Conventional hard carbon anodes,despite their high sodium storage capacity,suffer from two major limitations:sluggish ion diffusion kinetics due to tortuous micropore networks and significant volume expansion arising ...Conventional hard carbon anodes,despite their high sodium storage capacity,suffer from two major limitations:sluggish ion diffusion kinetics due to tortuous micropore networks and significant volume expansion arising from disordered carbon structures.These inherent defects collectively compromise rate capability and cycling stability.Herein,we devise a graphene oxide(GO)-directed templating approach to architect zeolitic imidazolate framework(ZIF)-derived carbon into a hierarchical nanoflower superstructure with radially aligned meso/macroporous nanosheets.This superstructure integrates three synergistic features:three-dimensional interconnected channels and graphitic domains enabling fast ion/electron transport,radially aligned nanosheets maximizing electrode-electrolyte contact while accommodating volume expansion,and nitrogen-doped defect sites providing preferential redox-active centers for sodium storage.The optimized ZIF-9@GO-6 achieves a high specific capacity of 521.8 mAh·g-1at 0.05 A·g-1with an initial Coulombic efficiency of 89.2%,and retains a specific capacity of 298.2 mAh·g-1after 500 cycles.This GO-directed morphological engineering strategy effectively resolves the intrinsic trade-offs between porosity,conductivity,and structural stability in conventional hard carbon anodes,paving the way for scalable,high-performance sodium-ion batteries.展开更多
Rationally design the morphology and structure of electroactive nanomaterials is an effective approach to enhance the performance of aqueous batteries.Herein,we co-engineered the hollow architecture and interlayer spa...Rationally design the morphology and structure of electroactive nanomaterials is an effective approach to enhance the performance of aqueous batteries.Herein,we co-engineered the hollow architecture and interlayer spacing of layered double hydroxides(LDH)to achieve high electrochemical activity.The hierarchical hollow LDH was prepared from bimetallic zeolitic imidazolate frameworks(ZIF)by a facile cation exchange strategy.Zn and Cu elements were selected as the second metals incorporated in Co-ZIF.The characteristics of the corresponding derivatives were studied.Besides,the transformation mechanism of CoZn-ZIF into nanosheet-assembled hollow Co Zn Ni LDH(denoted as CoZnNi-OH)was systematically investigated.Importantly,the interlayer spacing of CoZnNi-OH expands due to Zn2+incorporation.The prepared CoZnNi-OH offers large surface area,exposed active sites,and rapid mass transfer/diffusion rate,which lead to a significant enhancement in the specific capacitance,rate performance,and cycle stability of CoZnNi-OH electrode.In addition,the aqueous alkaline CoZnNi-OH//Zn showed a maximum energy density/power density of 0.924 m Wh/cm2,8.479 m W/cm2.This work not only raises an insightful strategy for regulating the morphology and interlayer spacing of LDH,but also provides a reference of designing hollow nickel-based nanomaterials for aqueous batteries.展开更多
Biological nanotechnologies based on functional nanoplatforms have synergistically catalyzed the emergence of cancer therapies.As a subtype of metal-organic frameworks(MOFs),zeolitic imidazolate frameworks(ZIFs)have e...Biological nanotechnologies based on functional nanoplatforms have synergistically catalyzed the emergence of cancer therapies.As a subtype of metal-organic frameworks(MOFs),zeolitic imidazolate frameworks(ZIFs)have exploded in popularity in the field of biomaterials as excellent protective materials with the advantages of conformational flexibility,thermal and chemical stability,and functional controllability.With these superior properties,the applications of ZIF-based materials in combination with various therapies for cancer treatment have grown rapidly in recent years,showing remarkable achievements and great potential.This review elucidates the recent advancements in the use of ZIFs as drug delivery agents for cancer therapy.The structures,synthesis methods,properties,and various modifiers of ZIFs used in oncotherapy are presented.Recent advances in the application of ZIF-based nanoparticles as single or combination tumor treatments are reviewed.Furthermore,the future prospects,potential limitations,and challenges of the application of ZIF-based nanomaterials in cancer treatment are discussed.We except to fully explore the potential of ZIF-based materials to present a clear outline for their application as an effective cancer treatment to help them achieve early clinical application.展开更多
In this work,the synthesis of uniform zeolitic imidazolate framework-coated Mo-glycerate spheres and their subsequent conversion into hierarchical architecture containing bimetallic selenides heterostructures and nitr...In this work,the synthesis of uniform zeolitic imidazolate framework-coated Mo-glycerate spheres and their subsequent conversion into hierarchical architecture containing bimetallic selenides heterostructures and nitrogen-doped carbon shell are reported.Selenization temperature plays a significant role in determining the phases,morphology,and lithium-ion storage performance of the composite.Notably,the optimal electrode demonstrates an ultrahigh reversible capacity of 1298.2 mAh/g after 100 cycles at 0.2 A/g and an outstanding rate capability with the capacity still maintained 505.7 mAh/g after 300 cycles at 1.0 A/g,surpassing the calculated theoretical capacity according to individual component and most of the reported MoSe@C-or ZnSe@C-based anodes.Furthermore,ex-situ X-ray diffraction patterns reveal the combined conversion and alloying reaction mechanisms of the composite.展开更多
Suboptimal treatment of laryngeal squamous cell carcinoma(LSCC)provides poor survival rate.The poor bioavailability,resistance to cetuximab(Cet),and the instability of small interfering RNA(siRNA)limit their efficacy ...Suboptimal treatment of laryngeal squamous cell carcinoma(LSCC)provides poor survival rate.The poor bioavailability,resistance to cetuximab(Cet),and the instability of small interfering RNA(siRNA)limit their efficacy in LSCC therapy.The present study has been aimed to develop a Cet and focal adhesion kinase(FAK)siRNA(siFAK)co-delivery nanosystem.Zeolitic imidazolate framework-8(ZIF-8),with its large specific surface area and pH-responsive properties,is an ideal delivery carrier allowing controlled drug release in the acidic tumor microenvironment.Therefore,Cet was loaded onto ZIF-8 and encapsulated in a TU177 cell membrane(TCM)after the electrostatic adsorption of siFAK.Fourier transform infrared(FTIR)spectroscopy,transmission electron microscopy(TEM),scanning electron microscopy(SEM),zeta potential,X-ray diffraction,and particle size analyses were deployed to characterize Cet/siFAK@ZIF-8@TCM.TU177 cells and subcutaneously transplanted tumor-bearing nude mice were used to evaluate the intracellular uptake,cytotoxicity,in vivo biocompatibility,biodistribution,biosafety,pH responsiveness,and anti-LSCC efficacy of Cet/siFAK@ZIF-8@TCM.After ZIF-8@TCM were loaded with Cet and siFAK,alterations in their physical and crystal structures,particle size,and zeta potential were observed.Meanwhile,the co-delivery system increased the loading of Cet through the electrostatic adsorption of siFAK to Cet-loaded ZIF-8.The intracellular uptake of Cet/siFAK@ZIF-8@TCM also protected siFAK from degradation,effectively decreasing the messenger RNA(mRNA)and protein expression levels of FAK in LSCC cells.The ZIF-8@TCM nanosystem for co-delivery of Cet and siFAK exhibited pH-responsiveness and tumor-targeting capabilities,thereby exerting anti-LSCC effects.Co-delivery of Cet and siFAK via the pH-responsive ZIF-8@TCM system enabled the targeted release of the chemotherapeutic and gene,in turn maximizing their anti-LSCC effect while ensuring biosafety.展开更多
A zeolite imidazolate framework,ZIF-8,was synthesized and characterized by dynamic laser light scattering,X-ray powder diffraction,scanning electron microscopy,transmission electron microscopy,thermogravimetric analys...A zeolite imidazolate framework,ZIF-8,was synthesized and characterized by dynamic laser light scattering,X-ray powder diffraction,scanning electron microscopy,transmission electron microscopy,thermogravimetric analysis,Fourier transform infrared,atomic absorption spectrophotometry,and nitrogen adsorption measurements.The ZIF-8 was highly crystalline and porous with a surface area of over 1600 m2/g.Friedel-Crafts acylation of anisole and benzoyl chloride proceeded well in the presence of ZIF-8(2-6 mol%)without the need for an inert atmosphere.The reaction afforded a selectivity of 93%-95%to the p-isomer.The solid catalyst can be separated from the reaction mixture by simple centrifugation and reused without significant degradation in catalytic activity.There was no leaching of active acid species into the reaction solution.展开更多
Metal-organic frameworks(MOFs)have been intensely studied for the past few decades as an enormous family of highly tunable porous materials with promisingly applicable functionalities in adsorption,separation,catalysi...Metal-organic frameworks(MOFs)have been intensely studied for the past few decades as an enormous family of highly tunable porous materials with promisingly applicable functionalities in adsorption,separation,catalysis,sensing,electrochemistry,and a great number of emerging purposes.As a classic MOF,zeolitic imidazolate framework-8(ZIF-8)is conventionally one of the very few MOF members that has been commercialized with considerable production.展开更多
Zeolitic imidazolate frameworks(ZIFs)as smart drug delivery systems with microenvironment-triggered release have attracted much attention for tumor therapy.However,the exploration of ZIFs in biomedicine still encounte...Zeolitic imidazolate frameworks(ZIFs)as smart drug delivery systems with microenvironment-triggered release have attracted much attention for tumor therapy.However,the exploration of ZIFs in biomedicine still encounters many issues,such as inconvenient surface modification,fast drug release during blood circulation,undesired damage to major organs,and severe in vivo toxicity.To address the above issues,we developed an Mn-ZIF-90 nanosystem functionalized with an originally designed active-targeting and pH-responsive magnetic resonance imaging(MRI)Y1 receptor ligand[Asn28,Pro30,Trp32]-NPY(25-36)for imaging-guided tumor therapy.After Y1 receptor ligand modification,the Mn-ZIF-90 nanosystem exhibited high drug loading,better blood circulation stability,and dual breast cancer cell membrane and mitochondria targetability,further favoring specific microenvironment-triggered tumor therapy.Meanwhile,this nanosystem showed promising T1-weighted magnetic resonance imaging contrast in vivo in the tumor sites.Especially,this nanosystem with fast clean-up had almost no obvious toxicity and no damage occurred to the major organs in mice.Therefore,this nanosystem shows potential for use in imaging-guided tumor therapy.展开更多
The development of a simple and facile synthesis route is a highly desirable but challenging process in the fabrication of nanoscale hierarchical porous zeolitic imidazolate frameworks(ZIFs).Herein we describe a facil...The development of a simple and facile synthesis route is a highly desirable but challenging process in the fabrication of nanoscale hierarchical porous zeolitic imidazolate frameworks(ZIFs).Herein we describe a facile method for rapidly synthesizing hierarchically porous ZIF-90 nanocrystals(particle sizes of~300 nm)using hydroxyl double salts as intermediates at room temperature.The as-synthesized ZIF-90 contained hierarchical porous structures developed using a crystalline interior and a random stack of multiple nanoparticles.Both the morphology and particle size of ZIF-90 nanocrystals could be tuned by controlling the molar ratio of ICA/Zn2+.Note that the as-synthesized hierarchically porous ZIF-90 nanocrystals exhibited higher thermal stability compared with the conventional ZIF-90.Because of the introduction of hierarchical porous structures,the resultant hierarchically porous ZIF-90 nanocrystals showed enhanced toluene adsorption capacity than those of conventional metal organic frameworks and zeolites.展开更多
Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowi...Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowing wearable electronics. Herein, we report a flexible bifunctional oxygen catalyst thin film consisting of Co–N–C bifunctional catalysts embedding in carbon nanotube(CNT) networks. The catalyst is readily prepared by pyrolysis of cobalt-based zeolitic imidazolate frameworks(ZIF-67) that are in-situ synthesized in CNT networks. Such catalyst film demonstrates very high catalytic activities for oxygen reduction(onset potential: 0.91 V, and half-wave potential: 0.87 V vs. RHE) and oxygen evolution(10 m Acm^-2 at 1.58 V) reactions, high methanol tolerance property, and long-term stability(97% current retention). Moreover, our integrated catalyst film shows very good structure flexibility and robustness. Based on the obtained film air electrodes, flexible Zn–air batteries demonstrate low charging and discharging overpotentials(0.82 V at 1 m A cm^-1) and excellent structure stability in the bending tests. These results indicate that presently reported catalyst films are potential air electrodes for flexible metal–air batteries.展开更多
Although zeolitic imidazolate frameworks(ZIFs)have bright prospects in wide fields like gas storage/separation,catalysis and medicine,etc.,their large-scale applications are bottlenecked by the absence of their low-co...Although zeolitic imidazolate frameworks(ZIFs)have bright prospects in wide fields like gas storage/separation,catalysis and medicine,etc.,their large-scale applications are bottlenecked by the absence of their low-cost commercial production technique.Here,we report an uncon ventional method suitable for environmentally friendly and low-cost mass-production of ZIFs.In this method,taking the synthesis of ZIF-8 as an example,ZnO was used instead of Zn(NO3)2 in traditional solvent synthesis methods and CO2 was introduced to dissolve ZnO in aqueous solution of 2-methylimidazole(HMeim)and form water soluble salt([ZnMeim]+[MeimCOO]-)at room temperature.Then,by removing CO2 through heating or vacuuming,Meim-ions are produced and instantaneously assemble with[ZnMeim]+s to generate ZIF-8 without any by product.Due to the absence of strong acid anions(such as NO-3 and Cl- et al.)in solution,the washing of filter cake required in the conventional approaches could be omitted and the filtrate containing only water and HMeim could be reused completely.This method is really green as no waste gas or liquid generates because CO2 and water could be recycled perfectly.It overcomes almost all bottlenecks occurred in commercial production of ZIF-8 when using traditional methods.A pilot plant was established for mass-production of ZIF-8 and hundreds kilograms of ZIF-8 was produced,which indicates that the new method is not only environmentally friendly but also low cost and commercial accessibility.It is expected that the new method would open an avenue for commercial applications of ZIFs.展开更多
As a prevailing cathode material of lithium-ion batteries(LIBs),LiCoO2(LCO)still encounters the tricky problems of structural collapse,whose morphological engineering and cation doping are crucial for surmounting t...As a prevailing cathode material of lithium-ion batteries(LIBs),LiCoO2(LCO)still encounters the tricky problems of structural collapse,whose morphological engineering and cation doping are crucial for surmounting the mechanical strains and alleviating phase degradation upon cycling.Hereinafter,we propose a strategy using a zeolitic imidazolate framework(ZIF)as the self-sacrificing template to directionally prepare a series of LiNi0.1Co0.9O2(LNCO)with tailorable electrochemical properties.The rational selection of sintering temperature imparts the superiority of the resultant products in lithium storage,during which the sample prepared at 700℃(LNCO-700)outperforms its counterparts in cyclability(156.8 mA h g-1at 1 C for 200 cycles in half cells,1 C=275 mA g-1)and rate capability due to the expedited ion/electron transport and the strengthen mechanical robustness.The feasibility of proper Ni doping is also divulged by half/full cell tests and theoretical study,during which LNCO-700(167 mA h g-1at 1 C for 100 cycles in full cells)surpasses LCO-700 in battery performance due to the mitigated phase deterioration,stabilized layered structu re,ameliorated electro nic co nductivity,a nd exalted lithium sto rage activity.This work systematically unveils tailorable electrochemical behaviors of LNCO to better direct their practical application.展开更多
Freestanding carbon nanofibers loaded with bimetallic hollow nanocage structures were synthesized.The nanocages inherited the rhombic dodecahedral morphology of the zeolitic imidazolate framework(ZIF)precursors,ZIF-8 ...Freestanding carbon nanofibers loaded with bimetallic hollow nanocage structures were synthesized.The nanocages inherited the rhombic dodecahedral morphology of the zeolitic imidazolate framework(ZIF)precursors,ZIF-8 and ZIF-67.As anode materials for lithium-ion batteries(LIBs),the bimetallic nanocage-loaded freestanding carbon nanofibers effectively buffered volume expansions and alleviated pulverization through their different reduction and oxidation potentials.The higher capacities of the composite anodes arose via the formation of the LixZn alloy and Li2O by Zn and Co ions,respectively,and the enhanced conductivity conferred by the carbon nanofibers.A synergistic effect of the composite components toward the strong electrochemical performance(688 m A h·g-1at 1200 m A·g-1)of the bimetallic nanocage-loaded fibers was demonstrated through the superior long-term stability of the anode(1048 m A h·g-1after 300 cycles at 100 m A·g-1),suggesting that the fabricated anode can be a promising material for use in portable LIBs.展开更多
The use of intumescent flame retardants(IFRs)is considered an environmentally friendly and cost-effective strategy to suppress potential fire hazards from synthetic polymers.However,some conventional IFRs are neither ...The use of intumescent flame retardants(IFRs)is considered an environmentally friendly and cost-effective strategy to suppress potential fire hazards from synthetic polymers.However,some conventional IFRs are neither efficient in developing a thermally stable char layer nor reducing the release of toxic byproducts during polymer combustion.In this work,we aim to discuss the effects of zeolitic imidazolate frameworks(ZIFs)on synergistically improving the flame retardancy behaviors in polypropylene(PP)composites,including thermal degradation(evolved gas analysis),free radical reactions in the gaseous phase(in-situ chemiluminescent image analysis),and carbonaceous structure in the condensed phase(micro-morphology and composition analysis).It is found that the transition metals in ZIFs can catalytically accelerate the crosslinking reaction at a lower initial temperature and decrease the amount of hydrocarbon volatiles in the gaseous phase.Once ignited,the embedded ZIFs can firstly bridge adjacent phosphorus chains in the polymer matrix to expand crosslinking degrees and then they are anchored in the developed N-doped phospho-carbonaceous networks after pyrolysis.As a result,more compact char residue structures are observed in the condensed phase for ZIF-reinforced composites.For example,by replacing 2 wt%of IFR with ZIF-67,the peak heat release rate,peak smoke production rate,and peak CO production rate are reduced by 69%,80%,and 72%,respectively,when compared to the conventional composite.These results indicate an excellent solution to resolve inherent fire hazards associated with IFRs in polymers and achieve necessary efficiency for industrial applications.It also provides a new strategy for determining flammability characteristics and combustion mechanisms of polymer composites using in-situ chemiluminescence analysis.展开更多
Two new boron imidazolate frameworks(BIFs),Zn2[HBH(2-mim)3]2(1,2-PEA)2(EG)2(BIF-120,EG=ethylene glycol)and Zn[BH(2-mim)3](1,2-HPEA)(BIF-121),were successfully synthesized by mixing the KBH(2-mim)3 ligand and the semir...Two new boron imidazolate frameworks(BIFs),Zn2[HBH(2-mim)3]2(1,2-PEA)2(EG)2(BIF-120,EG=ethylene glycol)and Zn[BH(2-mim)3](1,2-HPEA)(BIF-121),were successfully synthesized by mixing the KBH(2-mim)3 ligand and the semirigid aromatic dicarboxylate ligand 1,2-benzenediacetic acid(1,2-H2PEA)under solvothermal conditions.In this paper,the two samples were structurally characterized by single-crystal X-ray diffraction and tested by infrared spectroscopy(IR),UV-visible spectroscopy(UV-Vis),thermogravimetric analysis TGA and X-ray powder diffractions.In addition,the solid-state luminescent properties of these crystals were also investigated.展开更多
Layered assembled membranes of 2D leaf-like zeolitic imidazolate frameworks(ZIF-L)nanosheets have received great attention in the field of water treatment due to the porous structure and excellent antibacterial abilit...Layered assembled membranes of 2D leaf-like zeolitic imidazolate frameworks(ZIF-L)nanosheets have received great attention in the field of water treatment due to the porous structure and excellent antibacterial ability,but the dense accumulation on the membrane surface and the low permeate flux greatly hinder their application.Herein,we synthesized m HNTs(modified halloysite nanotubes)/ZIF-L nanocomposites on modified m HNTs by in situ growth method.Interestingly,due to the different size of m HNTs and ZIF-L,m HNTs were packed in ZIF-L nanosheets.The hollow m HNTs provided additional transport channels for water molecules,and the accumulation of the ZIF-L nanosheets was decreased after assembling m HNTs/ZIF-L nanocomposites into membrane by filtration.The prepared m HNTs/ZIF-L membrane presented high permeate flux(59.6 L·m-2·h-1),which is 2-4 times of the ZIF-L membranes(14.8 L·m-2·h-1).Moreover,m HNTs/ZIF-L membranes are intrinsically antimicrobial,which exhibit extremely high bacterial resistance.We provide a controllable strategy to improve 2D ZIF-L assembles,and develops novel membranes using 2D package structure as building units.展开更多
To find potential zeolitic imidazolate frameworks(ZIFs)for CO2capture from flue gas,we built 169,898 ZIF models from 84,949 hypothetical zeolite networks.By calculating their lattice energies,accessible volumes to ...To find potential zeolitic imidazolate frameworks(ZIFs)for CO2capture from flue gas,we built 169,898 ZIF models from 84,949 hypothetical zeolite networks.By calculating their lattice energies,accessible volumes to CO2,the isosteric adsorption heat(Qst)of H2 O,Henry’s constant ratio(SKH)of CO2/N2,percent regenerability(R%),CO2working capacity(ΔN CO2),CO2/N2adsorption selectivity(S CO2/N2)and adsorbent performance score(APS),we identi fied 49 hydrophobic ZIF structures that might outplay already-realised ZIFs built from the same imidazolate linkers for CO2capture from flue gas.展开更多
A novel ZIF-8-CMC hybrid material was fabricated from the hybridization of ZIF-8 and carboxymethylcellulose(CMC) by impregnation method for n-hexane/3-methylpentane separation.The surface properties of ZIF-8 were tail...A novel ZIF-8-CMC hybrid material was fabricated from the hybridization of ZIF-8 and carboxymethylcellulose(CMC) by impregnation method for n-hexane/3-methylpentane separation.The surface properties of ZIF-8 were tailored by introducing CMC into ZIF-8 nanoparticles.In this work,adsorption separation of n-hexane(nHEX) and 3-methylpentane(3 MP) on ZIF-8-CMC were investigated by batch vapor-phase adsorption and liquid-phase breakthrough adsorption.The adsorption selectivity of nHEX/3 MP reversed from preferable adsorption of nHEX to preferable adsorption of 3 MP upon the increasing of CMC containing in the hybrid materials.As the temperature increases,the adsorption amounts of nHEX and 3 MP decrease.With the increasing of CMC contents,the nHEX uptake decreased,the uptake capacity of 3 MP increased gradually.For liquid-phase breakthrough adsorption,the dynamic adsorption capacity of nHEX also decreased with the increasing of temperature.展开更多
A novel flower-shaped zeolitic imidazolate framework(ZIF) doped organic-inorganic hybrid monolithic column(ZIF-HMC) was prepared by a simple sol-gel "one-step" method and utilized for efficient capillary mic...A novel flower-shaped zeolitic imidazolate framework(ZIF) doped organic-inorganic hybrid monolithic column(ZIF-HMC) was prepared by a simple sol-gel "one-step" method and utilized for efficient capillary microextraction(CME) of four brominated flame retardants.The prepared monolithic was characterized by Fourier transform infrared,scanning electron microscopy,X-ray photoelectron spectroscopy,energy disperse spectroscopy,and N2 adsorption-desorption.The parameters of CME were optimized by orthogonal array design.Under the optimal conditions,the ZIF-HMC showed excellent extraction efficiency,the limit of detection(LODs) and the limit of quantification(LOQs) were in the range of0.52$3.1 mg/L and 1.7$10 mg/L,respectively,and the proposed method demonstrated good recovery(88.8%–116.6%) with the RSD less than 13.6% and a reusability of at least 30 times.The ZIF-HMC possessed great potential for separating organic pollutants and the strategy used here could be extended to prepare other derivatized HMC functionalized monoliths.展开更多
Immunogenic antigen downregulation combined with an immunosuppressive tumor microenvironment(TME)remain major barriers to effective treatment of“cold”tumors.Here,we report a dual-functional nanotherapy that integrat...Immunogenic antigen downregulation combined with an immunosuppressive tumor microenvironment(TME)remain major barriers to effective treatment of“cold”tumors.Here,we report a dual-functional nanotherapy that integrates C70fullerene with hyaluronic acid(HA)–modified zeolitic imidazolate framework-8(ZIF-8)to enhance tumor immunogenicity and reprogram the TME.The resulting HA-C70@ZIF-8 nanocomposites exploit HAmediated CD44 targeting to promote selective tumor uptake and retention.Once internalized,acidic lysosomal conditions trigger Zn2+release from ZIF-8,causing ion overload,caspase-1 activation,gasdermin D cleavage,and pyroptotic tumor cell death accompanied by the release of damage-associated molecular patterns(DAMPs).Concurrently,encapsulated C70facilitates metabolic reprogramming of tumor-associated macrophages(TAMs)from an M2-to M1-like phenotype,thereby alleviating immunosuppression.Together,these mechanisms elicit robust immune activation and potentiate the efficacy of immune checkpoint blockade,offering a streamlined and impactful strategy for personalized tumor therapy and paving the way for novel approaches to highly effective immunotherapy.展开更多
基金supported by the National Natural Science Foundation of China(No.22478236)the Fundamental Research Program of Shanxi Province,China(No.202403021221146)。
摘要Conventional hard carbon anodes,despite their high sodium storage capacity,suffer from two major limitations:sluggish ion diffusion kinetics due to tortuous micropore networks and significant volume expansion arising from disordered carbon structures.These inherent defects collectively compromise rate capability and cycling stability.Herein,we devise a graphene oxide(GO)-directed templating approach to architect zeolitic imidazolate framework(ZIF)-derived carbon into a hierarchical nanoflower superstructure with radially aligned meso/macroporous nanosheets.This superstructure integrates three synergistic features:three-dimensional interconnected channels and graphitic domains enabling fast ion/electron transport,radially aligned nanosheets maximizing electrode-electrolyte contact while accommodating volume expansion,and nitrogen-doped defect sites providing preferential redox-active centers for sodium storage.The optimized ZIF-9@GO-6 achieves a high specific capacity of 521.8 mAh·g-1at 0.05 A·g-1with an initial Coulombic efficiency of 89.2%,and retains a specific capacity of 298.2 mAh·g-1after 500 cycles.This GO-directed morphological engineering strategy effectively resolves the intrinsic trade-offs between porosity,conductivity,and structural stability in conventional hard carbon anodes,paving the way for scalable,high-performance sodium-ion batteries.
基金supported by the National Natural Science Foundation of China(Nos.52371240,U1904215)Natural Science Foundation of Jiangsu Province(No.BK20200044)Changjiang scholars’program of the Ministry of Education(No.Q2018270)。
摘要Rationally design the morphology and structure of electroactive nanomaterials is an effective approach to enhance the performance of aqueous batteries.Herein,we co-engineered the hollow architecture and interlayer spacing of layered double hydroxides(LDH)to achieve high electrochemical activity.The hierarchical hollow LDH was prepared from bimetallic zeolitic imidazolate frameworks(ZIF)by a facile cation exchange strategy.Zn and Cu elements were selected as the second metals incorporated in Co-ZIF.The characteristics of the corresponding derivatives were studied.Besides,the transformation mechanism of CoZn-ZIF into nanosheet-assembled hollow Co Zn Ni LDH(denoted as CoZnNi-OH)was systematically investigated.Importantly,the interlayer spacing of CoZnNi-OH expands due to Zn2+incorporation.The prepared CoZnNi-OH offers large surface area,exposed active sites,and rapid mass transfer/diffusion rate,which lead to a significant enhancement in the specific capacitance,rate performance,and cycle stability of CoZnNi-OH electrode.In addition,the aqueous alkaline CoZnNi-OH//Zn showed a maximum energy density/power density of 0.924 m Wh/cm2,8.479 m W/cm2.This work not only raises an insightful strategy for regulating the morphology and interlayer spacing of LDH,but also provides a reference of designing hollow nickel-based nanomaterials for aqueous batteries.
基金National Natural Science Foundation of China(52073278)the“Medical Science+X”Cross-innovation Team of the Norman Bethune Health Science of Jilin University(2022JBGS10)+2 种基金the Jilin Province Science and Technology Development Program(20190201044JC20230101045JC)the Education Department of Jilin Province(JJKH20231205KJ).
摘要Biological nanotechnologies based on functional nanoplatforms have synergistically catalyzed the emergence of cancer therapies.As a subtype of metal-organic frameworks(MOFs),zeolitic imidazolate frameworks(ZIFs)have exploded in popularity in the field of biomaterials as excellent protective materials with the advantages of conformational flexibility,thermal and chemical stability,and functional controllability.With these superior properties,the applications of ZIF-based materials in combination with various therapies for cancer treatment have grown rapidly in recent years,showing remarkable achievements and great potential.This review elucidates the recent advancements in the use of ZIFs as drug delivery agents for cancer therapy.The structures,synthesis methods,properties,and various modifiers of ZIFs used in oncotherapy are presented.Recent advances in the application of ZIF-based nanoparticles as single or combination tumor treatments are reviewed.Furthermore,the future prospects,potential limitations,and challenges of the application of ZIF-based nanomaterials in cancer treatment are discussed.We except to fully explore the potential of ZIF-based materials to present a clear outline for their application as an effective cancer treatment to help them achieve early clinical application.
基金supported by the National Natural Science Foundation of China(No.22265017)the Open Fund of Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education(No.KF-21-04).
摘要In this work,the synthesis of uniform zeolitic imidazolate framework-coated Mo-glycerate spheres and their subsequent conversion into hierarchical architecture containing bimetallic selenides heterostructures and nitrogen-doped carbon shell are reported.Selenization temperature plays a significant role in determining the phases,morphology,and lithium-ion storage performance of the composite.Notably,the optimal electrode demonstrates an ultrahigh reversible capacity of 1298.2 mAh/g after 100 cycles at 0.2 A/g and an outstanding rate capability with the capacity still maintained 505.7 mAh/g after 300 cycles at 1.0 A/g,surpassing the calculated theoretical capacity according to individual component and most of the reported MoSe@C-or ZnSe@C-based anodes.Furthermore,ex-situ X-ray diffraction patterns reveal the combined conversion and alloying reaction mechanisms of the composite.
摘要Suboptimal treatment of laryngeal squamous cell carcinoma(LSCC)provides poor survival rate.The poor bioavailability,resistance to cetuximab(Cet),and the instability of small interfering RNA(siRNA)limit their efficacy in LSCC therapy.The present study has been aimed to develop a Cet and focal adhesion kinase(FAK)siRNA(siFAK)co-delivery nanosystem.Zeolitic imidazolate framework-8(ZIF-8),with its large specific surface area and pH-responsive properties,is an ideal delivery carrier allowing controlled drug release in the acidic tumor microenvironment.Therefore,Cet was loaded onto ZIF-8 and encapsulated in a TU177 cell membrane(TCM)after the electrostatic adsorption of siFAK.Fourier transform infrared(FTIR)spectroscopy,transmission electron microscopy(TEM),scanning electron microscopy(SEM),zeta potential,X-ray diffraction,and particle size analyses were deployed to characterize Cet/siFAK@ZIF-8@TCM.TU177 cells and subcutaneously transplanted tumor-bearing nude mice were used to evaluate the intracellular uptake,cytotoxicity,in vivo biocompatibility,biodistribution,biosafety,pH responsiveness,and anti-LSCC efficacy of Cet/siFAK@ZIF-8@TCM.After ZIF-8@TCM were loaded with Cet and siFAK,alterations in their physical and crystal structures,particle size,and zeta potential were observed.Meanwhile,the co-delivery system increased the loading of Cet through the electrostatic adsorption of siFAK to Cet-loaded ZIF-8.The intracellular uptake of Cet/siFAK@ZIF-8@TCM also protected siFAK from degradation,effectively decreasing the messenger RNA(mRNA)and protein expression levels of FAK in LSCC cells.The ZIF-8@TCM nanosystem for co-delivery of Cet and siFAK exhibited pH-responsiveness and tumor-targeting capabilities,thereby exerting anti-LSCC effects.Co-delivery of Cet and siFAK via the pH-responsive ZIF-8@TCM system enabled the targeted release of the chemotherapeutic and gene,in turn maximizing their anti-LSCC effect while ensuring biosafety.
基金supported by the Vietnam Department of Science and Technology through contract 40/2010/HD-NDT
摘要A zeolite imidazolate framework,ZIF-8,was synthesized and characterized by dynamic laser light scattering,X-ray powder diffraction,scanning electron microscopy,transmission electron microscopy,thermogravimetric analysis,Fourier transform infrared,atomic absorption spectrophotometry,and nitrogen adsorption measurements.The ZIF-8 was highly crystalline and porous with a surface area of over 1600 m2/g.Friedel-Crafts acylation of anisole and benzoyl chloride proceeded well in the presence of ZIF-8(2-6 mol%)without the need for an inert atmosphere.The reaction afforded a selectivity of 93%-95%to the p-isomer.The solid catalyst can be separated from the reaction mixture by simple centrifugation and reused without significant degradation in catalytic activity.There was no leaching of active acid species into the reaction solution.
基金This work was supported by the National Natural Science Foundation of China(Grant Nos.51603052 and 51573216)the Fundamental Research Funds for the Central Universities(Grant Nos.18lgpy02 and 16lgjc66).
摘要Metal-organic frameworks(MOFs)have been intensely studied for the past few decades as an enormous family of highly tunable porous materials with promisingly applicable functionalities in adsorption,separation,catalysis,sensing,electrochemistry,and a great number of emerging purposes.As a classic MOF,zeolitic imidazolate framework-8(ZIF-8)is conventionally one of the very few MOF members that has been commercialized with considerable production.
基金financially supported by Natural Science Foundation of China(No.81871411)National Key R&D Program of China(2018YFC0910601)+1 种基金Youth Innovation Promotion Association Foundation of CAS(2017340)The Science&Technology Bureau of Ningbo City(2015B11002).
摘要Zeolitic imidazolate frameworks(ZIFs)as smart drug delivery systems with microenvironment-triggered release have attracted much attention for tumor therapy.However,the exploration of ZIFs in biomedicine still encounters many issues,such as inconvenient surface modification,fast drug release during blood circulation,undesired damage to major organs,and severe in vivo toxicity.To address the above issues,we developed an Mn-ZIF-90 nanosystem functionalized with an originally designed active-targeting and pH-responsive magnetic resonance imaging(MRI)Y1 receptor ligand[Asn28,Pro30,Trp32]-NPY(25-36)for imaging-guided tumor therapy.After Y1 receptor ligand modification,the Mn-ZIF-90 nanosystem exhibited high drug loading,better blood circulation stability,and dual breast cancer cell membrane and mitochondria targetability,further favoring specific microenvironment-triggered tumor therapy.Meanwhile,this nanosystem showed promising T1-weighted magnetic resonance imaging contrast in vivo in the tumor sites.Especially,this nanosystem with fast clean-up had almost no obvious toxicity and no damage occurred to the major organs in mice.Therefore,this nanosystem shows potential for use in imaging-guided tumor therapy.
基金the National Natural Science Foundation of China(No.21576094)the Guangdong Natural Science Foundation(No.2017A030313052)the Guangdong Basic and Applied Basic Research Foundation(Nos.2019A1515110706,2019A1515110259 and 2019A1515110535)。
摘要The development of a simple and facile synthesis route is a highly desirable but challenging process in the fabrication of nanoscale hierarchical porous zeolitic imidazolate frameworks(ZIFs).Herein we describe a facile method for rapidly synthesizing hierarchically porous ZIF-90 nanocrystals(particle sizes of~300 nm)using hydroxyl double salts as intermediates at room temperature.The as-synthesized ZIF-90 contained hierarchical porous structures developed using a crystalline interior and a random stack of multiple nanoparticles.Both the morphology and particle size of ZIF-90 nanocrystals could be tuned by controlling the molar ratio of ICA/Zn2+.Note that the as-synthesized hierarchically porous ZIF-90 nanocrystals exhibited higher thermal stability compared with the conventional ZIF-90.Because of the introduction of hierarchical porous structures,the resultant hierarchically porous ZIF-90 nanocrystals showed enhanced toluene adsorption capacity than those of conventional metal organic frameworks and zeolites.
基金financial supports from the National Natural Science Foundation of China(21773293 , 21603264)CAS Pioneer Hundred Talents Program (J. Di)+1 种基金The National Key Research and Development Program of China(2016YFA0203301)Key Research Program of Frontier Science of Chinese Academy of Sciences(QYZDB-SSW-SLH031)
摘要Recently, the development of high-performance bifunctional oxygen catalysts integrated with flexible conductive scaffolds f or rechargeable metal-air batteries has attracted considerable interest, driving by fastgrowing wearable electronics. Herein, we report a flexible bifunctional oxygen catalyst thin film consisting of Co–N–C bifunctional catalysts embedding in carbon nanotube(CNT) networks. The catalyst is readily prepared by pyrolysis of cobalt-based zeolitic imidazolate frameworks(ZIF-67) that are in-situ synthesized in CNT networks. Such catalyst film demonstrates very high catalytic activities for oxygen reduction(onset potential: 0.91 V, and half-wave potential: 0.87 V vs. RHE) and oxygen evolution(10 m Acm^-2 at 1.58 V) reactions, high methanol tolerance property, and long-term stability(97% current retention). Moreover, our integrated catalyst film shows very good structure flexibility and robustness. Based on the obtained film air electrodes, flexible Zn–air batteries demonstrate low charging and discharging overpotentials(0.82 V at 1 m A cm^-1) and excellent structure stability in the bending tests. These results indicate that presently reported catalyst films are potential air electrodes for flexible metal–air batteries.
基金supports received from the National Natural Science Foundation of China (21776301,21636009)are gratefully acknowledged.
摘要Although zeolitic imidazolate frameworks(ZIFs)have bright prospects in wide fields like gas storage/separation,catalysis and medicine,etc.,their large-scale applications are bottlenecked by the absence of their low-cost commercial production technique.Here,we report an uncon ventional method suitable for environmentally friendly and low-cost mass-production of ZIFs.In this method,taking the synthesis of ZIF-8 as an example,ZnO was used instead of Zn(NO3)2 in traditional solvent synthesis methods and CO2 was introduced to dissolve ZnO in aqueous solution of 2-methylimidazole(HMeim)and form water soluble salt([ZnMeim]+[MeimCOO]-)at room temperature.Then,by removing CO2 through heating or vacuuming,Meim-ions are produced and instantaneously assemble with[ZnMeim]+s to generate ZIF-8 without any by product.Due to the absence of strong acid anions(such as NO-3 and Cl- et al.)in solution,the washing of filter cake required in the conventional approaches could be omitted and the filtrate containing only water and HMeim could be reused completely.This method is really green as no waste gas or liquid generates because CO2 and water could be recycled perfectly.It overcomes almost all bottlenecks occurred in commercial production of ZIF-8 when using traditional methods.A pilot plant was established for mass-production of ZIF-8 and hundreds kilograms of ZIF-8 was produced,which indicates that the new method is not only environmentally friendly but also low cost and commercial accessibility.It is expected that the new method would open an avenue for commercial applications of ZIFs.
基金the financial support from the Special Funds for the Cultivation of Guangdong College Students’Scientific and Technological Innovation(“Climbing Program”Special Funds,pdjh2023b0145)Guangdong Provincial International Joint Research Center for Energy Storage Materials(2023A0505090009)。
摘要As a prevailing cathode material of lithium-ion batteries(LIBs),LiCoO2(LCO)still encounters the tricky problems of structural collapse,whose morphological engineering and cation doping are crucial for surmounting the mechanical strains and alleviating phase degradation upon cycling.Hereinafter,we propose a strategy using a zeolitic imidazolate framework(ZIF)as the self-sacrificing template to directionally prepare a series of LiNi0.1Co0.9O2(LNCO)with tailorable electrochemical properties.The rational selection of sintering temperature imparts the superiority of the resultant products in lithium storage,during which the sample prepared at 700℃(LNCO-700)outperforms its counterparts in cyclability(156.8 mA h g-1at 1 C for 200 cycles in half cells,1 C=275 mA g-1)and rate capability due to the expedited ion/electron transport and the strengthen mechanical robustness.The feasibility of proper Ni doping is also divulged by half/full cell tests and theoretical study,during which LNCO-700(167 mA h g-1at 1 C for 100 cycles in full cells)surpasses LCO-700 in battery performance due to the mitigated phase deterioration,stabilized layered structu re,ameliorated electro nic co nductivity,a nd exalted lithium sto rage activity.This work systematically unveils tailorable electrochemical behaviors of LNCO to better direct their practical application.
基金supported by the Technology Development Program to Solve Climate Changes of the National Research Foundation(NRF)funded by the Ministry of Science,ICT&Future Planning(NRF-2016M1A2A2936760)supported by Advanced Research Center Program(NRF-2013R1A5A1073861)through the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIP)contracted through Advanced Space Propulsion Research Center at Seoul National UniversityDeanship of Scientific Research at King Saud University for funding this work through research Group no.RG-1440-111。
摘要Freestanding carbon nanofibers loaded with bimetallic hollow nanocage structures were synthesized.The nanocages inherited the rhombic dodecahedral morphology of the zeolitic imidazolate framework(ZIF)precursors,ZIF-8 and ZIF-67.As anode materials for lithium-ion batteries(LIBs),the bimetallic nanocage-loaded freestanding carbon nanofibers effectively buffered volume expansions and alleviated pulverization through their different reduction and oxidation potentials.The higher capacities of the composite anodes arose via the formation of the LixZn alloy and Li2O by Zn and Co ions,respectively,and the enhanced conductivity conferred by the carbon nanofibers.A synergistic effect of the composite components toward the strong electrochemical performance(688 m A h·g-1at 1200 m A·g-1)of the bimetallic nanocage-loaded fibers was demonstrated through the superior long-term stability of the anode(1048 m A h·g-1after 300 cycles at 100 m A·g-1),suggesting that the fabricated anode can be a promising material for use in portable LIBs.
摘要The use of intumescent flame retardants(IFRs)is considered an environmentally friendly and cost-effective strategy to suppress potential fire hazards from synthetic polymers.However,some conventional IFRs are neither efficient in developing a thermally stable char layer nor reducing the release of toxic byproducts during polymer combustion.In this work,we aim to discuss the effects of zeolitic imidazolate frameworks(ZIFs)on synergistically improving the flame retardancy behaviors in polypropylene(PP)composites,including thermal degradation(evolved gas analysis),free radical reactions in the gaseous phase(in-situ chemiluminescent image analysis),and carbonaceous structure in the condensed phase(micro-morphology and composition analysis).It is found that the transition metals in ZIFs can catalytically accelerate the crosslinking reaction at a lower initial temperature and decrease the amount of hydrocarbon volatiles in the gaseous phase.Once ignited,the embedded ZIFs can firstly bridge adjacent phosphorus chains in the polymer matrix to expand crosslinking degrees and then they are anchored in the developed N-doped phospho-carbonaceous networks after pyrolysis.As a result,more compact char residue structures are observed in the condensed phase for ZIF-reinforced composites.For example,by replacing 2 wt%of IFR with ZIF-67,the peak heat release rate,peak smoke production rate,and peak CO production rate are reduced by 69%,80%,and 72%,respectively,when compared to the conventional composite.These results indicate an excellent solution to resolve inherent fire hazards associated with IFRs in polymers and achieve necessary efficiency for industrial applications.It also provides a new strategy for determining flammability characteristics and combustion mechanisms of polymer composites using in-situ chemiluminescence analysis.
基金We gratefully acknowledge the National Key Research and Development Program of China(No.2018YFA0208600)。
摘要Two new boron imidazolate frameworks(BIFs),Zn2[HBH(2-mim)3]2(1,2-PEA)2(EG)2(BIF-120,EG=ethylene glycol)and Zn[BH(2-mim)3](1,2-HPEA)(BIF-121),were successfully synthesized by mixing the KBH(2-mim)3 ligand and the semirigid aromatic dicarboxylate ligand 1,2-benzenediacetic acid(1,2-H2PEA)under solvothermal conditions.In this paper,the two samples were structurally characterized by single-crystal X-ray diffraction and tested by infrared spectroscopy(IR),UV-visible spectroscopy(UV-Vis),thermogravimetric analysis TGA and X-ray powder diffractions.In addition,the solid-state luminescent properties of these crystals were also investigated.
基金supported by the Excellent Youth Foundation of Henan Scientific Committee,China(222300420018)Key Scientific Research Projects in Universities of Henan Province,China(21zx006)。
摘要Layered assembled membranes of 2D leaf-like zeolitic imidazolate frameworks(ZIF-L)nanosheets have received great attention in the field of water treatment due to the porous structure and excellent antibacterial ability,but the dense accumulation on the membrane surface and the low permeate flux greatly hinder their application.Herein,we synthesized m HNTs(modified halloysite nanotubes)/ZIF-L nanocomposites on modified m HNTs by in situ growth method.Interestingly,due to the different size of m HNTs and ZIF-L,m HNTs were packed in ZIF-L nanosheets.The hollow m HNTs provided additional transport channels for water molecules,and the accumulation of the ZIF-L nanosheets was decreased after assembling m HNTs/ZIF-L nanocomposites into membrane by filtration.The prepared m HNTs/ZIF-L membrane presented high permeate flux(59.6 L·m-2·h-1),which is 2-4 times of the ZIF-L membranes(14.8 L·m-2·h-1).Moreover,m HNTs/ZIF-L membranes are intrinsically antimicrobial,which exhibit extremely high bacterial resistance.We provide a controllable strategy to improve 2D ZIF-L assembles,and develops novel membranes using 2D package structure as building units.
基金supported by the National Key Research and Development Program of China(No.2016YFB0701100)the National Natural Science Foundation of China(Nos.21622102 and 21621001)+1 种基金the National 111 Project(No.B17020)Program for JLUSTIRT,and High Performance Computing Center of Jilin University
摘要To find potential zeolitic imidazolate frameworks(ZIFs)for CO2capture from flue gas,we built 169,898 ZIF models from 84,949 hypothetical zeolite networks.By calculating their lattice energies,accessible volumes to CO2,the isosteric adsorption heat(Qst)of H2 O,Henry’s constant ratio(SKH)of CO2/N2,percent regenerability(R%),CO2working capacity(ΔN CO2),CO2/N2adsorption selectivity(S CO2/N2)and adsorbent performance score(APS),we identi fied 49 hydrophobic ZIF structures that might outplay already-realised ZIFs built from the same imidazolate linkers for CO2capture from flue gas.
基金supported by the National Natural Science Foundation of China (Nos. 11775037 and 21676030)the Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology (BM212110)The Postgraduate Innovation Project of Changzhou University (KYCX19_1782)。
摘要A novel ZIF-8-CMC hybrid material was fabricated from the hybridization of ZIF-8 and carboxymethylcellulose(CMC) by impregnation method for n-hexane/3-methylpentane separation.The surface properties of ZIF-8 were tailored by introducing CMC into ZIF-8 nanoparticles.In this work,adsorption separation of n-hexane(nHEX) and 3-methylpentane(3 MP) on ZIF-8-CMC were investigated by batch vapor-phase adsorption and liquid-phase breakthrough adsorption.The adsorption selectivity of nHEX/3 MP reversed from preferable adsorption of nHEX to preferable adsorption of 3 MP upon the increasing of CMC containing in the hybrid materials.As the temperature increases,the adsorption amounts of nHEX and 3 MP decrease.With the increasing of CMC contents,the nHEX uptake decreased,the uptake capacity of 3 MP increased gradually.For liquid-phase breakthrough adsorption,the dynamic adsorption capacity of nHEX also decreased with the increasing of temperature.
基金supported by the National Natural Science Foundation of China (Nos.21467028 and 21777129)the Program for Innovative Research Group of Gansu Province+3 种基金China(No.1210RJIA001)Special Fund Project for the Central Government to Guide Local Science and Technology Development (2020)Key Laboratory of Polymer Materials of Gansu Provincethe Key Laboratory of Ecological Environment Related Polymer Materials of Ministry of Education。
摘要A novel flower-shaped zeolitic imidazolate framework(ZIF) doped organic-inorganic hybrid monolithic column(ZIF-HMC) was prepared by a simple sol-gel "one-step" method and utilized for efficient capillary microextraction(CME) of four brominated flame retardants.The prepared monolithic was characterized by Fourier transform infrared,scanning electron microscopy,X-ray photoelectron spectroscopy,energy disperse spectroscopy,and N2 adsorption-desorption.The parameters of CME were optimized by orthogonal array design.Under the optimal conditions,the ZIF-HMC showed excellent extraction efficiency,the limit of detection(LODs) and the limit of quantification(LOQs) were in the range of0.52$3.1 mg/L and 1.7$10 mg/L,respectively,and the proposed method demonstrated good recovery(88.8%–116.6%) with the RSD less than 13.6% and a reusability of at least 30 times.The ZIF-HMC possessed great potential for separating organic pollutants and the strategy used here could be extended to prepare other derivatized HMC functionalized monoliths.
摘要Immunogenic antigen downregulation combined with an immunosuppressive tumor microenvironment(TME)remain major barriers to effective treatment of“cold”tumors.Here,we report a dual-functional nanotherapy that integrates C70fullerene with hyaluronic acid(HA)–modified zeolitic imidazolate framework-8(ZIF-8)to enhance tumor immunogenicity and reprogram the TME.The resulting HA-C70@ZIF-8 nanocomposites exploit HAmediated CD44 targeting to promote selective tumor uptake and retention.Once internalized,acidic lysosomal conditions trigger Zn2+release from ZIF-8,causing ion overload,caspase-1 activation,gasdermin D cleavage,and pyroptotic tumor cell death accompanied by the release of damage-associated molecular patterns(DAMPs).Concurrently,encapsulated C70facilitates metabolic reprogramming of tumor-associated macrophages(TAMs)from an M2-to M1-like phenotype,thereby alleviating immunosuppression.Together,these mechanisms elicit robust immune activation and potentiate the efficacy of immune checkpoint blockade,offering a streamlined and impactful strategy for personalized tumor therapy and paving the way for novel approaches to highly effective immunotherapy.