The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we re...The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we report the rational design of nanoreactors comprising hollow carbon sphere-confined PtNi bimetallic NPs(PtNi@HCS)as highly efficient catalysts for hydrogen generation via ammonia borane hydrolysis in water.Using both density functional theory calculations and molecular dynamics simulations,the effects of an active PtNi combination and the critical synergistic role of a hollow carbon shell on the molecule diffusion adsorption behaviors are explored.Kinetic isotope effects and theoretical calculations allow the clarification of the mechanism,with oxidative addition of an O-H bond of water to the catalyst surface being the rate-determining step.The remarkable catalytic activity of the PtNi@HCS nanoreactor was also utilized for successful tandem catalytic hydrogenation reactions,using in situ-generated H_(2) from ammonia borane with high efficiency.The concerted design,theoretical calculations,and experimental work presented here shed light on the rational elaboration of efficient nanocatalysts and contribute to the establishment of a circular carbon economy using green hydrogen.展开更多
The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) utilization.Photothermal catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosyn...The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) utilization.Photothermal catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosynthesis by coupling both photochemistry and thermochemistry.However,strategies for maximizing the use of solar spectra with different frequencies in photothermal catalysis are urgently needed.Here,a hierarchical full-spectrum solar light utilization strategy is proposed.Based on this strategy,a Cu@hollow titanium silicalite-1 zeolite(TS-1)nanoreactor with spatially separated photo/thermal catalytic sites is designed to realize high-efficiency photothermal catalytic artificial photosynthesis.The space-time yield of alcohol products over the optimal catalyst reached 64.4μmol g−1 h−1,with the selectivity of CH3CH2OH of 69.5%.This rationally designed hierarchical utilization strategy for solar light can be summarized as follows:(1)high-energy ultraviolet light is utilized to drive the initial and difficult CO_(2) activation step on the TS-1 shell;(2)visible light can induce the localized surface plasmon resonance effect on plasmonic Cu to generate hot electrons for H2O dissociation and subsequent reaction steps;and(3)low-energy near-infrared light is converted into heat by the simulated greenhouse effect by cavities to accelerate the carrier dynamics.This work provides some scientific and experimental bases for research on novel,highly efficient photothermal catalysts for artificial photosynthesis.展开更多
Photothermal and photodynamic therapies(PTT/PDT)hold promise for localized tumor treatment,yet their full potential is hampered by limitations such as the hypoxic tumor microenvironment and inadequate systemic immune ...Photothermal and photodynamic therapies(PTT/PDT)hold promise for localized tumor treatment,yet their full potential is hampered by limitations such as the hypoxic tumor microenvironment and inadequate systemic immune activation.Addressing these challenges,we present a novel near-infrared(NIR)-triggered RNS nanoreactor(PBNO-Ce6)to amplify the photodynamic and photothermal therapy efficacy against triple-negative breast cancer(TNBC).The designed PBNOCe6 combines sodium nitroprusside-doped Prussian Blue nanoparticles with Chlorin e6 to enable on-site RNS production through NIR-induced concurrent NO release and ROS generation.This not only enhances tumor cell eradication but also potentiates local and systemic antitumor immune responses,protecting mice from tumor rechallenge.Our in vivo evaluations revealed that treatment with PBNO-Ce6 leads to a remarkable 2.7-fold increase in cytotoxic T lymphocytes and a 62%decrease in regulatory T cells in comparison to the control PB-Ce6(Prussian Blue nanoparticles loaded with Chlorin e6),marking a substantial improvement over traditional PTT/PDT.As such,the PBNO-Ce6 nanoreactor represents a transformative approach for improving outcomes in TNBC and potentially other malignancies affected by similar barriers.展开更多
Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improv...Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.展开更多
Traditional microtubule inhibitors fail to significantly enhance+e effect of colorectal cancer;hence,new and efficient strategies are necessary.In+is study,a supramolecular nanoreactor(DOC@TA-Fe^(3+))based on tannic a...Traditional microtubule inhibitors fail to significantly enhance+e effect of colorectal cancer;hence,new and efficient strategies are necessary.In+is study,a supramolecular nanoreactor(DOC@TA-Fe^(3+))based on tannic acid(TA),iron ion(Fe^(3+)),and docetaxel(DOC)wi+microtubule inhibition,reactive oxygen species(ROS)generation,and gluta+ione peroxidase 4(GPX4)inhibition,is prepared for ferroptosis/apoptosis treatment.After internalization by CT26 cells,+e DOC@TA-Fe^(3+)nanoreactor escapes from+e lysosomes to release payloads.+e subsequent Fe^(3+)/Fe^(2+)conversion mediated by TA reducibility can trigger+e Fenton reaction to enhance+e ROS concentration.Additionally,Fe^(3+)can consume gluta+ione to repress+e activity of GPX4 to induce ferroptosis.Meanwhile,+e released DOC controls microtubule dynamics to activate+e apoptosis pa+way.+e superior in vivo antitumor efficacy of DOC@TA-Fe^(3+)nanoreactor in terms of tumor grow+inhibition and improved survival is verified in CT26 tumor-bearing mouse model.+erefore,+e nanoreactor can act as an effective apoptosis and ferroptosis inducer for application in colorectal cancer+erapy.展开更多
The enzyme-mediated elevation of reactive oxygen species(ROS)at the tumor sites has become an emerging strategy for regulating intracellular redox status for anticancer treatment.Herein,we proposed a camouflaged bioni...The enzyme-mediated elevation of reactive oxygen species(ROS)at the tumor sites has become an emerging strategy for regulating intracellular redox status for anticancer treatment.Herein,we proposed a camouflaged bionic cascaded-enzyme nanoreactor based on Ti_(3)C_(2)nanosheets for combined tumor enzyme dynamic therapy(EDT),phototherapy and deoxygenation-activated chemotherapy.Briefly,glucose oxidase(GOX)and chloroperoxidase(CPO)were chemically conjugated onto Ti_(3)C_(2)nanosheets,where the deoxygenation-activated drug tirapazamine(TPZ)was also loaded,and the Ti_(3)C_(2)-GOX-CPO/TPZ(TGCT)was embedded into nanosized cancer cell-derived membrane vesicles with high-expressed CD47(m_eTGCT).Due to biomimetic membrane camouflage and CD47 overexpression,m_eTGCT exhibited superior immune escape and homologous targeting capacities,which could effectively enhance the tumor preferential targeting and internalization.Once internalized into tumor cells,the cascade reaction of GOX and CPO could generate HClO for efficient EDT.Simultaneously,additional laser irradiation could accelerate the enzymic-catalytic reaction rate and increase the generation of singlet oxygen(~1O_(2)).Furthermore,local hypoxia environment with the oxygen depletion by EDT would activate deoxygenation-sensitive prodrug for additional chemotherapy.Consequently,m_eTGCT exhibits amplified synergistic therapeutic effects of tumor phototherapy,EDT and chemotherapy for efficient tumor inhibition.This intelligent cascaded-enzyme nanoreactor provides a promising approach to achieve concurrent and significant antitumor therapy.展开更多
Yolk‐shell structured nanoparticles are of immense scientific and technological interests because of their unique architecture and myriad of applications.This review summarizes recent progresses in the use of yolk‐s...Yolk‐shell structured nanoparticles are of immense scientific and technological interests because of their unique architecture and myriad of applications.This review summarizes recent progresses in the use of yolk‐shell structured nanoparticles as nanoreactors for various chemical reactions.A very brief overview of synthetic strategies is provided with emphasis on recent research progress in the last five years.Catalytic applications of these yolk‐shell structured nanoreactors are then discussed by covering photocatalysis,methane reforming and electrochemical conversion.The state of the art research and perspective in future development are also highlighted.展开更多
Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartme...Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.展开更多
SO_(2)poisoning is a common problem in the catalytic combustion of volatile organic compounds(VOCs).In this work,we took three-dimensionally ordered macroporous and mesoporous(3DOM)SiO_(2)as the nanoreactor to protect...SO_(2)poisoning is a common problem in the catalytic combustion of volatile organic compounds(VOCs).In this work,we took three-dimensionally ordered macroporous and mesoporous(3DOM)SiO_(2)as the nanoreactor to protect active sites from SO_(2)erosion in the catalytic combustion of benzene.Simultaneously,the confined growth of metal active nanoparticles in the multi-stage pore is also full of challenges.And we successfully confined Co_(3)O_(4)nanoparticles(NPs)in macroporous and mesoporous channels.Interestingly,the precursors’growth in the pore was controlled and nanoreactors with different pore sizes were prepared by adjusting the loading amount and preparation methods.It is discovered that the Co_(3)O_(4)NPs confined in 3DOM SiO_(2)nanoreactor showed superior sulfur and water resistance.Density functional theory(DFT)calculations verified that the Co-Si catalyst had high SO_(2)adsorption energy(-0.48 eV),which illustrated that SO_(2)was hard to attach to the surface of the Co-Si catalyst.The SiO_(2)nanoreactor had low SO_(2)adsorption energy(-5.15 eV),which indicated that SO_(2)was easily absorbed on SiO_(2)nanoreactor.This illustrated that the SiO_(2)nanoreactor could protect effectively active sites from SO_(2)erosion.展开更多
Tumor microenvironment(TME),as the“soil”of tumor growth and metastasis,exhibits significant differences from normal physiological conditions.However,how to manipulate the distinctions to achieve the accurate therapy...Tumor microenvironment(TME),as the“soil”of tumor growth and metastasis,exhibits significant differences from normal physiological conditions.However,how to manipulate the distinctions to achieve the accurate therapy of primary and metastatic tumors is still a challenge.Herein,an innovative nanoreactor(AH@MBTF)is developed to utilize the apparent differences(copper concentration and H_(2)O_(2)level)between tumor cells and normal cells to eliminate primary tumor based on H_(2)O_(2)-dependent photothermal-chemodynamic therapy and suppress metastatic tumor through copper complexation.This nanoreactor is constructed using functionalized MSN incorporating benzoyl thiourea(BTU),triphenylphosphine(TPP),and folic acid(FA),while being co-loaded with horseradish peroxidase(HRP)and its substrate ABTS.During therapy,the BTU moieties on AH@MBTF could capture excessive copper(highly correlated with tumor metastasis),presenting exceptional anti-metastasis activity.Simultaneously,the complexation between BTU and copper triggers the formation of cuprous ions,which further react with H_(2)O_(2)to generate cytotoxic hydroxyl radical(•OH),inhibiting tumor growth via che-modynamic therapy.Additionally,the stepwise targeting of FA and TPP guides AH@MBTF to accurately accu-mulate in tumor mitochondria,containing abnormally high levels of H_(2)O_(2).As a catalyst,HRP mediates the oxidation reaction between ABTS and H_(2)O_(2)to yield activated ABTS•^(+).Upon 808 nm laser irradiation,the activated ABTS•^(+)performs tumor-specific photothermal therapy,achieving the ablation of primary tumor by raising the tissue temperature.Collectively,this intelligent nanoreactor possesses profound potential in inhib-iting tumor progression and metastasis.展开更多
Titanium dioxide(TiO_(2))hollow nanoparticles present significant potential for photocatalytic applications while their straightforward preparation with precise structure control is still challenging.This work reports...Titanium dioxide(TiO_(2))hollow nanoparticles present significant potential for photocatalytic applications while their straightforward preparation with precise structure control is still challenging.This work reports the approach to preparing tunable hollow TiO_(2) nanospheres by utilization of spherical polyelectrolyte brushes(SPB)as nanoreactors and templates.During the preparation,the evolution of the structure was characterized by small angle X-ray scattering(SAXS),and in combination with dynamic light scattering and transmission electron microscopy.The formation of TiO_(2) shell within the brush(SPB@TiO_(2))is confirmed by the significant increase of the electron density,and its internal structure has been analyzed by fitting SAXS data,which can be influenced by Titanium precursors and ammonia concentration.After calcining SPB@TiO_(2) in a muffle furnace,hollow TiO_(2) nanospheres are produced,and their transition to the anatase crystal form is triggered,as confirmed by X-ray diffraction analysis.Utilizing the advantages of their hollow structure,these TiO_(2) nanospheres exhibit exceptional catalytic degradation efficiency of methylene blue(MB),tetracycline(TC),and 2,4-dichlorophenoxyacetic acid(2,4-D),and also demonstrate excellent recyclability.展开更多
Covalent organic frameworks(COFs)-based nanoreactors have attracted broad interest in many fields due to their voidconfinement effects.However,the inherent drawback of conventional nanoreactors is the lack of internal...Covalent organic frameworks(COFs)-based nanoreactors have attracted broad interest in many fields due to their voidconfinement effects.However,the inherent drawback of conventional nanoreactors is the lack of internal active sites,which limits their widespread utilization.Herein,we report the construction of hierarchical COF(EB-TFP)nanoreactor with pre-synthesized polyoxometalates(POM,[PV_(2)W_(10)O_(40)]^(5–)(PV_(2)W_(10)))clusters encapsulated inside of COF(POM@COF).PV_(2)W_(10)@EB-TFP anchors nucleophilic-group(Br–ions)and PV_(2)W_(10)anion cluster within the COF framework via electrostatic interactions,which not only simplifies the reaction system but also enhances catalytic efficiency.The reaction performance of the PV_(2)W_(10)@EB-TFP nanoreactor can be tuned to achieve excellent catalytic activity in CO_(2)cycloaddition reaction(CCR)for~97.63%conversion and~100%selectivity under visible light irradiation.A mechanistic study based on density functional theory(DFT)calculations and insitu characterization was also carried out.In summary,we have reported a method for achieving the uniform dispersion of POM single clusters into COF nanoreactor,demonstrating the potential of POM@COF nanoreactor for synergistic photothermal catalytic CO_(2)cycloaddition.展开更多
The current strategy of co-delivering copper ions and disulfiram(DSF)to generate cytotoxic CuET faces limitations in achieving rapid and substantial CuET production,specifically in tumor lesions.To overcome this chall...The current strategy of co-delivering copper ions and disulfiram(DSF)to generate cytotoxic CuET faces limitations in achieving rapid and substantial CuET production,specifically in tumor lesions.To overcome this challenge,we introduce a novel burst-release cascade reactor composed of phase change materials(PCMs)encapsulating ultrasmall Cu_(2-x)Se nanoparticles(NPs)and DSF(DSF/Cu_(2-x)Se@PCM).Once triggered by second near-infrared(NIR-II)light irradiation,the reactor swiftly releases Cu_(2-x)Se NPs and DSF,enabling catalytic reactions that lead to the rapid and massive production of Cu_(2-x)Se-ET complexes,thereby achieving in situ chemotherapy.The mechanism of the burst reaction is due to the unique properties of ultrasmall Cu_(2-x)Se NPs,including their small size,multiple defects,and high surface activity.These characteristics allow DSF to be directly reduced and chelated on the surface defect sites of Cu_(2-x)Se,forming Cu_(2-x)Se-ET complexes without the need for copper ion release.Additionally,Cu_(2-x)Se-ET has demonstrated a similar(to CuET)anti-tumor activity through increased autophagy,but with even greater potency due to its unique two-dimensional-like structure.The light-triggered cascade of interlocking reactions,coupled with in situ explosive generation of tumor-suppressive substances mediated by the size and valence of Cu_(2-x)Se,presents a promising approach for the development of innovative nanoplatforms in the field of precise tumor chemotherapy.展开更多
Core-shell nanostructures consisting of active metal cores and protective shells often exhibit enhanced catalytic performance, in which reactants can access a small part of the core surfaces through the pores in the s...Core-shell nanostructures consisting of active metal cores and protective shells often exhibit enhanced catalytic performance, in which reactants can access a small part of the core surfaces through the pores in the shells. In this study, we show that Pt nanoparticles (NPs) can be embedded into few-layer hexagonal boron nitride (h-BN) overlayers, forming Pt@h-BN core-shell nanocatalysts. The h-BN shells not only protect the Pt NPs under harsh conditions but also allow gaseous molecules such as CO and 02 to access a large part of the Pt surfaces through a facile intercalation process. As a result, the Pt@h-BN nanostructures act as nanoreactors, and CO oxidation reactions with improved activity, selectivity, and stability occur at the core-shell interfaces. The confinement effect exerted by the h-BN shells promotes the Pt-catalyzed reactions. Our work suggests that two-dimensional shells can function as robust but flexible covers on nanocatalyst surfaces and tune the surface reactivity.展开更多
Carbon-carbon(C–C)coupling reactions represent one of the most powerful tools for the synthesis of complex natural products,bioactive molecules developed as drugs and agrochemicals.In this work,a multifunctional nano...Carbon-carbon(C–C)coupling reactions represent one of the most powerful tools for the synthesis of complex natural products,bioactive molecules developed as drugs and agrochemicals.In this work,a multifunctional nanoreactor for C–C coupling reaction was successfully fabricated via encapsulating the core-shell Cu@Ni nanocubes into ZIF-8(Cu@Ni@ZIF-8).In this nanoreactor,Ni shell of the core-shell Cu@Ni nanocubes was the catalytical active center,and Cu core was in situ heating source for the catalyst by absorbing the visible light.Moreover,benefiting from the plasmonic resonance effect between Cu@Ni nanocubes encapsulated in ZIF-8,the absorption range of nanoreactor was widened and the utilization rate of visible light was enhanced.Most importantly,the microporous structure of ZIF-8 provided shape-selective of reactant.This composite was used for the highly shape-selective and stable photocatalysed C–C coupling reaction of boric acid under visible light irradiation.After five cycles,the nanoreactor still remained high catalytical activity.This Cu@Ni@ZIF-8 nanoreactor opens a way for photocatalytic C–C coupling reactions with shape-selectivity.展开更多
Zinc oxide nanoparticles (ZnO NPs), as a new type of pH-sensitive drug carrier, have received much attention. ZnO NPs are stable at physiological pH, but can dissolve quickly in the acidic tumor environment (pH 〈 ...Zinc oxide nanoparticles (ZnO NPs), as a new type of pH-sensitive drug carrier, have received much attention. ZnO NPs are stable at physiological pH, but can dissolve quickly in the acidic tumor environment (pH 〈 6) to generate cytotoxic zinc ions and reactive oxygen species (ROS). However, the protein corona usually causes the non-specific degradation of ZnO NPs, which has limited their application considerably. Herein, a new type of pH-sensitive nanoreactor (ZnO-DOX@F-mSiO2-FA), aimed at reducing the non-specific degradation of ZnO NPs, is presented. In the acidic tumor environment (pH 〈 6), it can release cytotoxic zinc ions, ROS, and anticancer drugs to kill cancer cells effectively. In addition, the fluorescence emitted from fluorescein isothiocyanate (FITC)-labeled mesoporous silica (F-mSiO2) and doxorubicin (DOX) can be used to monitor the release behavior of the anticancer drug. This report provides a new method to avoid the non-specific degradation of ZnO NPs, resulting in synergetic therapy by taking advantage of ZnO NPs-induced oxidative stress and targeted drug release.展开更多
Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes...Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes and lean electrolytes.Herein,a novel carbon foam integrated by hollow carbon bubble nanoreactors with ultrahigh pore volume of 6.9 cm3·g−1 is meticulously designed for ultrahigh sulfur content up to 96 wt.%.Tailoring polysulfide trapping and ion/electron transport kinetics during the charge-discharge process can be achieved by adjusting the wall thickness of hollow carbon bubbles.And a further in-depth understanding of electrochemical reaction mechanism for the cathode is impelled by the in-situ Raman spectroscopy.As a result,the as-prepared cathode delivers high specific capacitances of 1,269 and 695 mAh·g−1 at 0.1 and 5 C,respectively.Furthermore,Li-S pouch cells with high areal sulfur loading of 6.9 mg·cm−2 yield exceptional practical energy density of 382 Wh·kg−1 under lean electrolyte of 3.5µL·mg−1,which demonstrates the great potential for realistic high-energy Li-S batteries.展开更多
It remains a great challenge to explore the facile way to fabricate multi-component nanoparticles in theranostic nanomedicine. Herein, an albumin nanoreactor templated synthesis of theranostic Gd203/CuS hybrid nanodo...It remains a great challenge to explore the facile way to fabricate multi-component nanoparticles in theranostic nanomedicine. Herein, an albumin nanoreactor templated synthesis of theranostic Gd203/CuS hybrid nanodots (NDs) has been developed for multimodal imaging guided photothermal tumor ablation. Gd2O3/CuS NDs are found to possess particle size of 4.4 ± 1.1nm, enhanced longitudinal relaxivity, effective photothermal conversion of 45.5%, as well as remarkable near-infrared fluorescence (NIRF) from Cy7.5-conjugated on albumin corona. The Gd203/CuS NDs further exhibited good photostability, en- hanced cellular uptake, and preferable tumor accumulation. Thus, the Gd203/CuS NDs generate remarkable NIRF imag- ing and Tl-weighted magnetic resonance (MR) imaging, and simultaneously result in effective photothermal tumor ab- lation upon irradiation. The albumin nanoreactor provides a facile and general strategy to synthesize multifunctional nanoparticles for cancer theranostics.展开更多
Bioorthogonal cleavage reaction-triggered prodrug activation by the pretargeted methods can achieve accurate cancer therapy.However,the click and release efficiency of these methods in vivo is limited by the space-tim...Bioorthogonal cleavage reaction-triggered prodrug activation by the pretargeted methods can achieve accurate cancer therapy.However,the click and release efficiency of these methods in vivo is limited by the space-time dislocation of bioorthogonal prodrug-trigger pairs within the tumor area,caused by their asynchronous administration and inconsistent accumulation for most delivery systems.We herein created a nanovoid-confinement and click-activated(NCCA)core–shell nanoreactor by incorporating prodrugs within zeolitic imidazolate framework-90(ZIF-90)as core and coating tetrazine-based covalent organic framework(COF)as shell.After surface modification of aptamer polymer,the NCCA nanoreactor enabled the sufficient delivery of photodynamic prodrugs within tumor.Notably,the core of ZIF-90 was decomposed by tumor acidic environment,inducing the high-efficiency activation of photodynamic prodrugs via nanoconfined bioorthogonal reaction with tetrazine-based COF shell.As a result,such photodynamic agents are efficiently and safely accumulated into tumor and specifically activated for precise photodynamic therapy of cancer cells and tumor bearing mice with minimizing toxic side effect.Taken together,such NCCA nanoreactor clearly demonstrates the critical feasibility to realize the synchronous delivery of both prodrugs and triggers for precise treatment,which most of delivery systems are not able to afford.展开更多
Metallic phosphides as a crucial class of metal-like compounds show high electric conductivity and electrochemical properties.It is of significant benefit to understanding the relationship between the electrocatalytic...Metallic phosphides as a crucial class of metal-like compounds show high electric conductivity and electrochemical properties.It is of significant benefit to understanding the relationship between the electrocatalytic performance and phosphating degree of precursors.In this work,using Co3O4@SiO2 as precursor,core-shell structured CoP@SiO2 nanoreactors with outstanding oxygen evolution reaction performance were synthesized through a facile calcination method.The electrocatalytic performance of CoP@SiO2 modified electrode that treated with 500 mg NaH2PO2 was greatly enhanced.The obtained product displays a low overpotential of 280 mV at a current density of 10 mA/cm2 and a Tafel value 89 mV/dec in alkaline conditions.The easy available CoP@SiO2 with outstanding catalytic performance and stability possesses huge potential in future electrochemical applications.展开更多
基金Financial support was received from the National Key R&D Program of China (2021YFC2902505)the start-up funding by Beijing University of Technology (Changlong Wang)。
文摘The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we report the rational design of nanoreactors comprising hollow carbon sphere-confined PtNi bimetallic NPs(PtNi@HCS)as highly efficient catalysts for hydrogen generation via ammonia borane hydrolysis in water.Using both density functional theory calculations and molecular dynamics simulations,the effects of an active PtNi combination and the critical synergistic role of a hollow carbon shell on the molecule diffusion adsorption behaviors are explored.Kinetic isotope effects and theoretical calculations allow the clarification of the mechanism,with oxidative addition of an O-H bond of water to the catalyst surface being the rate-determining step.The remarkable catalytic activity of the PtNi@HCS nanoreactor was also utilized for successful tandem catalytic hydrogenation reactions,using in situ-generated H_(2) from ammonia borane with high efficiency.The concerted design,theoretical calculations,and experimental work presented here shed light on the rational elaboration of efficient nanocatalysts and contribute to the establishment of a circular carbon economy using green hydrogen.
基金supported by the National Natural Science Foundation of China(Grant Nos.21908052 and 22108200)the Key Program of the Natural Science Foundation of Hebei Province(Grant No.B2020209017)+2 种基金the Project of Science and Technology Innovation Team,Tangshan(Grant No.20130203D)the Natural Science Foundation of Zhejiang Province(Grant No.LQ22B060013)and the Science and Technology Project of Hebei Education Department(Grant No.QN2021113).
文摘The artificial photosynthesis technology has been recognized as a promising solution for CO_(2) utilization.Photothermal catalysis has been proposed as a novel strategy to promote the efficiency of artificial photosynthesis by coupling both photochemistry and thermochemistry.However,strategies for maximizing the use of solar spectra with different frequencies in photothermal catalysis are urgently needed.Here,a hierarchical full-spectrum solar light utilization strategy is proposed.Based on this strategy,a Cu@hollow titanium silicalite-1 zeolite(TS-1)nanoreactor with spatially separated photo/thermal catalytic sites is designed to realize high-efficiency photothermal catalytic artificial photosynthesis.The space-time yield of alcohol products over the optimal catalyst reached 64.4μmol g−1 h−1,with the selectivity of CH3CH2OH of 69.5%.This rationally designed hierarchical utilization strategy for solar light can be summarized as follows:(1)high-energy ultraviolet light is utilized to drive the initial and difficult CO_(2) activation step on the TS-1 shell;(2)visible light can induce the localized surface plasmon resonance effect on plasmonic Cu to generate hot electrons for H2O dissociation and subsequent reaction steps;and(3)low-energy near-infrared light is converted into heat by the simulated greenhouse effect by cavities to accelerate the carrier dynamics.This work provides some scientific and experimental bases for research on novel,highly efficient photothermal catalysts for artificial photosynthesis.
基金the financial support from the National Natural Science Foundation of China (No. 82372019, 82022034, 82173327)Jiangsu Province Natural Science Foundation of China (BK20200032)Double First Class Foundation of China Pharmaceutical University(CPUQNJC22_03)
文摘Photothermal and photodynamic therapies(PTT/PDT)hold promise for localized tumor treatment,yet their full potential is hampered by limitations such as the hypoxic tumor microenvironment and inadequate systemic immune activation.Addressing these challenges,we present a novel near-infrared(NIR)-triggered RNS nanoreactor(PBNO-Ce6)to amplify the photodynamic and photothermal therapy efficacy against triple-negative breast cancer(TNBC).The designed PBNOCe6 combines sodium nitroprusside-doped Prussian Blue nanoparticles with Chlorin e6 to enable on-site RNS production through NIR-induced concurrent NO release and ROS generation.This not only enhances tumor cell eradication but also potentiates local and systemic antitumor immune responses,protecting mice from tumor rechallenge.Our in vivo evaluations revealed that treatment with PBNO-Ce6 leads to a remarkable 2.7-fold increase in cytotoxic T lymphocytes and a 62%decrease in regulatory T cells in comparison to the control PB-Ce6(Prussian Blue nanoparticles loaded with Chlorin e6),marking a substantial improvement over traditional PTT/PDT.As such,the PBNO-Ce6 nanoreactor represents a transformative approach for improving outcomes in TNBC and potentially other malignancies affected by similar barriers.
基金financially supported by the National Natural Science Foundation of China (22372001)Starting Fund for Scientific Research of High-Level Talents, Anhui Agricultural University (rc382108)+1 种基金Anhui Provincial Key Research and Development Plan (2022e07020037)Innovation and Entrepreneurship Training Program for College Students (X202310364204, S202210364046, X202310364209)
文摘Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.
基金supported by the National Natural Science Foundation of China(Grant Nos.:31971308,81960769,and U1903211)National S&T Major Project(Grant No.:2019ZX09301-147),Luzhou Science and Technology Plan(Grant No.:2018CDLZ10)Sichuan Science and Technology Program(Grant No.:2021YFS0081).
文摘Traditional microtubule inhibitors fail to significantly enhance+e effect of colorectal cancer;hence,new and efficient strategies are necessary.In+is study,a supramolecular nanoreactor(DOC@TA-Fe^(3+))based on tannic acid(TA),iron ion(Fe^(3+)),and docetaxel(DOC)wi+microtubule inhibition,reactive oxygen species(ROS)generation,and gluta+ione peroxidase 4(GPX4)inhibition,is prepared for ferroptosis/apoptosis treatment.After internalization by CT26 cells,+e DOC@TA-Fe^(3+)nanoreactor escapes from+e lysosomes to release payloads.+e subsequent Fe^(3+)/Fe^(2+)conversion mediated by TA reducibility can trigger+e Fenton reaction to enhance+e ROS concentration.Additionally,Fe^(3+)can consume gluta+ione to repress+e activity of GPX4 to induce ferroptosis.Meanwhile,+e released DOC controls microtubule dynamics to activate+e apoptosis pa+way.+e superior in vivo antitumor efficacy of DOC@TA-Fe^(3+)nanoreactor in terms of tumor grow+inhibition and improved survival is verified in CT26 tumor-bearing mouse model.+erefore,+e nanoreactor can act as an effective apoptosis and ferroptosis inducer for application in colorectal cancer+erapy.
基金This work was supported by the National Natural Science Foundation of China(51773231)Shenzhen Science and Technology Project(JCYJ20190807160801664)the Project of Key Laboratory of Sensing Technology and Biomedical Instruments of Guangdong Province(2011A060901013).
文摘The enzyme-mediated elevation of reactive oxygen species(ROS)at the tumor sites has become an emerging strategy for regulating intracellular redox status for anticancer treatment.Herein,we proposed a camouflaged bionic cascaded-enzyme nanoreactor based on Ti_(3)C_(2)nanosheets for combined tumor enzyme dynamic therapy(EDT),phototherapy and deoxygenation-activated chemotherapy.Briefly,glucose oxidase(GOX)and chloroperoxidase(CPO)were chemically conjugated onto Ti_(3)C_(2)nanosheets,where the deoxygenation-activated drug tirapazamine(TPZ)was also loaded,and the Ti_(3)C_(2)-GOX-CPO/TPZ(TGCT)was embedded into nanosized cancer cell-derived membrane vesicles with high-expressed CD47(m_eTGCT).Due to biomimetic membrane camouflage and CD47 overexpression,m_eTGCT exhibited superior immune escape and homologous targeting capacities,which could effectively enhance the tumor preferential targeting and internalization.Once internalized into tumor cells,the cascade reaction of GOX and CPO could generate HClO for efficient EDT.Simultaneously,additional laser irradiation could accelerate the enzymic-catalytic reaction rate and increase the generation of singlet oxygen(~1O_(2)).Furthermore,local hypoxia environment with the oxygen depletion by EDT would activate deoxygenation-sensitive prodrug for additional chemotherapy.Consequently,m_eTGCT exhibits amplified synergistic therapeutic effects of tumor phototherapy,EDT and chemotherapy for efficient tumor inhibition.This intelligent cascaded-enzyme nanoreactor provides a promising approach to achieve concurrent and significant antitumor therapy.
文摘Yolk‐shell structured nanoparticles are of immense scientific and technological interests because of their unique architecture and myriad of applications.This review summarizes recent progresses in the use of yolk‐shell structured nanoparticles as nanoreactors for various chemical reactions.A very brief overview of synthetic strategies is provided with emphasis on recent research progress in the last five years.Catalytic applications of these yolk‐shell structured nanoreactors are then discussed by covering photocatalysis,methane reforming and electrochemical conversion.The state of the art research and perspective in future development are also highlighted.
基金support from the DFG through SFB 951 Hybrid Inorganic/Organic Systems for OptoElectronics(HIOS)funding by the European Research Council(ERC)Consolidator Grant with Project Number 646659-NANOREACTORthe Joint Lab for Structural Research at the Integrative Research Institute for the Sciences(IRIS Adlershof).
文摘Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.
基金supported by the National Natural Science Foundation of China(No.52070182)the DNL Cooperation Found,CAS(No.DNL202004)+3 种基金the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL)(No.202206)Talents of Innovation and Entrepreneurship Project of Lanzhou,China(No.2022-RC-26)Major Program of the Lanzhou Institute of Chemical Physics,CAS(No.ZYFZFX-10)Key talent project of Gansu Province.
文摘SO_(2)poisoning is a common problem in the catalytic combustion of volatile organic compounds(VOCs).In this work,we took three-dimensionally ordered macroporous and mesoporous(3DOM)SiO_(2)as the nanoreactor to protect active sites from SO_(2)erosion in the catalytic combustion of benzene.Simultaneously,the confined growth of metal active nanoparticles in the multi-stage pore is also full of challenges.And we successfully confined Co_(3)O_(4)nanoparticles(NPs)in macroporous and mesoporous channels.Interestingly,the precursors’growth in the pore was controlled and nanoreactors with different pore sizes were prepared by adjusting the loading amount and preparation methods.It is discovered that the Co_(3)O_(4)NPs confined in 3DOM SiO_(2)nanoreactor showed superior sulfur and water resistance.Density functional theory(DFT)calculations verified that the Co-Si catalyst had high SO_(2)adsorption energy(-0.48 eV),which illustrated that SO_(2)was hard to attach to the surface of the Co-Si catalyst.The SiO_(2)nanoreactor had low SO_(2)adsorption energy(-5.15 eV),which indicated that SO_(2)was easily absorbed on SiO_(2)nanoreactor.This illustrated that the SiO_(2)nanoreactor could protect effectively active sites from SO_(2)erosion.
基金supported by the National High Level Talents Special Support Plan(X.C.)the National Natural Science Foundation of China(82272141 to X.C.)+4 种基金the“Young Talent Support Plan”of Xi’an Jiaotong University(X.C.)the Shaanxi Innovative Research Team of Science and Technology(S2023-ZC-TD-0152)the Natural Science Foundation of Shaanxi Province(2022JZ-48 to X.C.)the National Key Research and Development Program of China(2023YFC2509104 to X.C.)the Postdoctoral Science Foundation of China(2023M732812 to T.L.).
文摘Tumor microenvironment(TME),as the“soil”of tumor growth and metastasis,exhibits significant differences from normal physiological conditions.However,how to manipulate the distinctions to achieve the accurate therapy of primary and metastatic tumors is still a challenge.Herein,an innovative nanoreactor(AH@MBTF)is developed to utilize the apparent differences(copper concentration and H_(2)O_(2)level)between tumor cells and normal cells to eliminate primary tumor based on H_(2)O_(2)-dependent photothermal-chemodynamic therapy and suppress metastatic tumor through copper complexation.This nanoreactor is constructed using functionalized MSN incorporating benzoyl thiourea(BTU),triphenylphosphine(TPP),and folic acid(FA),while being co-loaded with horseradish peroxidase(HRP)and its substrate ABTS.During therapy,the BTU moieties on AH@MBTF could capture excessive copper(highly correlated with tumor metastasis),presenting exceptional anti-metastasis activity.Simultaneously,the complexation between BTU and copper triggers the formation of cuprous ions,which further react with H_(2)O_(2)to generate cytotoxic hydroxyl radical(•OH),inhibiting tumor growth via che-modynamic therapy.Additionally,the stepwise targeting of FA and TPP guides AH@MBTF to accurately accu-mulate in tumor mitochondria,containing abnormally high levels of H_(2)O_(2).As a catalyst,HRP mediates the oxidation reaction between ABTS and H_(2)O_(2)to yield activated ABTS•^(+).Upon 808 nm laser irradiation,the activated ABTS•^(+)performs tumor-specific photothermal therapy,achieving the ablation of primary tumor by raising the tissue temperature.Collectively,this intelligent nanoreactor possesses profound potential in inhib-iting tumor progression and metastasis.
基金funded by the National Key Research and Development Program of China,grant number 2023YFD1700303.
文摘Titanium dioxide(TiO_(2))hollow nanoparticles present significant potential for photocatalytic applications while their straightforward preparation with precise structure control is still challenging.This work reports the approach to preparing tunable hollow TiO_(2) nanospheres by utilization of spherical polyelectrolyte brushes(SPB)as nanoreactors and templates.During the preparation,the evolution of the structure was characterized by small angle X-ray scattering(SAXS),and in combination with dynamic light scattering and transmission electron microscopy.The formation of TiO_(2) shell within the brush(SPB@TiO_(2))is confirmed by the significant increase of the electron density,and its internal structure has been analyzed by fitting SAXS data,which can be influenced by Titanium precursors and ammonia concentration.After calcining SPB@TiO_(2) in a muffle furnace,hollow TiO_(2) nanospheres are produced,and their transition to the anatase crystal form is triggered,as confirmed by X-ray diffraction analysis.Utilizing the advantages of their hollow structure,these TiO_(2) nanospheres exhibit exceptional catalytic degradation efficiency of methylene blue(MB),tetracycline(TC),and 2,4-dichlorophenoxyacetic acid(2,4-D),and also demonstrate excellent recyclability.
基金supported by the National Natural Science Foundation of China(No.22101289)Hundred Talents Programs in Chinese Academy of Sciences,the National Key Research and Development Program of China(No.2021YFA1502200)+2 种基金Bellwethers Project of Zhejiang Research and Development Plan(No.2022C01158)Ningbo S&T Innovation 2025 Major Special Program(Nos.2020Z107 and 2022Z205)Ningbo Yongjiang Talent Introduction Programme(Nos.2021A-111-G and 2021A-036-B).
文摘Covalent organic frameworks(COFs)-based nanoreactors have attracted broad interest in many fields due to their voidconfinement effects.However,the inherent drawback of conventional nanoreactors is the lack of internal active sites,which limits their widespread utilization.Herein,we report the construction of hierarchical COF(EB-TFP)nanoreactor with pre-synthesized polyoxometalates(POM,[PV_(2)W_(10)O_(40)]^(5–)(PV_(2)W_(10)))clusters encapsulated inside of COF(POM@COF).PV_(2)W_(10)@EB-TFP anchors nucleophilic-group(Br–ions)and PV_(2)W_(10)anion cluster within the COF framework via electrostatic interactions,which not only simplifies the reaction system but also enhances catalytic efficiency.The reaction performance of the PV_(2)W_(10)@EB-TFP nanoreactor can be tuned to achieve excellent catalytic activity in CO_(2)cycloaddition reaction(CCR)for~97.63%conversion and~100%selectivity under visible light irradiation.A mechanistic study based on density functional theory(DFT)calculations and insitu characterization was also carried out.In summary,we have reported a method for achieving the uniform dispersion of POM single clusters into COF nanoreactor,demonstrating the potential of POM@COF nanoreactor for synergistic photothermal catalytic CO_(2)cycloaddition.
基金support from the National Natural Science Foundation of China(NSFC,81971734,32071323,32271410,and 82202330)the National Key Research&Development Program of China(2019YFE0113600)+1 种基金the Science and Technology Projects in Fujian Province(2022FX1,2023Y4008)the Program for Innovative Research Team in Science and Technology in Fujian Province University,and the Scientific Research Funds of Huaqiao University(23BS113).
文摘The current strategy of co-delivering copper ions and disulfiram(DSF)to generate cytotoxic CuET faces limitations in achieving rapid and substantial CuET production,specifically in tumor lesions.To overcome this challenge,we introduce a novel burst-release cascade reactor composed of phase change materials(PCMs)encapsulating ultrasmall Cu_(2-x)Se nanoparticles(NPs)and DSF(DSF/Cu_(2-x)Se@PCM).Once triggered by second near-infrared(NIR-II)light irradiation,the reactor swiftly releases Cu_(2-x)Se NPs and DSF,enabling catalytic reactions that lead to the rapid and massive production of Cu_(2-x)Se-ET complexes,thereby achieving in situ chemotherapy.The mechanism of the burst reaction is due to the unique properties of ultrasmall Cu_(2-x)Se NPs,including their small size,multiple defects,and high surface activity.These characteristics allow DSF to be directly reduced and chelated on the surface defect sites of Cu_(2-x)Se,forming Cu_(2-x)Se-ET complexes without the need for copper ion release.Additionally,Cu_(2-x)Se-ET has demonstrated a similar(to CuET)anti-tumor activity through increased autophagy,but with even greater potency due to its unique two-dimensional-like structure.The light-triggered cascade of interlocking reactions,coupled with in situ explosive generation of tumor-suppressive substances mediated by the size and valence of Cu_(2-x)Se,presents a promising approach for the development of innovative nanoplatforms in the field of precise tumor chemotherapy.
基金Acknowledgements This work was financially supported by the National Natural Science Foundation of China (Nos. 21373208, 91545204, 21688102, and 21621063), and Ministry of Science and Technology of China (Nos. 2016YFA0200200, 2013CB834603, and 2013CB933100), and the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB17020200).
文摘Core-shell nanostructures consisting of active metal cores and protective shells often exhibit enhanced catalytic performance, in which reactants can access a small part of the core surfaces through the pores in the shells. In this study, we show that Pt nanoparticles (NPs) can be embedded into few-layer hexagonal boron nitride (h-BN) overlayers, forming Pt@h-BN core-shell nanocatalysts. The h-BN shells not only protect the Pt NPs under harsh conditions but also allow gaseous molecules such as CO and 02 to access a large part of the Pt surfaces through a facile intercalation process. As a result, the Pt@h-BN nanostructures act as nanoreactors, and CO oxidation reactions with improved activity, selectivity, and stability occur at the core-shell interfaces. The confinement effect exerted by the h-BN shells promotes the Pt-catalyzed reactions. Our work suggests that two-dimensional shells can function as robust but flexible covers on nanocatalyst surfaces and tune the surface reactivity.
基金We gratefully acknowledge the financial support from the Beijing Natural Science Foundation(No.2182061)Science Foundation of China University of Petroleum,Bejing(No.2462019BJRC001).
文摘Carbon-carbon(C–C)coupling reactions represent one of the most powerful tools for the synthesis of complex natural products,bioactive molecules developed as drugs and agrochemicals.In this work,a multifunctional nanoreactor for C–C coupling reaction was successfully fabricated via encapsulating the core-shell Cu@Ni nanocubes into ZIF-8(Cu@Ni@ZIF-8).In this nanoreactor,Ni shell of the core-shell Cu@Ni nanocubes was the catalytical active center,and Cu core was in situ heating source for the catalyst by absorbing the visible light.Moreover,benefiting from the plasmonic resonance effect between Cu@Ni nanocubes encapsulated in ZIF-8,the absorption range of nanoreactor was widened and the utilization rate of visible light was enhanced.Most importantly,the microporous structure of ZIF-8 provided shape-selective of reactant.This composite was used for the highly shape-selective and stable photocatalysed C–C coupling reaction of boric acid under visible light irradiation.After five cycles,the nanoreactor still remained high catalytical activity.This Cu@Ni@ZIF-8 nanoreactor opens a way for photocatalytic C–C coupling reactions with shape-selectivity.
文摘Zinc oxide nanoparticles (ZnO NPs), as a new type of pH-sensitive drug carrier, have received much attention. ZnO NPs are stable at physiological pH, but can dissolve quickly in the acidic tumor environment (pH 〈 6) to generate cytotoxic zinc ions and reactive oxygen species (ROS). However, the protein corona usually causes the non-specific degradation of ZnO NPs, which has limited their application considerably. Herein, a new type of pH-sensitive nanoreactor (ZnO-DOX@F-mSiO2-FA), aimed at reducing the non-specific degradation of ZnO NPs, is presented. In the acidic tumor environment (pH 〈 6), it can release cytotoxic zinc ions, ROS, and anticancer drugs to kill cancer cells effectively. In addition, the fluorescence emitted from fluorescein isothiocyanate (FITC)-labeled mesoporous silica (F-mSiO2) and doxorubicin (DOX) can be used to monitor the release behavior of the anticancer drug. This report provides a new method to avoid the non-specific degradation of ZnO NPs, resulting in synergetic therapy by taking advantage of ZnO NPs-induced oxidative stress and targeted drug release.
基金This work was financially supported by National Natural Science Foundation of China(Grant Nos.51702095,51702362,51722503,and 51621004)Natural Science Foundation of Hunan Province,China(Grant No.2018JJ3041)the scientific research project of National University of Defense Technology(Grant Nos.ZK19-27 and ZK17-03-61).
文摘Despite great progress of lithium-sulfur(Li-S)battery performance at the laboratory-level,both key parameters and challenges at cell scales to achieve practical high energy density require high-sulfur-loading cathodes and lean electrolytes.Herein,a novel carbon foam integrated by hollow carbon bubble nanoreactors with ultrahigh pore volume of 6.9 cm3·g−1 is meticulously designed for ultrahigh sulfur content up to 96 wt.%.Tailoring polysulfide trapping and ion/electron transport kinetics during the charge-discharge process can be achieved by adjusting the wall thickness of hollow carbon bubbles.And a further in-depth understanding of electrochemical reaction mechanism for the cathode is impelled by the in-situ Raman spectroscopy.As a result,the as-prepared cathode delivers high specific capacitances of 1,269 and 695 mAh·g−1 at 0.1 and 5 C,respectively.Furthermore,Li-S pouch cells with high areal sulfur loading of 6.9 mg·cm−2 yield exceptional practical energy density of 382 Wh·kg−1 under lean electrolyte of 3.5µL·mg−1,which demonstrates the great potential for realistic high-energy Li-S batteries.
基金financially supported by the National Natural Science Foundation of China (31422021, 51473109, and 81501585)National Basic Research Program of China (2014CB931900)+5 种基金Natural Science Foundation of Jiangsu Province of China (BK20150348)Natural Science Foundation of the Jiangsu Higher Education Institutions of China (15KJB310019)China Postdoctoral Science Foundation (2015M570475 and 2016T90496)Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)Jiangsu Key Laboratory of Translational Research and Therapy for Neuro-PsychoDiseases, Open Fund of CAS Key Laboratory of Nano-Bio Interface (16NBI02)Jiangsu Undergraduates Innovation and Entrepreneurship Program (20150285075Y)
文摘It remains a great challenge to explore the facile way to fabricate multi-component nanoparticles in theranostic nanomedicine. Herein, an albumin nanoreactor templated synthesis of theranostic Gd203/CuS hybrid nanodots (NDs) has been developed for multimodal imaging guided photothermal tumor ablation. Gd2O3/CuS NDs are found to possess particle size of 4.4 ± 1.1nm, enhanced longitudinal relaxivity, effective photothermal conversion of 45.5%, as well as remarkable near-infrared fluorescence (NIRF) from Cy7.5-conjugated on albumin corona. The Gd203/CuS NDs further exhibited good photostability, en- hanced cellular uptake, and preferable tumor accumulation. Thus, the Gd203/CuS NDs generate remarkable NIRF imag- ing and Tl-weighted magnetic resonance (MR) imaging, and simultaneously result in effective photothermal tumor ab- lation upon irradiation. The albumin nanoreactor provides a facile and general strategy to synthesize multifunctional nanoparticles for cancer theranostics.
基金supported by the National Key R&D Program of China(No.2019YFA0210103)the National Natural Science Foundation of China(No.21974039)+3 种基金China Postdoctoral Science Foundation(Nos.2020TQ0092 and 2020M682537)the Science and Technology Innovation Program of Hunan Province(No.2020RC2019)the Special Funds for the Construction of Innovative Provinces in Hunan Province(No.2019RS1031)the Opening Fund of Key Laboratory of Chemical Biology and Traditional Chinese Medicine Research(Hunan Normal University),the Ministry of Education.
文摘Bioorthogonal cleavage reaction-triggered prodrug activation by the pretargeted methods can achieve accurate cancer therapy.However,the click and release efficiency of these methods in vivo is limited by the space-time dislocation of bioorthogonal prodrug-trigger pairs within the tumor area,caused by their asynchronous administration and inconsistent accumulation for most delivery systems.We herein created a nanovoid-confinement and click-activated(NCCA)core–shell nanoreactor by incorporating prodrugs within zeolitic imidazolate framework-90(ZIF-90)as core and coating tetrazine-based covalent organic framework(COF)as shell.After surface modification of aptamer polymer,the NCCA nanoreactor enabled the sufficient delivery of photodynamic prodrugs within tumor.Notably,the core of ZIF-90 was decomposed by tumor acidic environment,inducing the high-efficiency activation of photodynamic prodrugs via nanoconfined bioorthogonal reaction with tetrazine-based COF shell.As a result,such photodynamic agents are efficiently and safely accumulated into tumor and specifically activated for precise photodynamic therapy of cancer cells and tumor bearing mice with minimizing toxic side effect.Taken together,such NCCA nanoreactor clearly demonstrates the critical feasibility to realize the synchronous delivery of both prodrugs and triggers for precise treatment,which most of delivery systems are not able to afford.
基金supported by the National Natural Science Foundation of China(Nos.U1904215,21671170 and 21673203)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)+4 种基金Program for New Century Excellent Talents of the University in China(No.NCET-13-0645)the Six Talent Plan(No.2015XCL-030)Qinglan Project of JiangsuProgram for Colleges Natural Science Research in Jiangsu Province(No.18KJB150036)the Science and Technology Innovation Foster Foundation of Yangzhou University(No.2016CXJ010)。
文摘Metallic phosphides as a crucial class of metal-like compounds show high electric conductivity and electrochemical properties.It is of significant benefit to understanding the relationship between the electrocatalytic performance and phosphating degree of precursors.In this work,using Co3O4@SiO2 as precursor,core-shell structured CoP@SiO2 nanoreactors with outstanding oxygen evolution reaction performance were synthesized through a facile calcination method.The electrocatalytic performance of CoP@SiO2 modified electrode that treated with 500 mg NaH2PO2 was greatly enhanced.The obtained product displays a low overpotential of 280 mV at a current density of 10 mA/cm2 and a Tafel value 89 mV/dec in alkaline conditions.The easy available CoP@SiO2 with outstanding catalytic performance and stability possesses huge potential in future electrochemical applications.