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
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
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
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
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
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
Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials prov...Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials provide a promising prospect for imaging-guided precision therapy.Considering that tumor-derived alkaline phosphatase(ALP)is over-expressed in metastatic PCa,it makes a great chance to develop a theranostics system with ALP responsive in the TME.Herein,an ALP-responsive aggregationinduced emission luminogens(AIEgens)nanoprobe AMNF self-assembly was designed for enhancing the diagnosis and treatment of metastatic PCa.The nanoprobe exhibited self-aggregation in the presence of ALP resulted in aggregation-induced fluorescence,and enhanced accumulation and prolonged retention period at the tumor site.In terms of detection,the fluorescence(FL)/computed tomography(CT)/magnetic resonance(MR)multi-mode imaging effect of nanoprobe was significantly improved post-aggregation,enabling precise diagnosis through the amalgamation of multiple imaging modes.Enhanced CT/MR imaging can achieve assist preoperative tumor diagnosis,and enhanced FL imaging technology can achieve“intraoperative visual navigation”,showing its potential application value in clinical tumor detection and surgical guidance.In terms of treatment,AMNF showed strong absorption in the near infrared region after aggregation,which improved the photothermal treatment effect.Overall,our work developed an effective aggregation-enhanced theranostic strategy for ALP-related cancers.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
Melanoma,a common malignant skin tumor,faces challenges with multidrug resistance and high recurrence rates.Combining photodynamic therapy(PDT)and immunotherapy offers a promising personalized treatment approach.Howev...Melanoma,a common malignant skin tumor,faces challenges with multidrug resistance and high recurrence rates.Combining photodynamic therapy(PDT)and immunotherapy offers a promising personalized treatment approach.However,poor water solubility and significant side effects of photosensitizers and immune checkpoint inhibitors(ICIs)limit their application.Enhancing delivery efficiency while reducing adverse effects is crucial.Herein,we formulate BM@HSSC nanoparticles(NPs),which consist of a reduction-responsive hyaluronic acid(HA)backbone modified with photosensitizer chlorin e6(Ce6)and loaded with the programmed cell death-ligand 1(PD-L1)inhibitor BMS-1.This system synergistically integrates PDT,immunogenic cell death(ICD),and immunotherapy for melanoma treatment.BM@HSSC NPs target and accumulate at the tumor site via the CD44 receptor.The disulfide bonds(-S-S-)in the NPs react with high glutathione(GSH)concentrations in tumor cells,rapidly releasing Ce6 and BMS-1.Under 660 nm laser irradiation,BM@HSSC NPs generate cytotoxic reactive oxygen species(ROS),inducing cell apoptosis and triggering ICD via PDT damage-associated molecular patterns(DAMPs)and tumor-associated antigens(TAAs)released from ICD promote dendritic cell(DC)maturation,enhancing antigen presentation and activating cytotoxic T lymphocytes(CTLs).Meanwhile,BMS-1 blocks the programmed cell death-1(PD-1)/PD-L1 pathway,countering the immunosuppressive tumor microenvironment(iTME)and inhibiting tumor cell immune escape.This strategy amplifies antitumor immune responses by enhancing immunogenicity and synergizing with ICIs,resulting in robust antitumor efficacy.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
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
Black wings of butterfly Ornithoptera goliath and infrared-band radiative cooling function of Rapala dioetas butterfly wings are associated with black pigment(e.g.,melanin)and unique hierarchical micro/nanostructures,...Black wings of butterfly Ornithoptera goliath and infrared-band radiative cooling function of Rapala dioetas butterfly wings are associated with black pigment(e.g.,melanin)and unique hierarchical micro/nanostructures,greatly stimulating biomimetic fabrication of functional photonic structures but mainly targeted to one prototype.Targeted at two-prototype integrated biomimetic fabrication from fully compositional/structural/functional aspects,femtosecond(fs)laser subtractive/additive-integrated hierarchical micro/nano-manufacturing technique is proposed in this work.This technique can one-step transfer refractory metals(e.g.,W,Mo,Nb,Ta)into black non-stoichiometric oxide nanomaterials with abundant oxygen vacancies and simultaneously enable the realization of in situ quasi-controllable micro/nanoscale hierarchical aggregation and assembly,all displaying black color but with tunable infrared emission.Adjusting the scan interval for biomimetic manufacturing can tailor the structural oxidation degree,the emission in the long-wave infrared(LWIR)band while keeping the blackness of hierarchical aggregates,and the confined height between the covering quartz plate and the ablated sample.The blackening efficiency of this technique can reach∼11.25 cm^(2)·min^(−1),opening opportunities for high-throughput optical/thermal applications.Selectively patterned Chinese characters,Arabic numbers,and English letters are easily fabricable,which are intrinsically invisible-infrared dual-band encrypted but decryptable via static/dynamic environment stimuli(e.g.,sample heating/cooling,introducing external hot/cold sources including human hands).The self-evolution from‘orderless’structuring to‘ordered’functionalization is validated for the proposed fs laser subtractive/additive-integrated biomimetic manufacturing,specifically from the synthesis of diverse black nanomaterials and the seemingly disordered micro/nano-aggregates to the ordered optical/thermal regulation capacities for a delicate modulation of information encryption and decryption,unveiling a new concept for future exploration and extension.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
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
Aggregation-induced emission luminogens(AIEgens)exhibit viscosity-responsive behavior resembling those of molecular rotors;however,their response mechanisms are more complex and cannot be adequately described using si...Aggregation-induced emission luminogens(AIEgens)exhibit viscosity-responsive behavior resembling those of molecular rotors;however,their response mechanisms are more complex and cannot be adequately described using simple rotational models.AIEgens demonstrate intricate dynamics that are highly dependent on their molecular structures.In this study,we synthesized water-soluble derivatives of representative AIEgens,including tetraphenylethene(TPE),bis(N,N-dialkylamino)anthracene(BDAA),and bridged stilbene,and systematically investigated the dependence of their photophysical properties in water/glycerol mixed solvents on temperature and viscosity.To elucidate the origin of their viscosity responsiveness,quantum chemical calculations were conducted to analyze their potential energy surfaces(PESs).The results revealed that compared to typical molecular rotors,these AIEgens exhibit significantly higher sensitivity to viscosity in low-viscosity regions.Notably,for TPE and BDAA derivatives,the viscosity responsiveness was found to be governed not by the activation energy barrier(ΔE_(a))based on the PES,but rather by the viscosity-dependent constraints on molecular structural changes.Furthermore,molecules possessing multiple aromatic rings or large,flexible,rotatable moieties were found to exhibit enhanced sensitivity to viscosity due to increased frictional interactions in solutions.This study provides critical insights into the mechanistic origins of the viscosity responsiveness of AIEgens,thereby advancing the fundamental understanding of their behavior and expanding their potential application as viscositysensitive probes.展开更多
In deep oil reservoir development,enhanced oil recovery(EOR)techniques encounter significant challenges under high-temperature and high-salinity conditions.Traditional profile-control agents often fail to maintain sta...In deep oil reservoir development,enhanced oil recovery(EOR)techniques encounter significant challenges under high-temperature and high-salinity conditions.Traditional profile-control agents often fail to maintain stable blocking under extreme conditions and exhibit poor resistance to high temperature and high salinity.This study develops a functionalized nanographite system(the MEGO system)with superior high-temperature dispersibility and thermosalinity-responsive capability through polyether amine(PEA)grafting and noncovalent interactions with disodium naphthalene sulfonate(DNS)molecules.The grafted PEA and DNS provide steric hindrance and electrostatic repulsion,enhancing thermal and salinity resistance.After ten days of aggregation,the MEGO system forms stable particle aggregates(55.51-61.80 lm)that are suitable for deep reservoir migration and profile control.Both experiments and simulations reveal that particle size variations are synergistically controlled by temperature and salt ions(Na^(+),Ca^(2+),and Mg^(2+)).Compared with monovalent ions,divalent ions promote nanographite aggregation more strongly through double-layer compression and bridging effects.In core displacement experiments,the MEGO system demonstrated superior performance in reservoirs with permeabilities ranging from 21.6 to 103 mD.The aggregates formed within the pore throats significantly enhanced flow resistance,expanded the sweep volume,and increased the overall oil recovery to 56.01%.This research indicates that the MEGO system holds excellent potential for EOR in deep oil reservoirs.展开更多
Glycyrrhetinic acid(GA)sheds new light on liver-targeted therapy due to high-specific accumulation to GA receptors in liver,however,the limitation of commonly used macromolecular GA modification approaches as well as ...Glycyrrhetinic acid(GA)sheds new light on liver-targeted therapy due to high-specific accumulation to GA receptors in liver,however,the limitation of commonly used macromolecular GA modification approaches as well as the application gap across various vector have constrained its use.In this study,we proposed a novel perspective to break out,disulfide bonds(SS)were employed as linkage to facilitate GA modification,which allowed further connections with various carriers,while provided additional glutathione(GSH)-responsive property.The superiority of GA-disulfide conjunction was validated using mesoporous silica nanoparticles(MSN)as model carriers,chemotherapeutic drug(doxorubicin)and photosensitizer(indocyanine green)were loaded into MSN-SS-GA to further achieve chemo-photothermal synergistic anti-tumor therapy.Based on results from multiple evaluations,the GA-disulfide drafted MSN(DI/MSN-SS-GA)demonstrated expected liver tumor targeting effect and exhibited GSH-stimuli release property to reduce preleakage.Taken together,this study presents an effective chemo-photothermal therapy for liver cancer(88.26%),offers a potential,robust and straightforward strategy on GA application for enhancing liver targeting therapy.展开更多
Rapid advances in thermal management technology and the increasing need for multi-energy conversion have placed stringent energy efficiency requirements on next-generation shape-stable composite phase change materials...Rapid advances in thermal management technology and the increasing need for multi-energy conversion have placed stringent energy efficiency requirements on next-generation shape-stable composite phase change materials(PCMs).Magnetically-responsive phase change thermal storage materials are considered an emerging concept for energy storage systems,enabling PCMs to perform unprecedented functions(such as green energy utilization,magnetic thermotherapy,drug release,etc.).The combination of multifunctional magnetic nanomaterials and PCMs is a milestone in the creation of advanced multifunctional composite PCMs.However,a timely and comprehensive review of composite PCMs based on magnetic nanoparticle modification is still missing.Herein,we furnish an exhaustive exposition elucidating the cutting-edge advancements in magnetically responsive composite PCMs.We delve deeply into the multifarious roles assumed by distinct nanoparticles within composite PCMs of varying dimensions,meticulously scrutinizing the intricate interplay between their architectures and thermophysical attributes.Moreover,we prognosticate future research trajectories,delineate alternative stratagems,and illuminate prospective avenues.This review is intended to stimulate broader academic interest in interdisciplinary fields and provide valuable insights into the development of next-generation magnetically-responsive composite PCMs.展开更多
Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this ...Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron reagent.Facile thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory performance.The thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of thiols.Moreover,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL materials.In addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.展开更多
Tumor microenvironment-responsive drug self-delivery systems utilize tumor microenvironment-responsive chemical bonds to link anti-tumor drugs,exploiting the hydrophilic and hydrophobic properties of different drugs t...Tumor microenvironment-responsive drug self-delivery systems utilize tumor microenvironment-responsive chemical bonds to link anti-tumor drugs,exploiting the hydrophilic and hydrophobic properties of different drugs to form amphiphilic prodrug molecules with self-assembly characteristics.Upon stimulation by specific factors in the tumor microenvironment,these amphiphilic prodrug molecules can release drugs at precise sites within the tumor.These strategies significantly increase the drug concentration at the tumor site while effectively reducing the damage of anti-cancer drugs to normal tissues.Owing to the advanced delivery strategies such as synergistic administration and controlled drug release,tumor microenvironment-responsive drug self-delivery systems hold great potential for treating malignant tumors with multidrug resistance(MDR).At the same time,the stimulus-reactivity of metal complexes provides an important opportunity to design site-specific prodrugs that can maximize therapeutic efficacy while minimizing adverse side effects of metal drugs.This innovative drug design complements the tumor microenvironment-responsive self-delivery system,providing more feasible therapeutic strategies and possibilities in the field of cancer therapy and drug delivery.This work provides a comprehensive review of recent advancements in drug self-delivery systems,offering insights into their potential applications in cancer therapy and MDR reversal.展开更多
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 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 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 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supported by Natural Science Foundation of Jilin Province(No.SKL202302002)Key Research and Development project of Jilin Provincial Science and Technology Department(No.20210204142YY)+2 种基金The Science and Technology Development Program of Jilin Province(No.2020122256JC)Beijing Kechuang Medical Development Foundation Fund of China(No.KC2023-JX-0186BQ079)Talent Reserve Program(TRP),the First Hospital of Jilin University(No.JDYY-TRP-2024007)。
文摘Prostate cancer(PCa)is characterized by high incidence and propensity for easy metastasis,presenting significant challenges in clinical diagnosis and treatment.Tumor microenvironment(TME)-responsive nanomaterials provide a promising prospect for imaging-guided precision therapy.Considering that tumor-derived alkaline phosphatase(ALP)is over-expressed in metastatic PCa,it makes a great chance to develop a theranostics system with ALP responsive in the TME.Herein,an ALP-responsive aggregationinduced emission luminogens(AIEgens)nanoprobe AMNF self-assembly was designed for enhancing the diagnosis and treatment of metastatic PCa.The nanoprobe exhibited self-aggregation in the presence of ALP resulted in aggregation-induced fluorescence,and enhanced accumulation and prolonged retention period at the tumor site.In terms of detection,the fluorescence(FL)/computed tomography(CT)/magnetic resonance(MR)multi-mode imaging effect of nanoprobe was significantly improved post-aggregation,enabling precise diagnosis through the amalgamation of multiple imaging modes.Enhanced CT/MR imaging can achieve assist preoperative tumor diagnosis,and enhanced FL imaging technology can achieve“intraoperative visual navigation”,showing its potential application value in clinical tumor detection and surgical guidance.In terms of treatment,AMNF showed strong absorption in the near infrared region after aggregation,which improved the photothermal treatment effect.Overall,our work developed an effective aggregation-enhanced theranostic strategy for ALP-related cancers.
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.
基金supported by the National Natural Sciences Foundation of China(Grant Nos.:31971308 and 81960769)Science and Technology Plan Project of Shihezi University,China(Grant No.:2023AB047)+2 种基金National S&T Major Project,China(Grant No.:2019ZX09301-147)Luzhou Science and Technology Plan,China(Grant No.:2018CDLZ-10)Sichuan Science and Technology Program,China(Grant No.:2021YFS0081).
文摘Melanoma,a common malignant skin tumor,faces challenges with multidrug resistance and high recurrence rates.Combining photodynamic therapy(PDT)and immunotherapy offers a promising personalized treatment approach.However,poor water solubility and significant side effects of photosensitizers and immune checkpoint inhibitors(ICIs)limit their application.Enhancing delivery efficiency while reducing adverse effects is crucial.Herein,we formulate BM@HSSC nanoparticles(NPs),which consist of a reduction-responsive hyaluronic acid(HA)backbone modified with photosensitizer chlorin e6(Ce6)and loaded with the programmed cell death-ligand 1(PD-L1)inhibitor BMS-1.This system synergistically integrates PDT,immunogenic cell death(ICD),and immunotherapy for melanoma treatment.BM@HSSC NPs target and accumulate at the tumor site via the CD44 receptor.The disulfide bonds(-S-S-)in the NPs react with high glutathione(GSH)concentrations in tumor cells,rapidly releasing Ce6 and BMS-1.Under 660 nm laser irradiation,BM@HSSC NPs generate cytotoxic reactive oxygen species(ROS),inducing cell apoptosis and triggering ICD via PDT damage-associated molecular patterns(DAMPs)and tumor-associated antigens(TAAs)released from ICD promote dendritic cell(DC)maturation,enhancing antigen presentation and activating cytotoxic T lymphocytes(CTLs).Meanwhile,BMS-1 blocks the programmed cell death-1(PD-1)/PD-L1 pathway,countering the immunosuppressive tumor microenvironment(iTME)and inhibiting tumor cell immune escape.This strategy amplifies antitumor immune responses by enhancing immunogenicity and synergizing with ICIs,resulting in robust antitumor efficacy.
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 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financially supported by Shanghai Pujiang Program 23PJ1406500.
文摘Black wings of butterfly Ornithoptera goliath and infrared-band radiative cooling function of Rapala dioetas butterfly wings are associated with black pigment(e.g.,melanin)and unique hierarchical micro/nanostructures,greatly stimulating biomimetic fabrication of functional photonic structures but mainly targeted to one prototype.Targeted at two-prototype integrated biomimetic fabrication from fully compositional/structural/functional aspects,femtosecond(fs)laser subtractive/additive-integrated hierarchical micro/nano-manufacturing technique is proposed in this work.This technique can one-step transfer refractory metals(e.g.,W,Mo,Nb,Ta)into black non-stoichiometric oxide nanomaterials with abundant oxygen vacancies and simultaneously enable the realization of in situ quasi-controllable micro/nanoscale hierarchical aggregation and assembly,all displaying black color but with tunable infrared emission.Adjusting the scan interval for biomimetic manufacturing can tailor the structural oxidation degree,the emission in the long-wave infrared(LWIR)band while keeping the blackness of hierarchical aggregates,and the confined height between the covering quartz plate and the ablated sample.The blackening efficiency of this technique can reach∼11.25 cm^(2)·min^(−1),opening opportunities for high-throughput optical/thermal applications.Selectively patterned Chinese characters,Arabic numbers,and English letters are easily fabricable,which are intrinsically invisible-infrared dual-band encrypted but decryptable via static/dynamic environment stimuli(e.g.,sample heating/cooling,introducing external hot/cold sources including human hands).The self-evolution from‘orderless’structuring to‘ordered’functionalization is validated for the proposed fs laser subtractive/additive-integrated biomimetic manufacturing,specifically from the synthesis of diverse black nanomaterials and the seemingly disordered micro/nano-aggregates to the ordered optical/thermal regulation capacities for a delicate modulation of information encryption and decryption,unveiling a new concept for future exploration and extension.
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JSPS Research Fellowships for Young Scientistssupported in part by JST SPRING,Japan(Nos.JPMJSP2106 and JPMJSP2180,Takuya Tanaka.and Yuki Sawatari.)+1 种基金MEXT/JSPS KAKENHI grants(No.23H02036,Gen-ichi Konishi)Murata Science and Education Foundation(Gen-ichi Konishi)。
文摘Aggregation-induced emission luminogens(AIEgens)exhibit viscosity-responsive behavior resembling those of molecular rotors;however,their response mechanisms are more complex and cannot be adequately described using simple rotational models.AIEgens demonstrate intricate dynamics that are highly dependent on their molecular structures.In this study,we synthesized water-soluble derivatives of representative AIEgens,including tetraphenylethene(TPE),bis(N,N-dialkylamino)anthracene(BDAA),and bridged stilbene,and systematically investigated the dependence of their photophysical properties in water/glycerol mixed solvents on temperature and viscosity.To elucidate the origin of their viscosity responsiveness,quantum chemical calculations were conducted to analyze their potential energy surfaces(PESs).The results revealed that compared to typical molecular rotors,these AIEgens exhibit significantly higher sensitivity to viscosity in low-viscosity regions.Notably,for TPE and BDAA derivatives,the viscosity responsiveness was found to be governed not by the activation energy barrier(ΔE_(a))based on the PES,but rather by the viscosity-dependent constraints on molecular structural changes.Furthermore,molecules possessing multiple aromatic rings or large,flexible,rotatable moieties were found to exhibit enhanced sensitivity to viscosity due to increased frictional interactions in solutions.This study provides critical insights into the mechanistic origins of the viscosity responsiveness of AIEgens,thereby advancing the fundamental understanding of their behavior and expanding their potential application as viscositysensitive probes.
基金supported by the General Program of the National Natural Science Foundation of China(52074335)the National Key Research and Development Program of China(2022YFE0129900 and 2019YFA0708700)+1 种基金the Fundamental Research Funds for the Central Universities(23CX07003A)the Special Funding Program for the Operational Expenses of National Research Institutions(SKLDOG2024-ZYRC-01).
文摘In deep oil reservoir development,enhanced oil recovery(EOR)techniques encounter significant challenges under high-temperature and high-salinity conditions.Traditional profile-control agents often fail to maintain stable blocking under extreme conditions and exhibit poor resistance to high temperature and high salinity.This study develops a functionalized nanographite system(the MEGO system)with superior high-temperature dispersibility and thermosalinity-responsive capability through polyether amine(PEA)grafting and noncovalent interactions with disodium naphthalene sulfonate(DNS)molecules.The grafted PEA and DNS provide steric hindrance and electrostatic repulsion,enhancing thermal and salinity resistance.After ten days of aggregation,the MEGO system forms stable particle aggregates(55.51-61.80 lm)that are suitable for deep reservoir migration and profile control.Both experiments and simulations reveal that particle size variations are synergistically controlled by temperature and salt ions(Na^(+),Ca^(2+),and Mg^(2+)).Compared with monovalent ions,divalent ions promote nanographite aggregation more strongly through double-layer compression and bridging effects.In core displacement experiments,the MEGO system demonstrated superior performance in reservoirs with permeabilities ranging from 21.6 to 103 mD.The aggregates formed within the pore throats significantly enhanced flow resistance,expanded the sweep volume,and increased the overall oil recovery to 56.01%.This research indicates that the MEGO system holds excellent potential for EOR in deep oil reservoirs.
基金funded by Research Project of Department of Education of Liaoning Province(No.LJKMZ20221363,China)。
文摘Glycyrrhetinic acid(GA)sheds new light on liver-targeted therapy due to high-specific accumulation to GA receptors in liver,however,the limitation of commonly used macromolecular GA modification approaches as well as the application gap across various vector have constrained its use.In this study,we proposed a novel perspective to break out,disulfide bonds(SS)were employed as linkage to facilitate GA modification,which allowed further connections with various carriers,while provided additional glutathione(GSH)-responsive property.The superiority of GA-disulfide conjunction was validated using mesoporous silica nanoparticles(MSN)as model carriers,chemotherapeutic drug(doxorubicin)and photosensitizer(indocyanine green)were loaded into MSN-SS-GA to further achieve chemo-photothermal synergistic anti-tumor therapy.Based on results from multiple evaluations,the GA-disulfide drafted MSN(DI/MSN-SS-GA)demonstrated expected liver tumor targeting effect and exhibited GSH-stimuli release property to reduce preleakage.Taken together,this study presents an effective chemo-photothermal therapy for liver cancer(88.26%),offers a potential,robust and straightforward strategy on GA application for enhancing liver targeting therapy.
基金financially supported by the National Natural Science Foundation of China(No.51902025).
文摘Rapid advances in thermal management technology and the increasing need for multi-energy conversion have placed stringent energy efficiency requirements on next-generation shape-stable composite phase change materials(PCMs).Magnetically-responsive phase change thermal storage materials are considered an emerging concept for energy storage systems,enabling PCMs to perform unprecedented functions(such as green energy utilization,magnetic thermotherapy,drug release,etc.).The combination of multifunctional magnetic nanomaterials and PCMs is a milestone in the creation of advanced multifunctional composite PCMs.However,a timely and comprehensive review of composite PCMs based on magnetic nanoparticle modification is still missing.Herein,we furnish an exhaustive exposition elucidating the cutting-edge advancements in magnetically responsive composite PCMs.We delve deeply into the multifarious roles assumed by distinct nanoparticles within composite PCMs of varying dimensions,meticulously scrutinizing the intricate interplay between their architectures and thermophysical attributes.Moreover,we prognosticate future research trajectories,delineate alternative stratagems,and illuminate prospective avenues.This review is intended to stimulate broader academic interest in interdisciplinary fields and provide valuable insights into the development of next-generation magnetically-responsive composite PCMs.
基金financially supported by the National Natural Science Foundation of China(No.22171182)Sichuan Tianfu Emei Plan.
文摘Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron reagent.Facile thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory performance.The thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of thiols.Moreover,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL materials.In addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.
基金supported by the National Natural Science Foundation of China(No.21907059)Shandong Province Chinese Medicine Science and Technology Development Project(No.M-2022258)+1 种基金the Young Scientist Development Foundation of Shandong First Medical University(No.202201-002)the Academic Promotion Program of Shandong First Medical University(Nos.2019LJ003 and 2019QL011).
文摘Tumor microenvironment-responsive drug self-delivery systems utilize tumor microenvironment-responsive chemical bonds to link anti-tumor drugs,exploiting the hydrophilic and hydrophobic properties of different drugs to form amphiphilic prodrug molecules with self-assembly characteristics.Upon stimulation by specific factors in the tumor microenvironment,these amphiphilic prodrug molecules can release drugs at precise sites within the tumor.These strategies significantly increase the drug concentration at the tumor site while effectively reducing the damage of anti-cancer drugs to normal tissues.Owing to the advanced delivery strategies such as synergistic administration and controlled drug release,tumor microenvironment-responsive drug self-delivery systems hold great potential for treating malignant tumors with multidrug resistance(MDR).At the same time,the stimulus-reactivity of metal complexes provides an important opportunity to design site-specific prodrugs that can maximize therapeutic efficacy while minimizing adverse side effects of metal drugs.This innovative drug design complements the tumor microenvironment-responsive self-delivery system,providing more feasible therapeutic strategies and possibilities in the field of cancer therapy and drug delivery.This work provides a comprehensive review of recent advancements in drug self-delivery systems,offering insights into their potential applications in cancer therapy and MDR reversal.
