Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composite...Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
The COVID-19 pandemic has caused severe global disasters,highlighting the importance of understanding the details and trends of epidemic transmission in order to introduce efficient intervention measures.While the wid...The COVID-19 pandemic has caused severe global disasters,highlighting the importance of understanding the details and trends of epidemic transmission in order to introduce efficient intervention measures.While the widely used deterministic compartmental models have qualitatively presented continuous “analytical” insight and captured some transmission features,their treatment usually lacks spatiotemporal variation.Here,we propose a stochastic individual dynamical(SID)model to mimic the random and heterogeneous nature of epidemic propagation.The SID model provides a unifying framework for representing the spatiotemporal variations of epidemic development by tracking the movements of each individual.Using this model,we reproduce the infection curves for COVID-19 cases in different areas globally and find the local dynamics and heterogeneity at the individual level that affect the disease outbreak.The macroscopic trend of virus spreading is clearly illustrated from the microscopic perspective,enabling a quantitative assessment of different interventions.Seemingly,this model is also applicable to studying stochastic processes at the “meter scale”,e.g.,human society’s collective dynamics.展开更多
Epidemiological studies suggest a global decline in male fertility, which accounts for approximately50% of infertility cases in couples. Male infertility is a multifactorial and complex issue that may arise due to con...Epidemiological studies suggest a global decline in male fertility, which accounts for approximately50% of infertility cases in couples. Male infertility is a multifactorial and complex issue that may arise due to congenital, acquired, idiopathic, or other unknown factors[1].展开更多
Recent innovations in nanomaterials inspire abundant novel tumor-targeting CRISPR-based gene therapies.However,the therapeutic efficiency of traditional targeted nanotherapeutic strategies is limited by that the bioma...Recent innovations in nanomaterials inspire abundant novel tumor-targeting CRISPR-based gene therapies.However,the therapeutic efficiency of traditional targeted nanotherapeutic strategies is limited by that the biomarkers vary in a spatiotemporal-dependent manner with tumor progression.Here,we propose a self-amplifying logic-gated gene editing strategy for gene/H_(2)O_(2)-mediated/starvation multimodal cancer therapy.In this approach,a hypoxia-degradable covalent-organic framework(COF) is synthesized to coat a-ZIF-8 in which glucose oxidase(GOx) and CRISPR system are packaged.To intensify intracellular redox dyshomeostasis,DNAzymes which can cleave catalase mRNA are loaded as well.When the nano system gets into the tumor,the weakly acidic and hypoxic microenvironment degrades the ZIF-8@COF to activate GOx,which amplifies intracellular H^(+)and hypoxia,accelerating the nanocarrier degradation to guarantee available CRISPR plasmid and GOx release in target cells.These tandem reactions deplete glucose and oxygen,leading to logic-gated-triggered gene editing as well as synergistic gene/H_(2)O_(2)-mediated/starvation therapy.Overall,this approach highlights the biocomputing-based CRISPR delivery and underscores the great potential of precise cancer therapy.展开更多
Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1–3].However,de...Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1–3].However,despite their importance,current nanoelectrode preparations are highly restrained to flame/electrochemical etching,metal sputtering,electrochemical deposition,etc.[3],resulting in a limited range of materials(mainly gold,platinum and carbon)for potential-resolved detection of redox-active species(Table S1 online).The enrichment of preparation methods to introduce novel materials and mechanisms should prove significant for the development of nanoelectrodes.展开更多
Promethazine(PHZ)is used as a sedative in veterinary medicine,and its residue can threaten the health of human.The electrochemical detection of PHZ is suitable method for application in the field.However,the tradition...Promethazine(PHZ)is used as a sedative in veterinary medicine,and its residue can threaten the health of human.The electrochemical detection of PHZ is suitable method for application in the field.However,the traditional electroanalysis is difficult to perform directly in meat samples due to matrix interference.This work integrates magnetic solid-phase extraction and differential pulse voltammetry for highly sensitive and selective determination of PHZ in beef and beef liver for the first time.CoFe_(2)O_(4)/graphene coated with C_(18)-functionalized mesoporous silica(MG@mSiO_(2)-C_(18))is synthesized as dispersed magnetic adsorbent to extract PHZ.Magnetic glassy carbon electrode modified with nitrogen-doped hollow carbon microspheres(HCM)attracts the MG@mSiO_(2)-C_(18)with PHZ,and directly detects the PHZ without elution procedure.MG@mSiO_(2)-C_(18)can separate PHZ to avoid the interference of impurities on following detection,and also concentrate PHZ on magnetic electrode.Additionally,the electrode modification with HCM can amplify the electrochemical signal of PHZ.Finally,the integrated PHZ determination method exhibits a wide linear range from 0.08μmol/L to 300μmol/L with a low limit of detection of 9.8 nmol/L.The beef sample analysis presents excellent recovery,demonstrating that this protocol is promising for the rapid and onsite detection of PHZ in real meat samples。展开更多
Cancer cachexia is a multifactorial syndrome characterized by progressive weight loss and a disease process that nutritional support cannot reverse.Although progress has been made in preclinical research,there is stil...Cancer cachexia is a multifactorial syndrome characterized by progressive weight loss and a disease process that nutritional support cannot reverse.Although progress has been made in preclinical research,there is still a long way to go in translating research findings into clinical practice.One of the main reasons for this is that existing preclinical models do not fully replicate the conditions seen in clinical patients.Therefore,it is important to understand the characteristics of existing preclinical models of cancer cachexia and pay close attention to the latest developments in preclinical models.The main models of cancer cachexia used in current research are allogeneic and xenograft models,genetically engineered mouse models,chemo-therapy drug-induced models,Chinese medicine spleen deficiency models,zebrafish and Drosophila models,and cellular models.This review aims to revisit and summarize the commonly used animal models of cancer cachexia by evaluating existing preclinical models,to provide tools and support for translational medicine research.展开更多
Inflammatory bowel disease(IBD)is an autoimmune gastrointestinal disease characterized by chronic relapsing inflammation of the intestine.Excessive pyroptosis that exists in the inflamed intestine can activate damage ...Inflammatory bowel disease(IBD)is an autoimmune gastrointestinal disease characterized by chronic relapsing inflammation of the intestine.Excessive pyroptosis that exists in the inflamed intestine can activate damage signals and aggravate local inflammation in IBD.Here,we designed an oral pyroptosis nanoinhibitor,DXMS@CuM@PPADT@PSS(DCMP),which can target intestinal lesions,and respond to reactive oxygen species(ROS)to release active sites and drugs at the lesion.DCMP can inhibit the activation of the nucleotide-binding domain and leucine-rich repeat family pyrin domain containing 3(NLRP3)inflammasomes by scavenging ROS,resulting in the down-regulation of gasdermin D(GSDMD)cleavage thus inhibiting pyroptosis.It also improved intestinal barrier function,decreased inflammatory cytokine levels,and increased the diversity of gut microbiota in mice with colitis.This work is believed to expand the biomedical application of nanomaterials for innate immunity modulation.展开更多
The cancer stem cell hypothesis provides a basis for prediction of the recurrence and risk of metastasis in breast cancer.However,the unique expression pattern of stemness markers and the presence of nonstem-like canc...The cancer stem cell hypothesis provides a basis for prediction of the recurrence and risk of metastasis in breast cancer.However,the unique expression pattern of stemness markers and the presence of nonstem-like cancer cells with varied phenotypes have brought great challenges to the characterization of breast cancer stem cells.To address these challenges,a phenotype-directed DNA nanomachine has been designed for high-accuracy labeling and in situ analysis of the stem cell-like subpopulation in breast cancer.The key for the design is to use cell surfaceanchored inputs to activate the nanomachine,which undergoes different branch migration pathways such that the signal strand can only be brought onto the cancer cells having the stem cell-like phenotype.Highly sensitive determination and single-step isolation of the stem cell-like subpopulation were achieved by incorporating functional groups into the signal strand such that the nanomachine was successfully applied in a tumor-bearing mouse model.Overall,the approach provides for a substantial improvement in capability for the analysis of the breast cancer stem cell-like subpopulation,and it is expected that the new approach will advance the use of DNA nanomachines in cancer-related studies.展开更多
In vitro toxicological assessment helps explore key fractions of particulate matter(PM)in association with the toxic mechanism.Previous studies mainly discussed the toxicity effects of the water-soluble and organic-so...In vitro toxicological assessment helps explore key fractions of particulate matter(PM)in association with the toxic mechanism.Previous studies mainly discussed the toxicity effects of the water-soluble and organic-soluble fractions of PM.However,the toxicity of insoluble fractions is relatively poorly understood,and the adsorption of proteins is rarely considered.In this work,the formation of protein corona on the surface of insoluble particles during incubation in a culture medium was investigated.It was found that highly abundant proteins in fetal bovine serum were the main components of the protein corona.The adsorbed proteins increased the dispersion stability of insoluble particles.Meanwhile,the leaching concentrations of some metal elements(e.g.,Cu,Zn,and Pb)from PM increased in the presence of proteins.The toxicity effects and potential mechanisms of the PM insoluble particle–protein corona complex on macrophage cells RAW264.7 were discussed.The results revealed that the PM insoluble particle–protein corona complex could influence the phagosome pathway in RAW264.7 cells.Thus,it promoted the intracellular reactive oxygen species generation and induced a greater degree of cell differentiation,significantly altering cell morphology.Consequently,this work sheds new light on the combination of insoluble particles and protein corona in terms of PM cytotoxicity assessment.展开更多
Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very power...Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very powerful analytical technique and has been widely used in such as clinical testing, biowarfare agent detection, and pharmaceutical analysis. This review focuses on the current trends of molecular recognition-based biosensing methods for pharmaceutical analysis since 2010. It introduces a background of ECL and presents the recent ECL developments in ECL immunoassay(ECLIA), immunosensors, enzyme-based biosensors, aptamer-based biosensors, and molecularly imprinted polymers(MIP)-based sensors. At last, the future perspective for these analytical methods is briefly discussed.展开更多
Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic an...Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic analysis has been a hot topic in recent years,especially for electrochemiluminescence(ECL).This paper describes a simple ECL method based on single gold microbeads to image lecithin.Lecithin reacts to produce hydrogen peroxide under the successive enzymatic reaction of phospholipase D and choline oxidase.ECL was generated by the electrochemical reaction between a luminol analog and hydrogen peroxide,and ECL signals were imaged by a camera.Despite the heterogeneity of single gold microbeads,their luminescence obeyed statistical regularity.The average luminescence of 30 gold microbeads is correlated with the lecithin concentration,and thus,a visualization method for analyzing lecithin was established.Calibration curves were constructed for ECL intensity and lecithin concentration,achieving detection limits of 0.05 m M lecithin.This ECL imaging platform based on single gold microbeads exhibits outstanding advantages,such as high throughput,versatility and low cost,and holds great potential in disease diagnostics,environmental monitoring and food safety.展开更多
Calcium-release-activated calcium(CARC)channels are one of the major pathways of calcium entry in non-excitable cells.Despite a decade or two of research,its regulatory mechanism is not yet thoroughly understood.The s...Calcium-release-activated calcium(CARC)channels are one of the major pathways of calcium entry in non-excitable cells.Despite a decade or two of research,its regulatory mechanism is not yet thoroughly understood.The slow progress is due to the complexity of its pores(i.e.,Orai)on one hand and the difficulty in capturing its regulatory complex on the other hand.As a result,possible gating mechanisms have often been speculated by exploring the structure and properties of constitutive open mutants.However,there is much debate about how they can truly reflect the gating of CRAC channels under physiological conditions.In the present study,we combined molecular dynamics simulations with free energy calculations to study three dOrai mutants(G170P,H206A,and P288A),and further calculated their current-voltage curves.Results show that these constructs adopt different approaches to maintain their conductive state.Meanwhile they have unique pore structures and distinctive rectification properties and ion selectivity for cations compared to wild-type pores.We conclude that although the mutants may partially capture the gating motion characteristics of wild-type pores,the information obtained from these mutants is likely not a true reflection of CRAC channel gating under physiological conditions.展开更多
Phospholipase A_(2)(PLA_(2))is a critical biomarker of many diseases.Among various fluorescent probes,the ratiometric ones have shown great promise because they can provide built-in calibration to avoid interference f...Phospholipase A_(2)(PLA_(2))is a critical biomarker of many diseases.Among various fluorescent probes,the ratiometric ones have shown great promise because they can provide built-in calibration to avoid interference from analyte-independent factors by simultaneously monitoring two or more fluorescence peaks.Herein,we develop a biomimetic membrane-coated ratiometric fluorescent nanoprobe for the detection of PLA_(2).In this design,silica nanoparticles modified with fluorescein isothiocyanate(FITC)are functionalized with a layer of biomimetic membrane that is loaded with Dil dye.Therefore,when the nanocomposite is illuminated by 488 nm incident light,in addition to the fluorescence of FITC centered at 522 nm,that of Dil peaked at 568 nm originating from the energy transfer from FITC to Dil can also be monitored,forming a ratiometric fluorescent nanoprobe.When the target PLA_(2)is added,FITC and Dil will no longer be in close proximity because it hydrolyzes the biomimetic membrane,cutting off the energy flow between the two dyes.Consequently,the ratiometric fluorescent signal of the nanoprobe is altered to quantitatively reflect the content of PLA_(2).This study provides an effective approach to PLA_(2)detection,and the biomimetic membrane-mediated ratiometric design is promising in developing a new generation of biosensors.展开更多
CaS phosphor activated with Dy ions is prepared by the solid-state diffusion method. The phosphor is characterized by x-ray powder diffraction, thermogravimetric analysis and photoiuminescence. Defect centres formed i...CaS phosphor activated with Dy ions is prepared by the solid-state diffusion method. The phosphor is characterized by x-ray powder diffraction, thermogravimetric analysis and photoiuminescence. Defect centres formed in CaS：Dy are studied using the technique of electron spin resonance. The thermoluminescence glow curve shows peaks at around 117℃ and 345℃. Irradiated CaS：Dy exhibits ESR lines due to defect centres. The thermal annealing behaviour of one of the defect centres appears to correlate with the TL peaks at 117℃ and 345℃. This centre is characterized by an isotropic g-value of 2.0035 and is assigned to an F^＋ centre.展开更多
The study aimed to achieve enhanced targeted cytotoxicity and cell-internalization of cisplatin-loaded deoxyribonucleic acid-nanothread(CPT-DNA-NT),mediated by scavenger receptors into HeLa cells.DNA-NT was developed ...The study aimed to achieve enhanced targeted cytotoxicity and cell-internalization of cisplatin-loaded deoxyribonucleic acid-nanothread(CPT-DNA-NT),mediated by scavenger receptors into HeLa cells.DNA-NT was developed with stiff-topology utilizing circular-scaffold to encapsulate CPT.Atomic force microscopy(AFM)characterization of the DNA-NT showed uniformity in the structure with a diameter of 50-150 nm and length of 300-600 nm.The successful fabrication of the DNA-NT was confirmed through native-polyacrylamide gel electrophoresis analysis,as large the molecular-weight(polymeric)DNA-NT did not split into constituting strands under applied current and voltage.The results of cell viability confirmed that blank DNA-NT had the least cytotoxicity at the highest concentration(512 nM)with a viability of 92%as evidence of its biocompatibility for drug delivery.MTT assay showed superior cytotoxicity of CPT-DNA-NT than that of the free CPT due to the depot release of CPT after DNA-NT internalization.The DNA-NT exhibited targeted cell internalizations with the controlled intracellular release of CPT(from DNA-NT),as illustrated in confocal images.Therefore,in vitro cytotoxicity assessment through flow cytometry showed enhanced apoptosis(72.7%)with CPT-DNA-NT(compared to free CPT;64.4%).CPT-DNA-NT,being poly-anionic,showed enhanced endocytosis via scavenger receptors.展开更多
Single nanoparticle(NP)collisions technique has been widely employed in electrocatalysis.However,the short collision duration of single NPs hinders the further improvement in their electrocatalytic performance.Here,to...Single nanoparticle(NP)collisions technique has been widely employed in electrocatalysis.However,the short collision duration of single NPs hinders the further improvement in their electrocatalytic performance.Here,to increase the dynamic collision duration of single NPs in the electron tunneling region,enhanced near-wall hindered diffusion is introduced in the stochastic collision process by coupling a Au ultramicroelectrode(UME)with a confined microchannel.In the case of single palladium nanoparticle(Pd NP)collisions for the hydrogen evolution reaction(HER),the hydrodynamic trapping confined in the microchannel effectively permits the activation of the HER on the single Pd NPs.The microchannel-based Au UME is promising in the application of single-NP collisions to energy conversion.展开更多
A rapid sol-gel method for preparing hydroxyapatite nanoparticles(nHAP) has been developed. Three different sets of experimental conditions, in terms of solvents(water and ethanol), synthesis temperatures(25, 40 and 6...A rapid sol-gel method for preparing hydroxyapatite nanoparticles(nHAP) has been developed. Three different sets of experimental conditions, in terms of solvents(water and ethanol), synthesis temperatures(25, 40 and 60℃), and microwave irradiation(on and off) were explored. Crystal phase composition, functional groups and morphology of the products were characterized by thermogravimetric analysis(TGA), X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FT-IR), scanning electron microscopy(SEM) and transmission electron microscopy(TEM). The solvent and temperature were optimized based on product properties. Most importantly, the microwave-assisted method(with little to no ageing necessary) was much faster than the conventional methods(with slow ageing processes needing from hours to days), while affording pure nHAP with virtually identical morphological and structural properties. This study represents a practical application of the powerful microwave technique in synthesis of nHAP, offering guidance on the selection of optimum experiment conditions.展开更多
The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐trip...The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐triplex(G‐tri).The results presented herein not only confirm that the structural integrity of the 3'‐end G‐quartet is necessary for G4s to be catalytically competent but also show how to remediate G‐vacancy‐mediated catalytic activity losses via the addition of guanine surrogates in an approach referred to as G‐vacancy complementation strategy that is applicable to parallel G4s only.Furthermore,this study demonstrates that the terminal G‐quartet could act as a proximal coordinating group and cooperate with the flanking nucleotide to activate the hemin cofactor.展开更多
基金We acknowledge the support from the National Key Research and Development Program of China(Grant No.2022YFA1405000)the Natural Science Foundation of Jiangsu Province,Major Project(Grant No.BK20212004)+1 种基金the National Natural Science Foundation of China(Grant No.62374083)the State Key Laboratory of Analytical Chemistry for Life Science(Grant No.5431ZZXM2205).
文摘Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
基金supported by the National Natural Science Foundation of China(Grant No.22273034)the Frontiers Science Center for Critical Earth Material Cycling of Nanjing University。
文摘The COVID-19 pandemic has caused severe global disasters,highlighting the importance of understanding the details and trends of epidemic transmission in order to introduce efficient intervention measures.While the widely used deterministic compartmental models have qualitatively presented continuous “analytical” insight and captured some transmission features,their treatment usually lacks spatiotemporal variation.Here,we propose a stochastic individual dynamical(SID)model to mimic the random and heterogeneous nature of epidemic propagation.The SID model provides a unifying framework for representing the spatiotemporal variations of epidemic development by tracking the movements of each individual.Using this model,we reproduce the infection curves for COVID-19 cases in different areas globally and find the local dynamics and heterogeneity at the individual level that affect the disease outbreak.The macroscopic trend of virus spreading is clearly illustrated from the microscopic perspective,enabling a quantitative assessment of different interventions.Seemingly,this model is also applicable to studying stochastic processes at the “meter scale”,e.g.,human society’s collective dynamics.
基金supported by National Natural Science Foundation of China [Grant no. 22276093, 31901182,31870492]Jiangsu Science and Technology Association-Young Scientific and Technological Talent Support Project [TJ-2022-054]Postgraduate Research&Practice Innovation Program of Jiangsu Province [KYCX22_0124]。
文摘Epidemiological studies suggest a global decline in male fertility, which accounts for approximately50% of infertility cases in couples. Male infertility is a multifactorial and complex issue that may arise due to congenital, acquired, idiopathic, or other unknown factors[1].
基金financially supported by the National Natural Science Foundation of China(21874066,and 82073288)the National Key R&D Program of China(2019YFA0709200)+5 种基金the Key Research and Development Program of Jiangsu Province(BE2021373,China)Jiangsu Provincial Medical Key Discipline Cultivation Unit(JSDW202239,China)the Natural Science Foundation of Jiangsu Province(BK20200336,China)the Fundamental Research Funds for Central Universities(China)the Program for Innovative Talents and Entrepreneur in Jiangsu(China)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_0146,China).
文摘Recent innovations in nanomaterials inspire abundant novel tumor-targeting CRISPR-based gene therapies.However,the therapeutic efficiency of traditional targeted nanotherapeutic strategies is limited by that the biomarkers vary in a spatiotemporal-dependent manner with tumor progression.Here,we propose a self-amplifying logic-gated gene editing strategy for gene/H_(2)O_(2)-mediated/starvation multimodal cancer therapy.In this approach,a hypoxia-degradable covalent-organic framework(COF) is synthesized to coat a-ZIF-8 in which glucose oxidase(GOx) and CRISPR system are packaged.To intensify intracellular redox dyshomeostasis,DNAzymes which can cleave catalase mRNA are loaded as well.When the nano system gets into the tumor,the weakly acidic and hypoxic microenvironment degrades the ZIF-8@COF to activate GOx,which amplifies intracellular H^(+)and hypoxia,accelerating the nanocarrier degradation to guarantee available CRISPR plasmid and GOx release in target cells.These tandem reactions deplete glucose and oxygen,leading to logic-gated-triggered gene editing as well as synergistic gene/H_(2)O_(2)-mediated/starvation therapy.Overall,this approach highlights the biocomputing-based CRISPR delivery and underscores the great potential of precise cancer therapy.
基金supported by the National Natural Science Foundation of China(21974059,22174063,22034003,and 21327902)the Fundamental Research Funds for the Central Universities(2022300285 and 020514380305)+1 种基金the Excellent Research Program of Nanjing University(ZYJH004)the State Key Laboratory of Analytical Chemistry for Life Science(5431ZZXM2203)。
文摘Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1–3].However,despite their importance,current nanoelectrode preparations are highly restrained to flame/electrochemical etching,metal sputtering,electrochemical deposition,etc.[3],resulting in a limited range of materials(mainly gold,platinum and carbon)for potential-resolved detection of redox-active species(Table S1 online).The enrichment of preparation methods to introduce novel materials and mechanisms should prove significant for the development of nanoelectrodes.
基金supported by the National Key R&D Program of China(No.2019YFC1605400)the National Natural Science Foundation of China(Nos.21874065 and 22176085)。
文摘Promethazine(PHZ)is used as a sedative in veterinary medicine,and its residue can threaten the health of human.The electrochemical detection of PHZ is suitable method for application in the field.However,the traditional electroanalysis is difficult to perform directly in meat samples due to matrix interference.This work integrates magnetic solid-phase extraction and differential pulse voltammetry for highly sensitive and selective determination of PHZ in beef and beef liver for the first time.CoFe_(2)O_(4)/graphene coated with C_(18)-functionalized mesoporous silica(MG@mSiO_(2)-C_(18))is synthesized as dispersed magnetic adsorbent to extract PHZ.Magnetic glassy carbon electrode modified with nitrogen-doped hollow carbon microspheres(HCM)attracts the MG@mSiO_(2)-C_(18)with PHZ,and directly detects the PHZ without elution procedure.MG@mSiO_(2)-C_(18)can separate PHZ to avoid the interference of impurities on following detection,and also concentrate PHZ on magnetic electrode.Additionally,the electrode modification with HCM can amplify the electrochemical signal of PHZ.Finally,the integrated PHZ determination method exhibits a wide linear range from 0.08μmol/L to 300μmol/L with a low limit of detection of 9.8 nmol/L.The beef sample analysis presents excellent recovery,demonstrating that this protocol is promising for the rapid and onsite detection of PHZ in real meat samples。
基金supported by grants from the National Natural Science Foundation of China (No.82070912,82370899,and 81773326)National Key Research and Development Program of China (2022YFF0710801).
文摘Cancer cachexia is a multifactorial syndrome characterized by progressive weight loss and a disease process that nutritional support cannot reverse.Although progress has been made in preclinical research,there is still a long way to go in translating research findings into clinical practice.One of the main reasons for this is that existing preclinical models do not fully replicate the conditions seen in clinical patients.Therefore,it is important to understand the characteristics of existing preclinical models of cancer cachexia and pay close attention to the latest developments in preclinical models.The main models of cancer cachexia used in current research are allogeneic and xenograft models,genetically engineered mouse models,chemo-therapy drug-induced models,Chinese medicine spleen deficiency models,zebrafish and Drosophila models,and cellular models.This review aims to revisit and summarize the commonly used animal models of cancer cachexia by evaluating existing preclinical models,to provide tools and support for translational medicine research.
基金supported by the National Natural Science Foundation of China(Nos.82270543,82170573,81770556 and 21874066)the National Key R&D Program of China(No.2019YFA0709200)+3 种基金the Key Research and Development Program of Jiangsu Province(No.BE2021373)the Natural Science Foundation of Jiangsu Province(No.BK20200336)the Fundamental Research Funds for Central Universities,and the Program for Innovative Talents and Entrepreneur in Jiangsu.All animal studies were approved by the Ethics Committee of Jinling Hospital(No.2021JLHDWLSZ-0010)Surgical specimens were collected from Department of Gastroenterology and Hepatology,General Hospital of Eastern Theater Command.The use of human biopsies was approved by the Ethics Committee of Jinling Hospital(No.2022DZKY-048-01).All patients enrolled were given informed written consent.
文摘Inflammatory bowel disease(IBD)is an autoimmune gastrointestinal disease characterized by chronic relapsing inflammation of the intestine.Excessive pyroptosis that exists in the inflamed intestine can activate damage signals and aggravate local inflammation in IBD.Here,we designed an oral pyroptosis nanoinhibitor,DXMS@CuM@PPADT@PSS(DCMP),which can target intestinal lesions,and respond to reactive oxygen species(ROS)to release active sites and drugs at the lesion.DCMP can inhibit the activation of the nucleotide-binding domain and leucine-rich repeat family pyrin domain containing 3(NLRP3)inflammasomes by scavenging ROS,resulting in the down-regulation of gasdermin D(GSDMD)cleavage thus inhibiting pyroptosis.It also improved intestinal barrier function,decreased inflammatory cytokine levels,and increased the diversity of gut microbiota in mice with colitis.This work is believed to expand the biomedical application of nanomaterials for innate immunity modulation.
基金the National Natural Science Foundation of China(grant nos.81972799 and 81871449)the Natural Science Foundation of Shanghai(grant no.23ZR1421400).
文摘The cancer stem cell hypothesis provides a basis for prediction of the recurrence and risk of metastasis in breast cancer.However,the unique expression pattern of stemness markers and the presence of nonstem-like cancer cells with varied phenotypes have brought great challenges to the characterization of breast cancer stem cells.To address these challenges,a phenotype-directed DNA nanomachine has been designed for high-accuracy labeling and in situ analysis of the stem cell-like subpopulation in breast cancer.The key for the design is to use cell surfaceanchored inputs to activate the nanomachine,which undergoes different branch migration pathways such that the signal strand can only be brought onto the cancer cells having the stem cell-like phenotype.Highly sensitive determination and single-step isolation of the stem cell-like subpopulation were achieved by incorporating functional groups into the signal strand such that the nanomachine was successfully applied in a tumor-bearing mouse model.Overall,the approach provides for a substantial improvement in capability for the analysis of the breast cancer stem cell-like subpopulation,and it is expected that the new approach will advance the use of DNA nanomachines in cancer-related studies.
基金supported by the National Natural Science Foundation of China(91643105,21874065,22176085).
文摘In vitro toxicological assessment helps explore key fractions of particulate matter(PM)in association with the toxic mechanism.Previous studies mainly discussed the toxicity effects of the water-soluble and organic-soluble fractions of PM.However,the toxicity of insoluble fractions is relatively poorly understood,and the adsorption of proteins is rarely considered.In this work,the formation of protein corona on the surface of insoluble particles during incubation in a culture medium was investigated.It was found that highly abundant proteins in fetal bovine serum were the main components of the protein corona.The adsorbed proteins increased the dispersion stability of insoluble particles.Meanwhile,the leaching concentrations of some metal elements(e.g.,Cu,Zn,and Pb)from PM increased in the presence of proteins.The toxicity effects and potential mechanisms of the PM insoluble particle–protein corona complex on macrophage cells RAW264.7 were discussed.The results revealed that the PM insoluble particle–protein corona complex could influence the phagosome pathway in RAW264.7 cells.Thus,it promoted the intracellular reactive oxygen species generation and induced a greater degree of cell differentiation,significantly altering cell morphology.Consequently,this work sheds new light on the combination of insoluble particles and protein corona in terms of PM cytotoxicity assessment.
文摘Electrogenerated chemiluminescence(electrochemiluminescence, ECL) generates species at electrode surfaces, which undergoes electron-transfer reactions and forms excited states to emit light. It has become a very powerful analytical technique and has been widely used in such as clinical testing, biowarfare agent detection, and pharmaceutical analysis. This review focuses on the current trends of molecular recognition-based biosensing methods for pharmaceutical analysis since 2010. It introduces a background of ECL and presents the recent ECL developments in ECL immunoassay(ECLIA), immunosensors, enzyme-based biosensors, aptamer-based biosensors, and molecularly imprinted polymers(MIP)-based sensors. At last, the future perspective for these analytical methods is briefly discussed.
基金supported by Anhui Provincial Natural Science Foundation(Grant Nos.2008085QB68 and 1808085QB29)Key Project of Provincial Natural Science Research Foundation of Anhui Universities(Grant Nos.KJ2018A0675 and KJ2018A0389)+1 种基金Foundation of State Key Laboratory of Analytical Chemistry for Life Science(Grant No.SKLACLS2003)Foundation of Henan Key Laboratory of Biomolecular Recognition and Sensing(Grant No.HKLBRSK1905)。
文摘Fast and high-throughput determination of drugs is a key trend in clinical medicine.Single particles have increasingly been adopted in a variety of photoanalytical and electroanalytical applications,and microscopic analysis has been a hot topic in recent years,especially for electrochemiluminescence(ECL).This paper describes a simple ECL method based on single gold microbeads to image lecithin.Lecithin reacts to produce hydrogen peroxide under the successive enzymatic reaction of phospholipase D and choline oxidase.ECL was generated by the electrochemical reaction between a luminol analog and hydrogen peroxide,and ECL signals were imaged by a camera.Despite the heterogeneity of single gold microbeads,their luminescence obeyed statistical regularity.The average luminescence of 30 gold microbeads is correlated with the lecithin concentration,and thus,a visualization method for analyzing lecithin was established.Calibration curves were constructed for ECL intensity and lecithin concentration,achieving detection limits of 0.05 m M lecithin.This ECL imaging platform based on single gold microbeads exhibits outstanding advantages,such as high throughput,versatility and low cost,and holds great potential in disease diagnostics,environmental monitoring and food safety.
基金supported by the National Natural Science Foundation of China(No.21773115,No.21833002,No.11771435,and No.22073110)the Natural Science Foundation of Jiangsu Province(No.BK20190056)the Fundamental Research Funds for the Central Universities(021514380018)。
文摘Calcium-release-activated calcium(CARC)channels are one of the major pathways of calcium entry in non-excitable cells.Despite a decade or two of research,its regulatory mechanism is not yet thoroughly understood.The slow progress is due to the complexity of its pores(i.e.,Orai)on one hand and the difficulty in capturing its regulatory complex on the other hand.As a result,possible gating mechanisms have often been speculated by exploring the structure and properties of constitutive open mutants.However,there is much debate about how they can truly reflect the gating of CRAC channels under physiological conditions.In the present study,we combined molecular dynamics simulations with free energy calculations to study three dOrai mutants(G170P,H206A,and P288A),and further calculated their current-voltage curves.Results show that these constructs adopt different approaches to maintain their conductive state.Meanwhile they have unique pore structures and distinctive rectification properties and ion selectivity for cations compared to wild-type pores.We conclude that although the mutants may partially capture the gating motion characteristics of wild-type pores,the information obtained from these mutants is likely not a true reflection of CRAC channel gating under physiological conditions.
基金supported by the National Natural Science Foundation of China(21904083)the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R43)+1 种基金the Fundamental Research Funds for the Central Universities(GK202201009,GK202101001,and GK202305001)the Innovation Capability Support Program of Shaanxi Province(2021TD-42).
文摘Phospholipase A_(2)(PLA_(2))is a critical biomarker of many diseases.Among various fluorescent probes,the ratiometric ones have shown great promise because they can provide built-in calibration to avoid interference from analyte-independent factors by simultaneously monitoring two or more fluorescence peaks.Herein,we develop a biomimetic membrane-coated ratiometric fluorescent nanoprobe for the detection of PLA_(2).In this design,silica nanoparticles modified with fluorescein isothiocyanate(FITC)are functionalized with a layer of biomimetic membrane that is loaded with Dil dye.Therefore,when the nanocomposite is illuminated by 488 nm incident light,in addition to the fluorescence of FITC centered at 522 nm,that of Dil peaked at 568 nm originating from the energy transfer from FITC to Dil can also be monitored,forming a ratiometric fluorescent nanoprobe.When the target PLA_(2)is added,FITC and Dil will no longer be in close proximity because it hydrolyzes the biomimetic membrane,cutting off the energy flow between the two dyes.Consequently,the ratiometric fluorescent signal of the nanoprobe is altered to quantitatively reflect the content of PLA_(2).This study provides an effective approach to PLA_(2)detection,and the biomimetic membrane-mediated ratiometric design is promising in developing a new generation of biosensors.
基金Supported by the National Natural Science Foundation of China under Grant No 20325516, and the Fund of National Grade Key laboratory of Tunable Laser Technology under Grant No 51472040JW1101.
文摘CaS phosphor activated with Dy ions is prepared by the solid-state diffusion method. The phosphor is characterized by x-ray powder diffraction, thermogravimetric analysis and photoiuminescence. Defect centres formed in CaS：Dy are studied using the technique of electron spin resonance. The thermoluminescence glow curve shows peaks at around 117℃ and 345℃. Irradiated CaS：Dy exhibits ESR lines due to defect centres. The thermal annealing behaviour of one of the defect centres appears to correlate with the TL peaks at 117℃ and 345℃. This centre is characterized by an isotropic g-value of 2.0035 and is assigned to an F^＋ centre.
基金supported by the China Scholarship Council(CSC)grant(Grant No.20180500458)。
文摘The study aimed to achieve enhanced targeted cytotoxicity and cell-internalization of cisplatin-loaded deoxyribonucleic acid-nanothread(CPT-DNA-NT),mediated by scavenger receptors into HeLa cells.DNA-NT was developed with stiff-topology utilizing circular-scaffold to encapsulate CPT.Atomic force microscopy(AFM)characterization of the DNA-NT showed uniformity in the structure with a diameter of 50-150 nm and length of 300-600 nm.The successful fabrication of the DNA-NT was confirmed through native-polyacrylamide gel electrophoresis analysis,as large the molecular-weight(polymeric)DNA-NT did not split into constituting strands under applied current and voltage.The results of cell viability confirmed that blank DNA-NT had the least cytotoxicity at the highest concentration(512 nM)with a viability of 92%as evidence of its biocompatibility for drug delivery.MTT assay showed superior cytotoxicity of CPT-DNA-NT than that of the free CPT due to the depot release of CPT after DNA-NT internalization.The DNA-NT exhibited targeted cell internalizations with the controlled intracellular release of CPT(from DNA-NT),as illustrated in confocal images.Therefore,in vitro cytotoxicity assessment through flow cytometry showed enhanced apoptosis(72.7%)with CPT-DNA-NT(compared to free CPT;64.4%).CPT-DNA-NT,being poly-anionic,showed enhanced endocytosis via scavenger receptors.
文摘Single nanoparticle(NP)collisions technique has been widely employed in electrocatalysis.However,the short collision duration of single NPs hinders the further improvement in their electrocatalytic performance.Here,to increase the dynamic collision duration of single NPs in the electron tunneling region,enhanced near-wall hindered diffusion is introduced in the stochastic collision process by coupling a Au ultramicroelectrode(UME)with a confined microchannel.In the case of single palladium nanoparticle(Pd NP)collisions for the hydrogen evolution reaction(HER),the hydrodynamic trapping confined in the microchannel effectively permits the activation of the HER on the single Pd NPs.The microchannel-based Au UME is promising in the application of single-NP collisions to energy conversion.
基金National Key Research Program of China(2016YFA0201700/2016YFA02017001)National Natural Science Foundation of China(31400813)
文摘A rapid sol-gel method for preparing hydroxyapatite nanoparticles(nHAP) has been developed. Three different sets of experimental conditions, in terms of solvents(water and ethanol), synthesis temperatures(25, 40 and 60℃), and microwave irradiation(on and off) were explored. Crystal phase composition, functional groups and morphology of the products were characterized by thermogravimetric analysis(TGA), X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FT-IR), scanning electron microscopy(SEM) and transmission electron microscopy(TEM). The solvent and temperature were optimized based on product properties. Most importantly, the microwave-assisted method(with little to no ageing necessary) was much faster than the conventional methods(with slow ageing processes needing from hours to days), while affording pure nHAP with virtually identical morphological and structural properties. This study represents a practical application of the powerful microwave technique in synthesis of nHAP, offering guidance on the selection of optimum experiment conditions.
文摘The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐triplex(G‐tri).The results presented herein not only confirm that the structural integrity of the 3'‐end G‐quartet is necessary for G4s to be catalytically competent but also show how to remediate G‐vacancy‐mediated catalytic activity losses via the addition of guanine surrogates in an approach referred to as G‐vacancy complementation strategy that is applicable to parallel G4s only.Furthermore,this study demonstrates that the terminal G‐quartet could act as a proximal coordinating group and cooperate with the flanking nucleotide to activate the hemin cofactor.
