer from sulfur poisoning,single-atom catalysts(SACs)offer a promising solution,where the precise coordination environment of metal centers becomes a critical determinant of catalytic performance.Herein,for the first time,we develop a Ni single-atom catalyst for SOR with unique Ni-N_(3)O_(1) coordination anchored on hierarchically porous carbon(Ni1@HPC),which demonstrates remarkable advantages over conventional Ni-N_(4) or Ni-O4 configurations,exhibiting a superior SOR activity(0.37 V vs.RHE at 100 mA·cm^(-2))that surpasses reported carbon-based catalysts and is comparable to most metal-based catalysts.In situ Raman and density functional theory(DFT)results reveal that the HPC facilitates rapid product S0 desorption while the Ni-N3O1 coordination enables appropriate reactant sulfide(S^(2-))adsorption,striking a critical balance between activity and stability that other coordination geometries fail to achieve.Additionally,the practical application of coupling hydrogen evolution reaction(HER)and SOR is realized on Ni1@HPC with low power consumption,which is a promising alternative to the traditional overall water splitting(OWS)process.This work not only establishes a structure–activity relationship for single-atom catalysts in SOR but also provides a general strategy for optimizing metal coordination in electrocatalytic systems.
基金supported by the National Natural Science Foundation of China(No.22179095)the Graduate Scientific Research Foundation of Jianghan University(No.KYCXJJ202423).
文摘Metal-bio-oxygen batteries establish a paradigmshifting energy architecture for biomedical implants,endowing these devices with extended service life in continuous physiological surveillance and precision theranostic operations.However,the conventional electrolytes in these semi-opened batteries fail to meet the requirements in biocompatibility and bio-safety for in vivo applications.Herein,we report a bio-compatible composite gel electrolyte for implanted Zn-O_(2) battery(ZOB),while also sustainably powering a mechanical sensor in vivo.This electrolyte composes a poly(L-lactide-co-epsilon-caprolactone)(PLCL)framework with a gelatin methacryloyl(GelMA)modification layer,and the salt in body fluid serves as ion transport carriers in the electrolyte.It displays an O_(2) impermeable property and lower polarization potentials as electrolyte in Zn||Zn symmetric cell.In vitro assay results demonstrate that the battery components illustrate excellent biocompatibility with negligible cytotoxicity.In vivo histopathological and hematological analyses further verified the biosafety of ZOB during operation,while capillary regeneration around the cathode ensured adequate oxygen supply for sustained performance.The assembled ZOB delivers a power density of 1.96μW/cm^(2) at 0.98 V in vivo,which also successfully powers an integrated hydrogel mechanical sensor and monitors cardiac signals in rats.The unique two-electron transfer pathway of oxygen reduction in blood has also been elucidated.This work offers a new insight into bio-compatible electrolyte design for next-generation implantable power sources,enabling robust implantable devices for healthcare technologies.
基金supported by the National Key Research and Development Program of China(No.2022YFB3205602)the National Natural Science Foundation of China(Nos.52372174,and 32401198)+1 种基金Beijing Nova Programme Interdisciplinary Cooperation Project(No.20250484970)the Carbon Neutrality Research Institute Fund(No.CNIF20230204).
文摘The delicate balance of oral microbiota is frequently disrupted by exogenous discoloration and biofilm formation,thus requiring integrated antibacterial and whitening strategies.Conventional peroxide treatments often damage the integrity of tooth enamel,while nanocatalysts pose cytotoxicity risks.In this work,we designed a biocompatible polydopamine-engineered barium titanate nanocomposite(BTO@PDA_(x)).By optimizing polydopamine(PDA)shell thickness,BTO@PDA_(0.5) exhibited superior excellent piezoelectric catalytic activity.Under ultrasound irradiation,PDA enhanced reactive oxygen species(ROS)generation by promoting charge carrier separation at the BTO interface,thereby accelerating chromogen degradation kinetics.Antibacterial assays and tooth whitening studies confirmed that BTO@PDA_(0.5) could effectively inhibit microorganisms and degrade pigments with extremely low cytotoxicity.This study designed a highly biocompatible organic-inorganic composite piezoelectric material,providing a new strategy for oral health care.
基金supported by the National Natural Science Foundation of China(Nos.22375101,and 62288102).
文摘Conventional antibiotic treatment of bacterial infections associated with biofilms usually suffers from poor penetration and drug resistance.Ultrasound(US)-responsive antibacterial systems have shown great promise in the elimination of bacterial biofilms,benefiting from their unique sonophysical and sonochemical effects.In this study,PFP@Lip-BNN6/Ce6 nanodroplets(PLBC NDs)were prepared by using perfluoropentane(PFP)to load chlorin e6(Ce6)and a nitric oxide(NO)precursor(BNN6)for treating Staphylococcus aureus(S.aureus)implant infection.PLBC NDs physically disrupt the biofilm structure by US-triggered PFP phase transition and cavitation to enhance the permeation of Ce6 and BNN6.Under US irradiation,Ce6 generates various reactive oxygen species(ROS),such as singlet oxygen(1O2)and superoxide anion(O_(2)^(•-));BNN6 releases NO and then reacts with O_(2)^(•-)to form peroxynitrite anion(ONOO^(-)),one of the long-lived reactive nitrogen species(RNS),thus realizing synergistic ROS/RNS antibacterial activity.In vitro experiments showed that PLBC NDs reduced the biofilm biomass of S.aureus in 96-well plates by 65.9%,with a bacterial inactivation rate of 4.4 log(99.995%),significantly surpassing single treatments.Transcriptomic analysis indicated that PLBC NDs can interfere with key pathways of S.aureus biosynthesis,metabolism,and oxidative stress.In a mouse titanium implant infection model,PLBC NDs reduced the number of viable bacteria in infected tissues by 3.5 log(99.97%)and promoted macrophage polarization towards an antiinflammatory phenotype(M2).Toxicity assessments demonstrated the favorable safety profile of PLBC NDs.This study presents a multifunctional US-responsive nanoplatform integrating sonophysical disruption and sonochemical killing for effective biofilm infection treatment.
