A novel[3]rotaxane,featuring two hydrogen-bonded aramide azo-macrocycles mechanically interlocked on a dumbbell with distinct recognition sites,a secondary dialkylammonium(AM)unit and a 4,4'-bipyridinium(BP)unit,h...A novel[3]rotaxane,featuring two hydrogen-bonded aramide azo-macrocycles mechanically interlocked on a dumbbell with distinct recognition sites,a secondary dialkylammonium(AM)unit and a 4,4'-bipyridinium(BP)unit,has been synthesized.This multi-stimuli-responsive[3]rotaxane exhibits unique molecular motion,with the macrocycles shuttling along the axle in response to acid-base reactions,temperature changes,solvent variations,and light irradiation.The molecular shuttle and reversibility were investigated by^(1)H NMR,2D NOESY,HRESI-MS,and UV-vis spectroscopy.This study provides a rare example of a higher order rotaxane with multi-stimuli responsiveness,highlighting its potential for multi-state control over the motion of interlocked rings on an axle.The ability to manipulate the molecular motion of the macrocycles through various external triggers offers insights for future developments in molecular machinery and adaptive materials.展开更多
A novel smart metal-organic gel(MOG) formed from biscarboxyl-functionalized benzimidazole derivative(D11) in the presence of lead nitrate has been investigated.The critical gel concentration for the formation of M...A novel smart metal-organic gel(MOG) formed from biscarboxyl-functionalized benzimidazole derivative(D11) in the presence of lead nitrate has been investigated.The critical gel concentration for the formation of MOG was just 0.36 wt%,which exhibits a super gelation capability of D11.The coordination of the metal to the ligand D11 was found to play a vital role in the construction of the supramolecular MOG.Microstructures determined by SEM observation demonstrated that the MOG was formed by intertwined fibrils.Interestingly,the MOG exhibits pH-induced,thermo-induced,and chemical-induced reversible gel-sol transition.Meanwhile,this supramolecular MOG shows desirable absorption ability of methyl orange dye molecules in aqueous solution.展开更多
Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches,memories,and molecular machines.The exploration of the material is currentl...Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches,memories,and molecular machines.The exploration of the material is currently focused on the pure organic system,which limits the development o such materials greatly.In this work,we present a new chiral organic-inorganic hybrid salt,(R-3hydroxypyrrolidinium)_(2)[Fe(CN)_(5)(NO)](1),which exhibits rare multi-stimuli responsive behaviors in ther mal,mechanical and optical channels.In detail,1 undergoes a C2-P2_(1)22_(1) phase transition deriving from the thermal motion of organic cations with the increase of temperature,but the reverse transition can only be induced by mechanical pressure.Moreover,polycrystalline hybrid salt showed photo-responsive performance,i.e.,the ground-state N-bound nitrosyl ligand adopts two configurations in excited state caused by light in 532 nm irradiation,accompanying with a photo-induced structural transformation o the anionic framework.Namely,the thermal motion characteristics of organic cations,the photoresponse characteristics of anionic inorganic skeleton and the pressure characteristics from hydrogen bonds are si multaneously integrated in 1.This unprecedented coupling mechanism of multi-stimuli responses make1 a potential candidate for future multichannel data storage applications.展开更多
Thin-film materials with flexibility and stretchability are essential for wearable smart technologies.However,achieving both superior mechanical properties and multi-stimuli responsiveness in ultrathin films remains a...Thin-film materials with flexibility and stretchability are essential for wearable smart technologies.However,achieving both superior mechanical properties and multi-stimuli responsiveness in ultrathin films remains a significant challenge.Herein,we report a novel class of multifunctional thin-film materials fabricated via dynamic covalent self-assembly of two key components:a renowned aggregation-induced emission(AIE)luminogen,tetraphenylethylene with four benzaldehyde groups(TTPE-CHO),serving as the emissive and rigid backbone,and hydrazide-functionalized polyethylene glycol(PEG 400 and PEG 600)chains,imparting flexibility.The resulting films exhibit green fluorescence,high flexibility,stretchability,anisotropic morphological features,and multiple stimuli-responsive properties—capabilities that are severely limited in the absence of PEG chains.Remarkably,even at an ultrathin thickness of only 4μm,the TTPE-DTH-400-G film achieves a record-breaking tensile stress of 47 MPa,demonstrating outstanding mechanical strength and elasticity.Furthermore,it enables reversible vapor-triggered actuation and exhibits exceptional fluorescence sensing performance for detecting the sarin analog diethyl chlorophosphate(DCP),with an ultralow detection limit of 1 ppt and a rapid response time.This study presents an effective strategy for integrating rigid and flexible components to construct functional thin films with superior mechanical properties and intelligent responsiveness,paving the way for advanced applications in wearable electronics and real-time hazardous substance detection.展开更多
Nanotechnology has provided thousands of novel nano-antimicrobials possessing features uncommon in clinically available antimicrobials.Here,nanocarriers loaded with conventional antimicrobials and responding to enviro...Nanotechnology has provided thousands of novel nano-antimicrobials possessing features uncommon in clinically available antimicrobials.Here,nanocarriers loaded with conventional antimicrobials and responding to environmental changes upon entry into oral biofilms are reviewed.Supra-gingival biofilms are characterized by acidic pH,the presence of bacterial enzymes,and the development of hypoxia in deeper layers.Sub-gingival biofilms are slightly alkaline,with hypoxia occurring over their entire depth.Upon entering biofilms,negatively charged,pH-and/or hypoxia-responsive nanocarriers become positively charged.This charge reversal leads to electrostatic double-layer attraction between positively charged nanocarriers towards negatively charged,waterfilled channel walls in biofilms,enhancing their accumulation in a biofilm.Degradation of bacterial enzyme-responsive nanocarriers causes in-biofilm release of antimicrobial cargo,yielding higher local antimicrobial concentrations than can be achieved through their direct,oral administration without harming soft tissues.Enhanced antibiofilm activity after in-biofilm antimicrobial release from biofilm-responsive micelles and liposomes has been demonstrated in vitro towards single-species Streptococcus mutans and Staphylococcus aureus biofilms or in vivo using specific-pathogen-free rodents inoculated with selected pathogens.This preferential antibacterial activity regulated the microbial composition of ex vivo human oral biofilm towards a more healthy microbiome composition.Although clinical confirmation is limited,the potential benefits of stimuli-responsive,antimicrobial-loaded nanocarriers for oral biofilm control and microbiome restoration are worth further investigation towards clinical translation.展开更多
Near-infrared(NIR)light-responsive shape memory polymers(SMPs)show great promise for biomedical applications,but conventional photothermal agents suffer from high cost,complex preparation,or poor biocompatibility,whil...Near-infrared(NIR)light-responsive shape memory polymers(SMPs)show great promise for biomedical applications,but conventional photothermal agents suffer from high cost,complex preparation,or poor biocompatibility,while lignin-based alternatives exhibit insufficient photothermal conversion efficiency.Herein,we developed a novel strategy to enhance photothermal performance of lignin through sequential demethylation modification and Fe^(3+)complexation for constructing NIR light responsive SMPs.Dealkaline lignin(DL)was first demethylated using iodocyclohexane to produce demethylated lignin(DDL)with increased catechol content,which was then incorporated into polycaprolactone-based polyurethane synthesis followed by Fe^(3+)complexation.Results showed that DDL-Fe^(3+)complexes have significantly enhanced photothermal conversion performance,and the resulting PU-DDL+Fe^(3+)polyurethane with 0.5 wt%DDL content demonstrated a temperature increases of 39.8℃under 0.33 W·cm-2808 nm NIR irradiation.This excellent photothermal performance enables the shape-fixed PU-DDL+Fe^(3+)polyurethane to rapidly recover to its initial shape under NIR light irradiation.Additionally,PU-DDL+Fe^(3+)polyurethane exhibits good mechanical properties and biocompatibility,demonstrating significant biomedical application potential.展开更多
Genomic destabilization and defective DNA repair are the most prominent features of tumour cells and are exploited by various chemotherapy drugs for cancer therapy.Long non-coding RNA(lncR-NAs)have emerged as powerful...Genomic destabilization and defective DNA repair are the most prominent features of tumour cells and are exploited by various chemotherapy drugs for cancer therapy.Long non-coding RNA(lncR-NAs)have emerged as powerful regulators of gene expression and are thus involved in diverse biological processes.Recent studies have demonstrated that several lncRNAs play critical roles in DNA repair.Nonetheless,the relationship between DNA damage-responsive lncRNAs and chemoresistance remains poorly defined.In this study,we established four different DNA damage models triggered by cisplatin(DDP),H2O2,neocarzinostatin(NCS)or ultraviolet(UV)irradiation and identified a specific upregu-lated lncRNA(lnc-DUSP6)involved in the cisplatin-induced DNA damage response.Furthermore,loss-or gain-of-function experiments confirmed that lnc-DUSP6 enhanced DNA repair and cell survival under cisplatin treatment,thus promoting cisplatin resistance.Mechanistically,an RNA immunoprecipitation(RIP)assay revealed that lnc-DUSP6 directly interacts with DUSP6(Dual Specificity Phosphatase 6),which is closely associated with cisplatin sensitivity.Additionally,overexpression of DUSP6 significantly rescued the effects of lnc-DUSP6 silencing on DNA repair and cell survival under cisplatin treatment.O-verall,our results show the effect and underlying mechanism of lnc-DUSP6 in cisplatin resistance:lnc-DUSP6 promotes cisplatin-induced DNA damage repair and cisplatin resistance by stabilizing DUSP6,which is highly clinically important for enhancing the efficacy of cisplatin for cancers.展开更多
Solvents in crystalline materials typically exist either as structural components that stabilize the framework or as adsorbed vips that modulate properties,yet achieving their orthogonal coexistence within a single ...Solvents in crystalline materials typically exist either as structural components that stabilize the framework or as adsorbed vips that modulate properties,yet achieving their orthogonal coexistence within a single system remains challenging.This study proposes a natural mineral-inspired solvent hierarchy strategy that enables the concurrent achievement of framework stability and dynamic responsiveness in hydrogen-bonded organic frameworks(HOFs)through the orthogonal integration of structural and adsorbed solvents.We have validated the feasibility of this solvent hierarchy approach based on four model systems with progressively increasing stability and dynamism:(1)unstable HOFs containing only adsorbed solvents,(2)unstable HOFs with low-binding-energy structural solvents,(3)stable HOFs incorporating strong-fitted structural solvents,and(4)stable HOFs with structural solvents and dynamically adjustable adsorption solvents.Crystallographic and theoretical analyses reveal that the superior stability of structural solvents originates from the high-electron-density oxygen of the DMSO S═O bond,which acts as a strong hydrogen-bond acceptor,forming stable N─H…O═S bonds with amine groups.The host’s aggregation-induced emission(AIE)characteristics allow real-time optical monitoring of reversible single-crystal-to-single-crystal transformations without compromising structural integrity,demonstrating promising applications for visual water content and water leakage detection.This work not only establishes a new paradigm in solvent engineering for developing smart crystalline materials but also expands the design possibilities for functional porous frameworks.展开更多
Hospital wastewater contains complex pollutants,including residual organic dyes and antibiotic-resistant pathogens,posing severe risks to ecosystems and human health.Conventional adsorbents,constrained by monopolar fu...Hospital wastewater contains complex pollutants,including residual organic dyes and antibiotic-resistant pathogens,posing severe risks to ecosystems and human health.Conventional adsorbents,constrained by monopolar functional groups and limited surface sites,fail to remove both pollutants simultaneously.Here,we report an intelligent responsive polyurethane microsphere adsorbent doped with diallyl dimethylammonium chloride modified carbon nanotubes,termed as PUCD microspheres.The PUCD integrates bipolar adsorption sites,tunable micrometer-scale pores,and a near-infrared(NIR)-triggered in situ capture mechanism within a single platform,which achieves up to 98.3%dye removal,maintains strong adsorption performance across a wide pH range and retains 83.3%efficiency for rhodamine B after five cycles.Notably,the PUCD employs a temperature-responsive phase transition:under NIR irradiation,the microspheres undergo shrinkage,reducing the pore size to generate a‘polymer trap',enabling in situ capture of bacteria with>99%efficiencies for both Staphylococcus aureus and Escherichia coli.By immobilizing live bacteria,the PUCD microspheres substantially reduces the risk of pathogen desorption and toxin release.This promising platform offers a safe,efficient,and single-stage strategy for hospital wastewater purification,enabling the simultaneous elimination of dyes and pathogenic bacteria.展开更多
Hepatic fibrosis is regulated by the synergistic actions of various cells and cytokines,with the activation and proliferation of hepatic stellate cells(HSCs) being considered the central event in this process.To achie...Hepatic fibrosis is regulated by the synergistic actions of various cells and cytokines,with the activation and proliferation of hepatic stellate cells(HSCs) being considered the central event in this process.To achieve specific targeting of activated hepatic stellate cells(a HSCs) and precise treatment of hepatic fibrosis,this study developed a dual-functional drug delivery system(SIL/c RGD-PEG-PPS PMs) with both targeting and responsive release capabilities.It aims to target the αvβ 3 receptor specifically expressed on the surface of a HSCs using the cyclic peptide c(RGDyk),and to exploit the high reactive oxygen species(ROS) level in the cellular microenvironment to achieve concentrated burst release of drugs at the pathological sites of hepatic fibrosis.Based on multiple assessments,SIL/c RGD-PEG-PPS PMs specifically enhanced the targeted delivery of silybin(SIL) to a HSCs,inhibited the proliferation and migration of a HSCs,and exhibited good biosafety.Additionally,it demonstrated excellent anti-fibrotic activity in fibrotic mice.In summary,this study shows great potential in targeted treatment of hepatic fibrosis and provides a multifunctional tool for advancing the research and therapeutic strategies of hepatic fibrosis.展开更多
Simultaneous integration of rich oxygen vacancies(OVs)and twin crystals in a photocatalyst can not only significantly enhance the near-infrared(NIR)light response but also greatly improve the photocharge separation an...Simultaneous integration of rich oxygen vacancies(OVs)and twin crystals in a photocatalyst can not only significantly enhance the near-infrared(NIR)light response but also greatly improve the photocharge separation and transfer efficiency owing to the induced high electrical conductivity and strong built-in electric field.However,thus far,there has been a lack of a model catalyst containing both twin crystals and OVs.Herein,we develop a simple wet chemical strategy for synthesizing of unprecedented NIR light-responsive OVs-rich Cu_(2)O black nanoparticles with high-density of twin crystals(denoted as black twinned Cu_(2)O).As expected,the black twinned Cu_(2)O exhibits higher visible-NIR and NIR light-driven photodegradation of tetracycline(TC)solution than the counterparts.Significantly,the mechanism insight into twin-dependent photocatalysis in NIR light-responsive Cu_(2)O black nanocrystals with rich OVs is uncovered in depth by density functional theory(DFT)calculations and a series of experimental evidence.Expectantly,this work would be beneficial for the scientific researchers currently focusing on the NIR light-responsive photocatalysis and twin engineering of photocatalysts.展开更多
Microneedle(MN)patches could be a promising treatment for diabetic foot ulcers that plague thousands of people worldwide.While reducing skin resistance or increasing driving force can accelerate the efficiency of tran...Microneedle(MN)patches could be a promising treatment for diabetic foot ulcers that plague thousands of people worldwide.While reducing skin resistance or increasing driving force can accelerate the efficiency of transdermal drug delivery with conventional MN patches,it can create toxic chemical residues or require the help of additional devices.Herein,a thermo-responsive microneedles patch(TMN)with high biocompatibility without additional equipment is proposed.The TMN consisted of a bilayer microneedles composed of sodium alginate(SA)-g-poly(N-isopropylacrylamide)layer(SA-g-PNIPAM)loaded with sucrose octasulfate sodium salt(SOS)and hyaluronic acid layer and a polycaprolactone/chitosan nanofiber membrane loading with tetracycline hydrochloride(TH)and SOS.PNIPAM accelerates drug release by extruding the drug through a volumetric phase transition in response to temperature changes,and TH and SOS promote wound healing by inhibiting bacterial growth and promoting vascular regeneration and epithelial formation.The results showed that the drug release of TMN was significantly faster,with the drug release rate of more than 80% in the 10th h,and the antibacterial rate of TMN could reach 800%.In addition,TMN had good biocompatibility and good healing effects in vivo,which may be helpful for the design of multifunctional dressings in the future.展开更多
A viologen-bearing Zn(Ⅱ) coordination polymer,[Zn(Bpybc)SO_(4)]·H_(2)O,has been successfully synthesized and structurally characterized.The title compound exhibits sunlight and UV-induced photochromism,thermosch...A viologen-bearing Zn(Ⅱ) coordination polymer,[Zn(Bpybc)SO_(4)]·H_(2)O,has been successfully synthesized and structurally characterized.The title compound exhibits sunlight and UV-induced photochromism,thermoschromism,and amine-selective chemochromism.展开更多
Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapi...Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapid,contactless,and environmentally benign operation,has emerged as a promising approach for precise liquid control.However,conventional magnetic strategies typically govern droplet movement on open surfaces,facing limitations such as restricted liquid volumes,uncertain flow paths,and inevitable evaporation,thereby constraining their broader practical applications.Recently,a variety of magneticdriven strategies have been developed to dynamically regulate liquids within enclosed spaces,especially through physicochemical mechanisms.These approaches provide efficient control over liquid behavior by leveraging magnetically induced chemical changes,structural deformations,and dragging motions,opening new opportunities for flexible and versatile fluid management.This review explores the design and mechanisms of magneto-responsive confined interfaces for the manipulation of nonmagnetic liquids,highlighting key advancements and potential applications including liquid valves,liquid mixing,liquid flow regulation,and liquid pumping.Finally,the existing challenges and future prospects in this field are presented.展开更多
The tumor microenvironment(TME)-activatable probes have proven effective in enhancing the signalto-background ratio(SBR)for precise fluorescence imaging in tumor diagnosis.However,many fluorophores have suboptimal emi...The tumor microenvironment(TME)-activatable probes have proven effective in enhancing the signalto-background ratio(SBR)for precise fluorescence imaging in tumor diagnosis.However,many fluorophores have suboptimal emission spectra and a short Stokes shift,which may lead to overlap with bioautofluorescence,excitation,and emission spectra,limiting their use in intraoperative guidance.Herein,aγ-glutathione(GSH)responsive near-infrared(NIR)BODIPY probe,named“Pro-Dye”was synthesized with a large Stokes shift of 91 nm.The Pro-Dye can be rapidly and specifically activated by high concentrations of GSH both in solution and inside cancer cells,while remaining inactive in normal cells(Human umbilical vein endothelial cells,HUVECs).The Pro-Dye was further encapsulated by 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-(polyethylene glycol)-5000(DSPE-PEG5000)to form Pro-Dye nanoparticles(NPs),making it water-dispersible for in vivo application.In vivo fluorescence imaging demonstrated that Pro-Dye NPs can accumulate at the tumor and exhibit an improved SBR compared to the“alwayson”probe(Dye NPs).Moreover,the tumor can be precisely resected under the real-time guidance of fluorescence imaging of Pro-Dye NPs,showing a well-defined tumor margin.展开更多
Rapid and ultrasensitive detection of pathogen-associated biomarkers is vital for the early diagnosis and therapy of bacterial infections.Herein,we developed a close-packed and ordered Au@AgPt array coupled with a cas...Rapid and ultrasensitive detection of pathogen-associated biomarkers is vital for the early diagnosis and therapy of bacterial infections.Herein,we developed a close-packed and ordered Au@AgPt array coupled with a cascade triggering strategy for surface-enhanced Raman scattering(SERS)and colorimetric identification of the Staphylococcus aureus biomarker micrococcal nuclease(MNase)in serum samples.The trimetallic Au@AgPt nanozymes can catalyze the oxidation of 3,3’,5,5’-tetramethylbenzidine(TMB)molecules to SERS-enhanced oxidized TMB(oxTMB),accompanied by the color change from colorless to blue.In the presence of S.aureus,the secreted MNase preferentially cut the nucleobase AT-rich regions of DNA sequences on magnetic beads(MBs)to release alkaline phosphatase(ALP),which subsequently mediated the oxTMB reduction for inducing the colorimetric/SERS signal fade away.Using this“on-to-off”triggering strategy,the target S.aureus can be recorded in a wide linear range with a limit of detection of 38 CFU/mL in the colorimetric mode and 6 CFU/mL in the SERS mode.Meanwhile,the MNase-mediated strategy characterized by high specificity and sensitivity successfully discriminated between patients with sepsis(n=7)and healthy participants(n=3),as well as monitored the prognostic progression of the disease(n=2).Overall,benefiting from highly active and dense“hot spot”substrate,MNase-mediated cascade response strategy,and colorimetric/SERS dual-signal output,this methodology will offer a promising avenue for the early diagnosis of S.aureus infection.展开更多
Strong polyelectrolyte brushes(SPBs)play an important role in enabling material surface functionalization due to their unique stimuli-responsive properties.Although the unexpected pH responsiveness of SPBs has been re...Strong polyelectrolyte brushes(SPBs)play an important role in enabling material surface functionalization due to their unique stimuli-responsive properties.Although the unexpected pH responsiveness of SPBs has been revealed in the past ten years,it is still unclear if the pH-responsive properties of SPBs are affected by the brush thickness.In this study,we employed the positively charged poly[2-(methacryloyloxy)ethyl]trimethylammonium chloride(PMETAC)and negatively charged sodium poly(styrenesulfonate)(NaPSS)brushes as model systems to explore the effect of thickness on the pH-responsive properties of SPBs.The results demonstrate that the pH-responsive properties of SPBs manifest different dependences on the brush thickness.Specifically,for both PMETAC and NaPSS brushes,the pH-responsive hydration and stiffness are influenced by the thickness,and the pH-responsive wettability and adhesion are almost unaffected by the thickness.This work not only provides a clear understanding of the relationship between the brush thickness and the pH responsiveness of SPBs,but also offers a new method to control the pH-responsive properties of SPBs.展开更多
Superhydrophobic/superhydrophilic antifouling materials are widely used to solve the severe water pollution and bio-adhesion of marine equipment.However,conventional antifouling materials rely on the static superwetta...Superhydrophobic/superhydrophilic antifouling materials are widely used to solve the severe water pollution and bio-adhesion of marine equipment.However,conventional antifouling materials rely on the static superwettability of surfaces,which suffer from poorly sustained antifouling effects.Inspired by the unique dynamic antifouling strategies of Calliphora Vicina wing surface based on the hydrophobic micro-cilia arrays,a Biomimetic Magnetic-Responsive Antifouling Surface(BMRAS)is designed and fabricated using a method combining UV lithography and an inverse molding.The BMRAS is coated by high-aspect-ratio micro-cilia,which are filled with synthesized magnetic Fe3O4 nanoparticles.The bioinspired hydrophobic micro-cilia arrays endow the BMRAS with excellent intrinsic superhydrophobicity,benefiting from the high-aspect-ratio feature and roughness effect.Remarkably,the static contact angle is more than 156.9±1.6°and the rolling angle is less than 2.3±0.3°.The synthesized magnetic nanomaterials play a key role in implementing dynamic antifouling strategies.On the one hand,the surface tension can be adjusted as required under magnetically controlled oscillations.On the other hand,the doping of magnetic nanomaterials can enhance mechanical properties and reduce capillary force-induced aggregation of high-aspect-ratio micro-cilia.The antifouling tests demonstrate that the chemically modified micro-cilia can effectively expel gravels under the stimulation of an external magnetic field and enable the BMRAS to achieve dynamic self-cleaning.Specifically,0.17 g gravel distributed on BMRAS can be completely cleaned up within 0.296 s,which improved by 14.2%compared with the flat materials.This work provides a brief and effective strategy for designing dynamic antifouling surfaces with excellent physicochemical durability and great potential value in the applications of marine fouling.展开更多
Diabetic liver injury is a widespread complication of diabetes and carries a high risk to liver function.Therefore,early diagnosis of diabetic liver injury is of great significance for providing quality of life for di...Diabetic liver injury is a widespread complication of diabetes and carries a high risk to liver function.Therefore,early diagnosis of diabetic liver injury is of great significance for providing quality of life for diabetic patients.Most of the activated dual-modal probes are usually activated by single factor stimulation,which greatly reduces the diagnostic accuracy of liver injury.Here,a novel cysteine(Cys)/homocysteine(Hcy)and viscosity-enhanced dual-modal probe DAL was developed for the first time to monitor diabetic liver injury and its repair process.In the presence of Cys/Hcy,the near-infrared fluorescence(NIRF)and photoacoustic(PA)signals of the probe DAL were activated,with further signal enhancement in high viscosity environments.This Cys/Hcy and viscosity cascade probe exhibits heightened sensitivity and enhanced anti-interference capabilities,contributing to the advancement of liver injury diagnosis accuracy.In addition,the probe DAL shows exceptional mitochondrial targeting ability,enabling sensitive monitoring of Cys/Hcy and viscosity alterations within mitochondria.Based on NIRF/PA dual-modal imaging technology,the probe was successfully used for the first time in a mouse diabetic liver injury model to evaluate the extent of liver damage and the repair process by tracking the levels of Cys/Hcy and viscosity.Therefore,the two-factor activated dual-modal probe developed in this study provides a powerful instrument for accurate diagnosis and efficacy evaluation of complications related to diabetes.展开更多
Soft actuators and stimuli responsive materials are highlighted in the research field for their enormous potential in transit tasks,sensing,and biomedical devices,particularly the magnetic responsive soft actu-ators d...Soft actuators and stimuli responsive materials are highlighted in the research field for their enormous potential in transit tasks,sensing,and biomedical devices,particularly the magnetic responsive soft actu-ators driven by magnetic force remotely.Nevertheless,the further study of magnetic responsive actuators with complex three-dimensional geometries and multiple functions is still limited by uncomplicated de-sign and flexible locomotion.This work provides a novel scheme integrating the origami method and modular designs,which defines the inner properties of magnetic material,extending the functions of magnetic responsive actuators with various modules.The directions of the inner magnetic moments can be programmed and the deformation degrees can be regulated by this approach,which promotes the fabrication of complicated soft actuators with multiple functions by integrating with modular designs.Especially,a movable actuator with various sensing modulus is designed by the origami method,which can perform the sensing application to external ultra-violet(UV),heat,and pH stimuli.Moreover,a mi-croneedle modular actuator which can be controlled wirelessly by a magnetic field was demonstrated for the potential application in the biomedical field.This proposed scheme for engineering magnetic respon-sive material with modular designs has shown great potential to improve the feasibility,versatility,and multiple functionalities of soft actuators.展开更多
基金supported by the National Natural Science Foundation of China(No.22271202 to L.Yuan,No.22201193 to X.Li)the Sichuan Science and Technology Program(No.2023NSFSC0109 to X.Li)+2 种基金the Fundamental Research Funds for the Central Universities and the Hundred Talent Program of Sichuan University(No.YJ2021158 to X.Li)Sichuan University Interdisciplinary Innovation Fund(X.Li)Open Project of State Key Laboratory of Supramolecular Structure and Materials(No.SKLSSM2024037)。
文摘A novel[3]rotaxane,featuring two hydrogen-bonded aramide azo-macrocycles mechanically interlocked on a dumbbell with distinct recognition sites,a secondary dialkylammonium(AM)unit and a 4,4'-bipyridinium(BP)unit,has been synthesized.This multi-stimuli-responsive[3]rotaxane exhibits unique molecular motion,with the macrocycles shuttling along the axle in response to acid-base reactions,temperature changes,solvent variations,and light irradiation.The molecular shuttle and reversibility were investigated by^(1)H NMR,2D NOESY,HRESI-MS,and UV-vis spectroscopy.This study provides a rare example of a higher order rotaxane with multi-stimuli responsiveness,highlighting its potential for multi-state control over the motion of interlocked rings on an axle.The ability to manipulate the molecular motion of the macrocycles through various external triggers offers insights for future developments in molecular machinery and adaptive materials.
基金supported by the National Natural Science Foundation of China(Nos.21064006,21161018 and 21262032)the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(No.IRT1177)+2 种基金the Natural Science Foundation of Gansu Province(No. 1010RJZA018)the Youth Foundation of Gansu Province(No.1208RJYA048)NWNU-LKQN-11-32
文摘A novel smart metal-organic gel(MOG) formed from biscarboxyl-functionalized benzimidazole derivative(D11) in the presence of lead nitrate has been investigated.The critical gel concentration for the formation of MOG was just 0.36 wt%,which exhibits a super gelation capability of D11.The coordination of the metal to the ligand D11 was found to play a vital role in the construction of the supramolecular MOG.Microstructures determined by SEM observation demonstrated that the MOG was formed by intertwined fibrils.Interestingly,the MOG exhibits pH-induced,thermo-induced,and chemical-induced reversible gel-sol transition.Meanwhile,this supramolecular MOG shows desirable absorption ability of methyl orange dye molecules in aqueous solution.
基金supported by the National Natural Science Foundation of China(Nos.22071273 and 21821003)Fundamental Research Funds for the Central Universities,Sun Yat-sen University(No.23lgzy001)。
文摘Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches,memories,and molecular machines.The exploration of the material is currently focused on the pure organic system,which limits the development o such materials greatly.In this work,we present a new chiral organic-inorganic hybrid salt,(R-3hydroxypyrrolidinium)_(2)[Fe(CN)_(5)(NO)](1),which exhibits rare multi-stimuli responsive behaviors in ther mal,mechanical and optical channels.In detail,1 undergoes a C2-P2_(1)22_(1) phase transition deriving from the thermal motion of organic cations with the increase of temperature,but the reverse transition can only be induced by mechanical pressure.Moreover,polycrystalline hybrid salt showed photo-responsive performance,i.e.,the ground-state N-bound nitrosyl ligand adopts two configurations in excited state caused by light in 532 nm irradiation,accompanying with a photo-induced structural transformation o the anionic framework.Namely,the thermal motion characteristics of organic cations,the photoresponse characteristics of anionic inorganic skeleton and the pressure characteristics from hydrogen bonds are si multaneously integrated in 1.This unprecedented coupling mechanism of multi-stimuli responses make1 a potential candidate for future multichannel data storage applications.
基金supported by the National Key Research and Development Program of China(2022YFA12055002)the National Natural Science Foundation of China(22272101,22427802)the Program of Introducing Talents of Discipline to Universities(“111”project,B14041)。
文摘Thin-film materials with flexibility and stretchability are essential for wearable smart technologies.However,achieving both superior mechanical properties and multi-stimuli responsiveness in ultrathin films remains a significant challenge.Herein,we report a novel class of multifunctional thin-film materials fabricated via dynamic covalent self-assembly of two key components:a renowned aggregation-induced emission(AIE)luminogen,tetraphenylethylene with four benzaldehyde groups(TTPE-CHO),serving as the emissive and rigid backbone,and hydrazide-functionalized polyethylene glycol(PEG 400 and PEG 600)chains,imparting flexibility.The resulting films exhibit green fluorescence,high flexibility,stretchability,anisotropic morphological features,and multiple stimuli-responsive properties—capabilities that are severely limited in the absence of PEG chains.Remarkably,even at an ultrathin thickness of only 4μm,the TTPE-DTH-400-G film achieves a record-breaking tensile stress of 47 MPa,demonstrating outstanding mechanical strength and elasticity.Furthermore,it enables reversible vapor-triggered actuation and exhibits exceptional fluorescence sensing performance for detecting the sarin analog diethyl chlorophosphate(DCP),with an ultralow detection limit of 1 ppt and a rapid response time.This study presents an effective strategy for integrating rigid and flexible components to construct functional thin films with superior mechanical properties and intelligent responsiveness,paving the way for advanced applications in wearable electronics and real-time hazardous substance detection.
基金supported by the National Science Fund for Excellent Young Scholars (32322044)the CQMU Program for Youth Innovation in Future Medicine (W0077)+1 种基金the Program for Scientific and Technological Innovation Leader of Chongqing (CQYC20220303655)the Young Scientists Fund of the National Natural Science Foundation of China (82301144)。
文摘Nanotechnology has provided thousands of novel nano-antimicrobials possessing features uncommon in clinically available antimicrobials.Here,nanocarriers loaded with conventional antimicrobials and responding to environmental changes upon entry into oral biofilms are reviewed.Supra-gingival biofilms are characterized by acidic pH,the presence of bacterial enzymes,and the development of hypoxia in deeper layers.Sub-gingival biofilms are slightly alkaline,with hypoxia occurring over their entire depth.Upon entering biofilms,negatively charged,pH-and/or hypoxia-responsive nanocarriers become positively charged.This charge reversal leads to electrostatic double-layer attraction between positively charged nanocarriers towards negatively charged,waterfilled channel walls in biofilms,enhancing their accumulation in a biofilm.Degradation of bacterial enzyme-responsive nanocarriers causes in-biofilm release of antimicrobial cargo,yielding higher local antimicrobial concentrations than can be achieved through their direct,oral administration without harming soft tissues.Enhanced antibiofilm activity after in-biofilm antimicrobial release from biofilm-responsive micelles and liposomes has been demonstrated in vitro towards single-species Streptococcus mutans and Staphylococcus aureus biofilms or in vivo using specific-pathogen-free rodents inoculated with selected pathogens.This preferential antibacterial activity regulated the microbial composition of ex vivo human oral biofilm towards a more healthy microbiome composition.Although clinical confirmation is limited,the potential benefits of stimuli-responsive,antimicrobial-loaded nanocarriers for oral biofilm control and microbiome restoration are worth further investigation towards clinical translation.
基金supported by the National Natural Science Foundation of China(Nos.51603005,52403186 and 52573150)Fujian Provincial Natural Science Foundation of China(No.2024J011447)+1 种基金Natural Science Foundation of Xiamen,China(No.3502Z20227305)the Postdoctoral Fellowship Program of CPSF(No.GZC20240095)。
文摘Near-infrared(NIR)light-responsive shape memory polymers(SMPs)show great promise for biomedical applications,but conventional photothermal agents suffer from high cost,complex preparation,or poor biocompatibility,while lignin-based alternatives exhibit insufficient photothermal conversion efficiency.Herein,we developed a novel strategy to enhance photothermal performance of lignin through sequential demethylation modification and Fe^(3+)complexation for constructing NIR light responsive SMPs.Dealkaline lignin(DL)was first demethylated using iodocyclohexane to produce demethylated lignin(DDL)with increased catechol content,which was then incorporated into polycaprolactone-based polyurethane synthesis followed by Fe^(3+)complexation.Results showed that DDL-Fe^(3+)complexes have significantly enhanced photothermal conversion performance,and the resulting PU-DDL+Fe^(3+)polyurethane with 0.5 wt%DDL content demonstrated a temperature increases of 39.8℃under 0.33 W·cm-2808 nm NIR irradiation.This excellent photothermal performance enables the shape-fixed PU-DDL+Fe^(3+)polyurethane to rapidly recover to its initial shape under NIR light irradiation.Additionally,PU-DDL+Fe^(3+)polyurethane exhibits good mechanical properties and biocompatibility,demonstrating significant biomedical application potential.
基金Supported by the National Natural Science Foundation of China(No.82071571)the Natural Science Foundation of Guangdong Province(No.2021A1515010601)+3 种基金Guangdong Provincial Basic and Applied Basic Research Foundation-Dongguan Joint Fund(No.2024A1515140121)the“Climbing”Program of Guangdong Province(No.pdjh2021b0226)the Innovation and Entrepreneurship Program for College Students(No.GDMU2022038,202310571038,ZZDC002,S202510571041)Guangdong Medical University Undergraduate Innovation and Entrepreneurship Education Base Project(No.JDXM2024039,JDXM2025046)。
文摘Genomic destabilization and defective DNA repair are the most prominent features of tumour cells and are exploited by various chemotherapy drugs for cancer therapy.Long non-coding RNA(lncR-NAs)have emerged as powerful regulators of gene expression and are thus involved in diverse biological processes.Recent studies have demonstrated that several lncRNAs play critical roles in DNA repair.Nonetheless,the relationship between DNA damage-responsive lncRNAs and chemoresistance remains poorly defined.In this study,we established four different DNA damage models triggered by cisplatin(DDP),H2O2,neocarzinostatin(NCS)or ultraviolet(UV)irradiation and identified a specific upregu-lated lncRNA(lnc-DUSP6)involved in the cisplatin-induced DNA damage response.Furthermore,loss-or gain-of-function experiments confirmed that lnc-DUSP6 enhanced DNA repair and cell survival under cisplatin treatment,thus promoting cisplatin resistance.Mechanistically,an RNA immunoprecipitation(RIP)assay revealed that lnc-DUSP6 directly interacts with DUSP6(Dual Specificity Phosphatase 6),which is closely associated with cisplatin sensitivity.Additionally,overexpression of DUSP6 significantly rescued the effects of lnc-DUSP6 silencing on DNA repair and cell survival under cisplatin treatment.O-verall,our results show the effect and underlying mechanism of lnc-DUSP6 in cisplatin resistance:lnc-DUSP6 promotes cisplatin-induced DNA damage repair and cisplatin resistance by stabilizing DUSP6,which is highly clinically important for enhancing the efficacy of cisplatin for cancers.
基金supported by the National Natural Science Foundation of China(22375002)the Anhui Provincial Natural Science Foundation(2308085Y10).
文摘Solvents in crystalline materials typically exist either as structural components that stabilize the framework or as adsorbed vips that modulate properties,yet achieving their orthogonal coexistence within a single system remains challenging.This study proposes a natural mineral-inspired solvent hierarchy strategy that enables the concurrent achievement of framework stability and dynamic responsiveness in hydrogen-bonded organic frameworks(HOFs)through the orthogonal integration of structural and adsorbed solvents.We have validated the feasibility of this solvent hierarchy approach based on four model systems with progressively increasing stability and dynamism:(1)unstable HOFs containing only adsorbed solvents,(2)unstable HOFs with low-binding-energy structural solvents,(3)stable HOFs incorporating strong-fitted structural solvents,and(4)stable HOFs with structural solvents and dynamically adjustable adsorption solvents.Crystallographic and theoretical analyses reveal that the superior stability of structural solvents originates from the high-electron-density oxygen of the DMSO S═O bond,which acts as a strong hydrogen-bond acceptor,forming stable N─H…O═S bonds with amine groups.The host’s aggregation-induced emission(AIE)characteristics allow real-time optical monitoring of reversible single-crystal-to-single-crystal transformations without compromising structural integrity,demonstrating promising applications for visual water content and water leakage detection.This work not only establishes a new paradigm in solvent engineering for developing smart crystalline materials but also expands the design possibilities for functional porous frameworks.
基金financially supported by the National Natural Science Foundation of China(Nos.52473139 and U21A2098)。
文摘Hospital wastewater contains complex pollutants,including residual organic dyes and antibiotic-resistant pathogens,posing severe risks to ecosystems and human health.Conventional adsorbents,constrained by monopolar functional groups and limited surface sites,fail to remove both pollutants simultaneously.Here,we report an intelligent responsive polyurethane microsphere adsorbent doped with diallyl dimethylammonium chloride modified carbon nanotubes,termed as PUCD microspheres.The PUCD integrates bipolar adsorption sites,tunable micrometer-scale pores,and a near-infrared(NIR)-triggered in situ capture mechanism within a single platform,which achieves up to 98.3%dye removal,maintains strong adsorption performance across a wide pH range and retains 83.3%efficiency for rhodamine B after five cycles.Notably,the PUCD employs a temperature-responsive phase transition:under NIR irradiation,the microspheres undergo shrinkage,reducing the pore size to generate a‘polymer trap',enabling in situ capture of bacteria with>99%efficiencies for both Staphylococcus aureus and Escherichia coli.By immobilizing live bacteria,the PUCD microspheres substantially reduces the risk of pathogen desorption and toxin release.This promising platform offers a safe,efficient,and single-stage strategy for hospital wastewater purification,enabling the simultaneous elimination of dyes and pathogenic bacteria.
基金supported by the financial assistance from Natural Science Fund Project of Science and Technology Department of Jilin Province (Nos.YDZJ202301ZYTS141,YDZJ202501ZYTS793)。
文摘Hepatic fibrosis is regulated by the synergistic actions of various cells and cytokines,with the activation and proliferation of hepatic stellate cells(HSCs) being considered the central event in this process.To achieve specific targeting of activated hepatic stellate cells(a HSCs) and precise treatment of hepatic fibrosis,this study developed a dual-functional drug delivery system(SIL/c RGD-PEG-PPS PMs) with both targeting and responsive release capabilities.It aims to target the αvβ 3 receptor specifically expressed on the surface of a HSCs using the cyclic peptide c(RGDyk),and to exploit the high reactive oxygen species(ROS) level in the cellular microenvironment to achieve concentrated burst release of drugs at the pathological sites of hepatic fibrosis.Based on multiple assessments,SIL/c RGD-PEG-PPS PMs specifically enhanced the targeted delivery of silybin(SIL) to a HSCs,inhibited the proliferation and migration of a HSCs,and exhibited good biosafety.Additionally,it demonstrated excellent anti-fibrotic activity in fibrotic mice.In summary,this study shows great potential in targeted treatment of hepatic fibrosis and provides a multifunctional tool for advancing the research and therapeutic strategies of hepatic fibrosis.
基金supported by the National Natural Science Foundation of China(NSFC Nos.52271228,52127802,52201279,52301288,52202298,and 22208262)the Natural Science Foundation of Shaanxi Province(No.2023-JC-ZD-21)+1 种基金the Key Research and Development Plan of Shaanxi Province(No.2023GXLH-046)the Science and Technology Project of Xi'an(No.2021SFGX0004)。
文摘Simultaneous integration of rich oxygen vacancies(OVs)and twin crystals in a photocatalyst can not only significantly enhance the near-infrared(NIR)light response but also greatly improve the photocharge separation and transfer efficiency owing to the induced high electrical conductivity and strong built-in electric field.However,thus far,there has been a lack of a model catalyst containing both twin crystals and OVs.Herein,we develop a simple wet chemical strategy for synthesizing of unprecedented NIR light-responsive OVs-rich Cu_(2)O black nanoparticles with high-density of twin crystals(denoted as black twinned Cu_(2)O).As expected,the black twinned Cu_(2)O exhibits higher visible-NIR and NIR light-driven photodegradation of tetracycline(TC)solution than the counterparts.Significantly,the mechanism insight into twin-dependent photocatalysis in NIR light-responsive Cu_(2)O black nanocrystals with rich OVs is uncovered in depth by density functional theory(DFT)calculations and a series of experimental evidence.Expectantly,this work would be beneficial for the scientific researchers currently focusing on the NIR light-responsive photocatalysis and twin engineering of photocatalysts.
基金supported by the Joint Funds of National Natural Science Foundation of China(No.U22A20162)the Natural Science Foundation of Hebei Province of China(No.C2021202002)+1 种基金the National Natural Science Foundation of China(No.52271245),the Natural Science Foundation of Tianjin(No.21JCQNJC01280)the financial support from the Danish Council for Independent Research(9040-00219B),European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement ENSIGN(Project ID:101086226),L4DNANO(Project ID:101086227).
文摘Microneedle(MN)patches could be a promising treatment for diabetic foot ulcers that plague thousands of people worldwide.While reducing skin resistance or increasing driving force can accelerate the efficiency of transdermal drug delivery with conventional MN patches,it can create toxic chemical residues or require the help of additional devices.Herein,a thermo-responsive microneedles patch(TMN)with high biocompatibility without additional equipment is proposed.The TMN consisted of a bilayer microneedles composed of sodium alginate(SA)-g-poly(N-isopropylacrylamide)layer(SA-g-PNIPAM)loaded with sucrose octasulfate sodium salt(SOS)and hyaluronic acid layer and a polycaprolactone/chitosan nanofiber membrane loading with tetracycline hydrochloride(TH)and SOS.PNIPAM accelerates drug release by extruding the drug through a volumetric phase transition in response to temperature changes,and TH and SOS promote wound healing by inhibiting bacterial growth and promoting vascular regeneration and epithelial formation.The results showed that the drug release of TMN was significantly faster,with the drug release rate of more than 80% in the 10th h,and the antibacterial rate of TMN could reach 800%.In addition,TMN had good biocompatibility and good healing effects in vivo,which may be helpful for the design of multifunctional dressings in the future.
基金Financially supported by the National Natural Science Foundation of China (21871027)。
文摘A viologen-bearing Zn(Ⅱ) coordination polymer,[Zn(Bpybc)SO_(4)]·H_(2)O,has been successfully synthesized and structurally characterized.The title compound exhibits sunlight and UV-induced photochromism,thermoschromism,and amine-selective chemochromism.
基金supported by the National Natural Science Foundation of China(Nos.52025132,U24A20205,52303373,21621091,22021001,and 22121001)the China Postdoctoral Science Foundation(No.2024M763174)+2 种基金the 111 Project(Nos.B17027,B16029)the Natural Science Foundation of Fujian Province of China(No.2022J02059)the New Cornerstone Science Foundation through the Xplorer Prize。
文摘Controllable liquid manipulation is of paramount scientific and technological importance in various fields,such as the chemical industry,biomedicine,and agricultural production.Magnetic actuation,characterized by rapid,contactless,and environmentally benign operation,has emerged as a promising approach for precise liquid control.However,conventional magnetic strategies typically govern droplet movement on open surfaces,facing limitations such as restricted liquid volumes,uncertain flow paths,and inevitable evaporation,thereby constraining their broader practical applications.Recently,a variety of magneticdriven strategies have been developed to dynamically regulate liquids within enclosed spaces,especially through physicochemical mechanisms.These approaches provide efficient control over liquid behavior by leveraging magnetically induced chemical changes,structural deformations,and dragging motions,opening new opportunities for flexible and versatile fluid management.This review explores the design and mechanisms of magneto-responsive confined interfaces for the manipulation of nonmagnetic liquids,highlighting key advancements and potential applications including liquid valves,liquid mixing,liquid flow regulation,and liquid pumping.Finally,the existing challenges and future prospects in this field are presented.
基金supported by the Natural Science Foundation of Shaanxi Province(Nos.2023-YBSF-270,2024SF-ZDCYL-02-08)Fundamental Research Funds for the Central Universities(No.xzy022024033)+2 种基金Horizontal Project of the First Affiliated Hospital of Xi’an Jiaotong University(No.202304174)supported by the Opening Project of Structural Optimization and Application of Functional Molecules Key Laboratory of Sichuan Province(No.2023GNFZ-03)The Key Laboratory for Screening and Diagnosis of Maternal and Child Genetic Disease of Health Commission of Jiangxi Province.
文摘The tumor microenvironment(TME)-activatable probes have proven effective in enhancing the signalto-background ratio(SBR)for precise fluorescence imaging in tumor diagnosis.However,many fluorophores have suboptimal emission spectra and a short Stokes shift,which may lead to overlap with bioautofluorescence,excitation,and emission spectra,limiting their use in intraoperative guidance.Herein,aγ-glutathione(GSH)responsive near-infrared(NIR)BODIPY probe,named“Pro-Dye”was synthesized with a large Stokes shift of 91 nm.The Pro-Dye can be rapidly and specifically activated by high concentrations of GSH both in solution and inside cancer cells,while remaining inactive in normal cells(Human umbilical vein endothelial cells,HUVECs).The Pro-Dye was further encapsulated by 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-(polyethylene glycol)-5000(DSPE-PEG5000)to form Pro-Dye nanoparticles(NPs),making it water-dispersible for in vivo application.In vivo fluorescence imaging demonstrated that Pro-Dye NPs can accumulate at the tumor and exhibit an improved SBR compared to the“alwayson”probe(Dye NPs).Moreover,the tumor can be precisely resected under the real-time guidance of fluorescence imaging of Pro-Dye NPs,showing a well-defined tumor margin.
基金supported by the National Natural Science Foundation of China(Grant Nos.:82373833,22177039,and 82304438)the National Key Research and Development Program of China(Grant No.:2021YFC2300400)Guangdong Basic and Applied Basic Research Foundation,China(Grant Nos.:2024A1515012204,2022A1515010300,and 2022A1515110618).
文摘Rapid and ultrasensitive detection of pathogen-associated biomarkers is vital for the early diagnosis and therapy of bacterial infections.Herein,we developed a close-packed and ordered Au@AgPt array coupled with a cascade triggering strategy for surface-enhanced Raman scattering(SERS)and colorimetric identification of the Staphylococcus aureus biomarker micrococcal nuclease(MNase)in serum samples.The trimetallic Au@AgPt nanozymes can catalyze the oxidation of 3,3’,5,5’-tetramethylbenzidine(TMB)molecules to SERS-enhanced oxidized TMB(oxTMB),accompanied by the color change from colorless to blue.In the presence of S.aureus,the secreted MNase preferentially cut the nucleobase AT-rich regions of DNA sequences on magnetic beads(MBs)to release alkaline phosphatase(ALP),which subsequently mediated the oxTMB reduction for inducing the colorimetric/SERS signal fade away.Using this“on-to-off”triggering strategy,the target S.aureus can be recorded in a wide linear range with a limit of detection of 38 CFU/mL in the colorimetric mode and 6 CFU/mL in the SERS mode.Meanwhile,the MNase-mediated strategy characterized by high specificity and sensitivity successfully discriminated between patients with sepsis(n=7)and healthy participants(n=3),as well as monitored the prognostic progression of the disease(n=2).Overall,benefiting from highly active and dense“hot spot”substrate,MNase-mediated cascade response strategy,and colorimetric/SERS dual-signal output,this methodology will offer a promising avenue for the early diagnosis of S.aureus infection.
基金financially supported by the National Natural Science Foundation of China(Nos.22273098,52033001 and 22303032)the Key Project of Anhui Province Science and Technology Innovation Platform(No.S202305a12020030)+1 种基金the Science and Technology Program Project of Zhejiang Province,China(No.2025ZY01057)partially carried out at the USTC Center for Micro and Nanoscale Research and Fabrication。
文摘Strong polyelectrolyte brushes(SPBs)play an important role in enabling material surface functionalization due to their unique stimuli-responsive properties.Although the unexpected pH responsiveness of SPBs has been revealed in the past ten years,it is still unclear if the pH-responsive properties of SPBs are affected by the brush thickness.In this study,we employed the positively charged poly[2-(methacryloyloxy)ethyl]trimethylammonium chloride(PMETAC)and negatively charged sodium poly(styrenesulfonate)(NaPSS)brushes as model systems to explore the effect of thickness on the pH-responsive properties of SPBs.The results demonstrate that the pH-responsive properties of SPBs manifest different dependences on the brush thickness.Specifically,for both PMETAC and NaPSS brushes,the pH-responsive hydration and stiffness are influenced by the thickness,and the pH-responsive wettability and adhesion are almost unaffected by the thickness.This work not only provides a clear understanding of the relationship between the brush thickness and the pH responsiveness of SPBs,but also offers a new method to control the pH-responsive properties of SPBs.
基金supported by the National Key Research and Development Program of China(2023YFB4605700)the Foundation for Innovative Research Groups of the National Natural Science Foundation of China(No.52021003)+4 种基金the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(No.52222509)the Natural Science Foundation of Jilin Province(No.20220101220JC)the Defense Industrial Technology Development Program(JCKY2023130C001)Changbai Talents Plan of Jilin Province“Fundamental Research Funds for the Central Universities”.
文摘Superhydrophobic/superhydrophilic antifouling materials are widely used to solve the severe water pollution and bio-adhesion of marine equipment.However,conventional antifouling materials rely on the static superwettability of surfaces,which suffer from poorly sustained antifouling effects.Inspired by the unique dynamic antifouling strategies of Calliphora Vicina wing surface based on the hydrophobic micro-cilia arrays,a Biomimetic Magnetic-Responsive Antifouling Surface(BMRAS)is designed and fabricated using a method combining UV lithography and an inverse molding.The BMRAS is coated by high-aspect-ratio micro-cilia,which are filled with synthesized magnetic Fe3O4 nanoparticles.The bioinspired hydrophobic micro-cilia arrays endow the BMRAS with excellent intrinsic superhydrophobicity,benefiting from the high-aspect-ratio feature and roughness effect.Remarkably,the static contact angle is more than 156.9±1.6°and the rolling angle is less than 2.3±0.3°.The synthesized magnetic nanomaterials play a key role in implementing dynamic antifouling strategies.On the one hand,the surface tension can be adjusted as required under magnetically controlled oscillations.On the other hand,the doping of magnetic nanomaterials can enhance mechanical properties and reduce capillary force-induced aggregation of high-aspect-ratio micro-cilia.The antifouling tests demonstrate that the chemically modified micro-cilia can effectively expel gravels under the stimulation of an external magnetic field and enable the BMRAS to achieve dynamic self-cleaning.Specifically,0.17 g gravel distributed on BMRAS can be completely cleaned up within 0.296 s,which improved by 14.2%compared with the flat materials.This work provides a brief and effective strategy for designing dynamic antifouling surfaces with excellent physicochemical durability and great potential value in the applications of marine fouling.
基金financially supported by the National Natural Science Foundation of China(Nos.21877048,22077048,and 22277014)Guangxi Natural Science Foundation(Nos.2021GXNSFDA075003,AD21220061)the Startup Fund of Guangxi University(No.A3040051003).
文摘Diabetic liver injury is a widespread complication of diabetes and carries a high risk to liver function.Therefore,early diagnosis of diabetic liver injury is of great significance for providing quality of life for diabetic patients.Most of the activated dual-modal probes are usually activated by single factor stimulation,which greatly reduces the diagnostic accuracy of liver injury.Here,a novel cysteine(Cys)/homocysteine(Hcy)and viscosity-enhanced dual-modal probe DAL was developed for the first time to monitor diabetic liver injury and its repair process.In the presence of Cys/Hcy,the near-infrared fluorescence(NIRF)and photoacoustic(PA)signals of the probe DAL were activated,with further signal enhancement in high viscosity environments.This Cys/Hcy and viscosity cascade probe exhibits heightened sensitivity and enhanced anti-interference capabilities,contributing to the advancement of liver injury diagnosis accuracy.In addition,the probe DAL shows exceptional mitochondrial targeting ability,enabling sensitive monitoring of Cys/Hcy and viscosity alterations within mitochondria.Based on NIRF/PA dual-modal imaging technology,the probe was successfully used for the first time in a mouse diabetic liver injury model to evaluate the extent of liver damage and the repair process by tracking the levels of Cys/Hcy and viscosity.Therefore,the two-factor activated dual-modal probe developed in this study provides a powerful instrument for accurate diagnosis and efficacy evaluation of complications related to diabetes.
基金support provided by the Hong Kong RGC Theme-based Research Scheme(No.AoE/M-402/20)Hong Kong RGC Area of Excellence Scheme(No.AoE/E-101/23-N)+1 种基金Hong Kong RGC Theme-based Research Scheme(No.T45-406/23-R)the Hong Kong Innovation and Technology Commission via the Hong Kong Branch of National Precious Metals Material Engineering Research Center.
文摘Soft actuators and stimuli responsive materials are highlighted in the research field for their enormous potential in transit tasks,sensing,and biomedical devices,particularly the magnetic responsive soft actu-ators driven by magnetic force remotely.Nevertheless,the further study of magnetic responsive actuators with complex three-dimensional geometries and multiple functions is still limited by uncomplicated de-sign and flexible locomotion.This work provides a novel scheme integrating the origami method and modular designs,which defines the inner properties of magnetic material,extending the functions of magnetic responsive actuators with various modules.The directions of the inner magnetic moments can be programmed and the deformation degrees can be regulated by this approach,which promotes the fabrication of complicated soft actuators with multiple functions by integrating with modular designs.Especially,a movable actuator with various sensing modulus is designed by the origami method,which can perform the sensing application to external ultra-violet(UV),heat,and pH stimuli.Moreover,a mi-croneedle modular actuator which can be controlled wirelessly by a magnetic field was demonstrated for the potential application in the biomedical field.This proposed scheme for engineering magnetic respon-sive material with modular designs has shown great potential to improve the feasibility,versatility,and multiple functionalities of soft actuators.