Lateral flow immunoassay(LFIA)has become popular in laboratories,at-home testing,and medical diagnostics due to its minimal cost and user-friendliness.Nevertheless,conventional test strips based on colloidal gold can ...Lateral flow immunoassay(LFIA)has become popular in laboratories,at-home testing,and medical diagnostics due to its minimal cost and user-friendliness.Nevertheless,conventional test strips based on colloidal gold can only obtain qualitative or semi-quantitative results with low sensitivity.In this work,AuFe_(3)O_(4) dumbbell-like nanoparticles were synthesized and used as the LFIA labelling marker for highly sensitive colorimetric-photothermal dual-mode detection of SARS-CoV-2 spike(S)protein.The unique dumbbell structure of Au-Fe_(3)O_(4) NPs makes it possible to combine the best features of both Au NPs and Fe_(3)O_(4) NPs.The increased surface area of these NPs enhances their LSPR effect and photothermal effect,which achieves signal amplification to increase sensitivity.The Au-Fe_(3)O_(4) NPs modified with S protein antibody could identify S protein in samples,which were recognized and accumulated on T-line by another antibody,generating color band for qualitative colorimetric detection.The T-line was irradiated by laser to obtain temperature change for quantitative detection of photothermal.In optimized conditions,the detection limit was 1.22 pg/m L,three orders of magnitude more sensitive than colorimetric detection.Finally,the approach was performed on SARS-CoV-2 pseudovirus samples and outperformed traditional colloidal gold strips.This LFIA platform exhibits significant promise for practical implementation,as it can satisfy the need for low-cost,high-sensitivity,and home-based quantitative detection for respiratory infectious diseases.展开更多
Perovskite nanocrystals (NCs), which have emerged as a new class of phosphors with superb luminescence properties and bandgaps that can be easily tuned using chemical methods, have generated tremendous interest for ...Perovskite nanocrystals (NCs), which have emerged as a new class of phosphors with superb luminescence properties and bandgaps that can be easily tuned using chemical methods, have generated tremendous interest for a wide variety of applications where colloidal quantum dots have been very successful as carrier sources. In this study, self-assembled films of CsPbBr3 NCs were produced via drop casting of colloidal NCs onto glassy carbon electrodes (GCEs) to form an NC film-modified electrode. The possible fabrication process of the CsPbBr3 NCs films was discussed. We further studied the anodic electrochemiluminescence (ECL) behavior of the perovskite CsPbBr3 NCs film using cyclic voltammetry with tripropylamine (TPA) as a coreactant, and a possible ECL mechanism was proposed. Briefly, TPA was oxidized to produce strongly reducing radical spedes, which can react with electrochemically oxidized CsPbBr3 NCs to generate excited CsPbBr3 NCs* capable of light emission. The relative stability of the ECL emission of the CsPbBr3 NC films under aqueous conditions was also investigated, and it was found that they showed operational stability over the first three hours, indicating suitable reliability for application as sensing materials. The results suggested that semiconducting perovskite NCs have great potential for application in the ECL field.展开更多
Due to the serious harm of diabetes to human health,development of sensitive assays for glucose level is of high significance for early prevention and treatment of diabetes.Currently,most conventional enzyme-based glu...Due to the serious harm of diabetes to human health,development of sensitive assays for glucose level is of high significance for early prevention and treatment of diabetes.Currently,most conventional enzyme-based glucose sensors suffer from high cost and low stability due to the inherent defects of natural enzymes.Herein,we develop a pure nanozyme-based glucose detection method using Ag@Au core/shell triangular nanoplates(TNPs),which combines glucose oxidase(GOD)-and horseradish peroxidase(HRP)-like activities of the Au shell and inherent plasmonic properties of Ag TNPs.The sensing mechanism is based on the fact that the Au shell possessed GOD-like activity,enabling the oxidation of glucose to produce H2O2,which can further etch the silver core,leading to the decrease of absorbance at 800 nm and the color change from blue to colorless.Compared with the previous nanozymes-based glucose sensors,our method avoids the use of enzymes and organic chromogenic agent.Moreover,the stability of the Ag@Au core/shell TNPs is much better than that of Ag TNPs due to the protection by the coating of the Au shell.This method was successfully applied to the detection of urine samples from patients with diabetes,indicating its practical applicability for real sample analysis.展开更多
Colorimetry often suffers from deficiency in quantitative determination,susceptibility to ambient illuminance,and low sensitivity and visual resolution to tiny color changes.To offset these deficiencies,we incorporate...Colorimetry often suffers from deficiency in quantitative determination,susceptibility to ambient illuminance,and low sensitivity and visual resolution to tiny color changes.To offset these deficiencies,we incorporate deep machine learning into colorimetry by introducing a convolutional neural network(CNN)with powerful parallel processing,self-organization,and self-learning capabilities.As a proof of concept,a plasmonic nanosensor is proposed for the colorimetric detection of glucose by coupling Benedict’s reagent with gold nanoparticles(AuNPs),which relies on the assemble of AuNPs into dendritic nanochains by Cu2O.The distinct difference of refractive index between Cu2O and Au and the localized surface plasmon resonance coupling effect among AuNPs leads to a broad spectral shift as well as abundant color changes,thereby providing sufficient data for selflearning enabled by machine learning.The CNN is then used to fully diversify the learning and training of the images from standard samples under different ambient conditions and to obtain a classifier that can not only recognize tiny color changes that are imperceptible to human eyes,but also exhibit high accuracy and excellent anti-environmental interference capability.This classifier is then compiled as an application(APP)and implanted into a smartphone with Android environment.306 clinical urine samples were detected using the proposed method and the results showed a satisfactory correlation(87.6%)with that of a standard blood glucose test method.More importantly,this method can be generalized to other applications in colorimetry,and more broadly,in other scientific domains that involve image analysis and quantification.展开更多
Although magnetic stirring is frequently used to enhance the kinetics for adsorption,chemical and biochemical reactions,the introduction of stirrers inevitably leads to the adsorption of analytes and thus interferes w...Although magnetic stirring is frequently used to enhance the kinetics for adsorption,chemical and biochemical reactions,the introduction of stirrers inevitably leads to the adsorption of analytes and thus interferes with the efficiency of the chemical process or reaction.In this work,magnetic Fe_(3) O_(4) nanorods with tunable length-to-diameter ratio were synthesized via a hydrothermal method and used as templates for the in-situ depositing of MIL-100(Fe) and gold nanoparticles.Such nanorod-based material can not only function as an adsorbent,nanozyme,and a heterogeneous catalyst for corresponding applications but also serve as a magnetic nanostirrer to enhance kinetics.As a proof-of-concept,the capture of bacteria pathogen,mimic-peroxidase-based colorimetric detection of hydrogen peroxide,and the catalytic reduction of selected organic pollutants were conducted using the as-synthesized Fe_(3) O_(4)@MIL-100(Fe)-Au nanostirrer with and without magnetic field.The results show that the rates of bacteria capture,mimetic enzyme reaction and catalysis were tremendously expedited.We believe this magnetic field-assisted approach holds great promise for future applications,because,not only does it eliminate the use of external magnetic stirrers and thereby decrease the risk of foreign pollution but also,is adaptable for nanoscale reaction systems where conventional stirring is not applicable due to size limitations.展开更多
Abstract:As an important component of the atmosphere,ammonia(NH_(3))plays a very important role in maintaining the balance of environment.However,it is also one of the most toxic gases that can cause damage to the hum...Abstract:As an important component of the atmosphere,ammonia(NH_(3))plays a very important role in maintaining the balance of environment.However,it is also one of the most toxic gases that can cause damage to the human respiratory system and mucous membranes even at low concentrations.As such,development of highly sensitive and selective NH_(3)sensors is of high significance for environmental monitoring and health maintenance.Herein,we have synthesized Au@Ag@Ag Cl core-shell nanoparticles(NPs)by oxidative etching and precipitating Au@Ag core-shell NPs using FeCl3 and further used them as optical probes for the colorimetric detection of NH_(3).The sensing mechanism is based on the fact that the etching of NH_(3)on AgCl and Ag shell leads to the variations of ingredients and core-to-shell ratio of the Au@Ag@AgCl NPs,thereby inducing noticeable spectral and color changes.By replacing the outmost layer of Ag with AgCl,not only is the stability of the sensor against oxygen significantly enhanced,but also is the sensitivity of the method improved.The method exhibits good linear relationship for the detection of NH_(3)from 0 to 5000 mmol/L with the limit of detection of 6.4 mmol/L.This method was successfully applied to the detection of simulated air polluted by NH_(3),indicating its practical applicability for environmental monitoring.This method shows great potential for on-site NH_(3)detection particularly in remote area,where a simple,fast,low-cost,and easy-to-handle method is highly desirable.展开更多
Although many plasmonic nanosenosrs have been established for the detection of mercury(Ⅱ)(Hg^(2+)),few of them is feasible for analyzing natural samples with very complex matrices because of insufficient method selec...Although many plasmonic nanosenosrs have been established for the detection of mercury(Ⅱ)(Hg^(2+)),few of them is feasible for analyzing natural samples with very complex matrices because of insufficient method selectivity.To address this challenge,we propose an epitaxial and lattice-mismatch approach to the synthesis of a unique Au/Ag_(2)S dimeric nanostructure,which consists of an Au segment with excellent plasmonic characteristics,and a highly stable Ag_(2)S portion with minimum solubility product (K_(sp)(Ag_(2)S)=6.3×10^(-50)).The detection relies on the chemical conversion of Ag_(2)S to HgS when reacting with Hg^(2+),resulting in a red shift in the absorption band of the connecting Au NPs.The concurrent color changes of the solution from gray purple to dark green and finally to navy correlate well with Hg^(2+)concentration,thus enables UV-vis quantitation and a naked-eye readout of the Hg^(2+)concentration.This method exhibits superior selectivity towards Hg^(2+) over other interfering ions tested because Hg^(2+) is the only ion that can react with Ag_(2)S to form HgS with even smaller solubility product (K_(sp)(HgS)=4×10^(-53)).The detection limit of this method is 1.21μmol/L,calculated by the signal-to-noise of 3.The practicability of the method was verified by analyzing the Hg^(2+)in sewage water samples without sample pretreatment with satisfactory recoveries (93.1%-102.8%) and relative standard deviations (1.38%-2.89%).We believe this method holds great potential for on-the-spot detection of Hg^(2+) in environmental water samples with complex matrices.展开更多
基金supported by the Natural Scientific Foundation of Shandong(Nos.ZR2023MC039,ZR2022JQ07)the National Natural Science Foundation of China(No.21876206)+1 种基金the Fundamental Research Funds for the Central Universities(No.21CX06014A)the Taishan Scholarship of Shandong Province(No.tsqn202211080)。
文摘Lateral flow immunoassay(LFIA)has become popular in laboratories,at-home testing,and medical diagnostics due to its minimal cost and user-friendliness.Nevertheless,conventional test strips based on colloidal gold can only obtain qualitative or semi-quantitative results with low sensitivity.In this work,AuFe_(3)O_(4) dumbbell-like nanoparticles were synthesized and used as the LFIA labelling marker for highly sensitive colorimetric-photothermal dual-mode detection of SARS-CoV-2 spike(S)protein.The unique dumbbell structure of Au-Fe_(3)O_(4) NPs makes it possible to combine the best features of both Au NPs and Fe_(3)O_(4) NPs.The increased surface area of these NPs enhances their LSPR effect and photothermal effect,which achieves signal amplification to increase sensitivity.The Au-Fe_(3)O_(4) NPs modified with S protein antibody could identify S protein in samples,which were recognized and accumulated on T-line by another antibody,generating color band for qualitative colorimetric detection.The T-line was irradiated by laser to obtain temperature change for quantitative detection of photothermal.In optimized conditions,the detection limit was 1.22 pg/m L,three orders of magnitude more sensitive than colorimetric detection.Finally,the approach was performed on SARS-CoV-2 pseudovirus samples and outperformed traditional colloidal gold strips.This LFIA platform exhibits significant promise for practical implementation,as it can satisfy the need for low-cost,high-sensitivity,and home-based quantitative detection for respiratory infectious diseases.
基金This research was financially supported by the National Natural Science Foundation of China (No. 21675133), the Marine high-tech industry development projects of Fujian Province (No. 2015-19). We thank Professor John Hodgkiss of the City University of Hong Kong for polishing the English.
文摘Perovskite nanocrystals (NCs), which have emerged as a new class of phosphors with superb luminescence properties and bandgaps that can be easily tuned using chemical methods, have generated tremendous interest for a wide variety of applications where colloidal quantum dots have been very successful as carrier sources. In this study, self-assembled films of CsPbBr3 NCs were produced via drop casting of colloidal NCs onto glassy carbon electrodes (GCEs) to form an NC film-modified electrode. The possible fabrication process of the CsPbBr3 NCs films was discussed. We further studied the anodic electrochemiluminescence (ECL) behavior of the perovskite CsPbBr3 NCs film using cyclic voltammetry with tripropylamine (TPA) as a coreactant, and a possible ECL mechanism was proposed. Briefly, TPA was oxidized to produce strongly reducing radical spedes, which can react with electrochemically oxidized CsPbBr3 NCs to generate excited CsPbBr3 NCs* capable of light emission. The relative stability of the ECL emission of the CsPbBr3 NC films under aqueous conditions was also investigated, and it was found that they showed operational stability over the first three hours, indicating suitable reliability for application as sensing materials. The results suggested that semiconducting perovskite NCs have great potential for application in the ECL field.
基金supported by the National Natural Science Foundation of China(No.21876206)the Fundamental Research Funds for the Central Universities(No.18CX02037A)。
文摘Due to the serious harm of diabetes to human health,development of sensitive assays for glucose level is of high significance for early prevention and treatment of diabetes.Currently,most conventional enzyme-based glucose sensors suffer from high cost and low stability due to the inherent defects of natural enzymes.Herein,we develop a pure nanozyme-based glucose detection method using Ag@Au core/shell triangular nanoplates(TNPs),which combines glucose oxidase(GOD)-and horseradish peroxidase(HRP)-like activities of the Au shell and inherent plasmonic properties of Ag TNPs.The sensing mechanism is based on the fact that the Au shell possessed GOD-like activity,enabling the oxidation of glucose to produce H2O2,which can further etch the silver core,leading to the decrease of absorbance at 800 nm and the color change from blue to colorless.Compared with the previous nanozymes-based glucose sensors,our method avoids the use of enzymes and organic chromogenic agent.Moreover,the stability of the Ag@Au core/shell TNPs is much better than that of Ag TNPs due to the protection by the coating of the Au shell.This method was successfully applied to the detection of urine samples from patients with diabetes,indicating its practical applicability for real sample analysis.
基金the National Natural Science Foundation of China(No.21876206)the Shandong Key Fundamental Research Project(No.ZR202010280003)+1 种基金the Fundamental Research Funds for the Central Universities(No.18CX02037A)the Youth Innovation and Technology project of Universities in Shandong Province(No.2020KJC007).
文摘Colorimetry often suffers from deficiency in quantitative determination,susceptibility to ambient illuminance,and low sensitivity and visual resolution to tiny color changes.To offset these deficiencies,we incorporate deep machine learning into colorimetry by introducing a convolutional neural network(CNN)with powerful parallel processing,self-organization,and self-learning capabilities.As a proof of concept,a plasmonic nanosensor is proposed for the colorimetric detection of glucose by coupling Benedict’s reagent with gold nanoparticles(AuNPs),which relies on the assemble of AuNPs into dendritic nanochains by Cu2O.The distinct difference of refractive index between Cu2O and Au and the localized surface plasmon resonance coupling effect among AuNPs leads to a broad spectral shift as well as abundant color changes,thereby providing sufficient data for selflearning enabled by machine learning.The CNN is then used to fully diversify the learning and training of the images from standard samples under different ambient conditions and to obtain a classifier that can not only recognize tiny color changes that are imperceptible to human eyes,but also exhibit high accuracy and excellent anti-environmental interference capability.This classifier is then compiled as an application(APP)and implanted into a smartphone with Android environment.306 clinical urine samples were detected using the proposed method and the results showed a satisfactory correlation(87.6%)with that of a standard blood glucose test method.More importantly,this method can be generalized to other applications in colorimetry,and more broadly,in other scientific domains that involve image analysis and quantification.
基金financially supported by the National Natural Science Foundation of China (No.21876206)the Science and Technolgy Projects of Qingdao (No.21-1-4-sf-7-nsh)+2 种基金the National Key Technologies R&D Program of ChinaKey Projects of Intergovernmental International Innovation Cooperation (No.2018YFE0118200)the Shandong Key Research and Development Project (Nos.2019JZZY010506, ZR2020ZD13)。
文摘Although magnetic stirring is frequently used to enhance the kinetics for adsorption,chemical and biochemical reactions,the introduction of stirrers inevitably leads to the adsorption of analytes and thus interferes with the efficiency of the chemical process or reaction.In this work,magnetic Fe_(3) O_(4) nanorods with tunable length-to-diameter ratio were synthesized via a hydrothermal method and used as templates for the in-situ depositing of MIL-100(Fe) and gold nanoparticles.Such nanorod-based material can not only function as an adsorbent,nanozyme,and a heterogeneous catalyst for corresponding applications but also serve as a magnetic nanostirrer to enhance kinetics.As a proof-of-concept,the capture of bacteria pathogen,mimic-peroxidase-based colorimetric detection of hydrogen peroxide,and the catalytic reduction of selected organic pollutants were conducted using the as-synthesized Fe_(3) O_(4)@MIL-100(Fe)-Au nanostirrer with and without magnetic field.The results show that the rates of bacteria capture,mimetic enzyme reaction and catalysis were tremendously expedited.We believe this magnetic field-assisted approach holds great promise for future applications,because,not only does it eliminate the use of external magnetic stirrers and thereby decrease the risk of foreign pollution but also,is adaptable for nanoscale reaction systems where conventional stirring is not applicable due to size limitations.
基金supported by the Graduate Student Innovation Project of China University of Petroleum(East China)in 2020(No.YCX2020031)the financial support by the National Natural Science Foundation of China(Nos.21876206,21505157)+1 种基金the Fundamental Research Funds for the Central Universities(China University of Petroleum(East China),Nos.18CX02037A,20CX05015A)the Youth Innovation and Technology project of Universities in Shandong Province(No.2020KJC007)。
文摘Abstract:As an important component of the atmosphere,ammonia(NH_(3))plays a very important role in maintaining the balance of environment.However,it is also one of the most toxic gases that can cause damage to the human respiratory system and mucous membranes even at low concentrations.As such,development of highly sensitive and selective NH_(3)sensors is of high significance for environmental monitoring and health maintenance.Herein,we have synthesized Au@Ag@Ag Cl core-shell nanoparticles(NPs)by oxidative etching and precipitating Au@Ag core-shell NPs using FeCl3 and further used them as optical probes for the colorimetric detection of NH_(3).The sensing mechanism is based on the fact that the etching of NH_(3)on AgCl and Ag shell leads to the variations of ingredients and core-to-shell ratio of the Au@Ag@AgCl NPs,thereby inducing noticeable spectral and color changes.By replacing the outmost layer of Ag with AgCl,not only is the stability of the sensor against oxygen significantly enhanced,but also is the sensitivity of the method improved.The method exhibits good linear relationship for the detection of NH_(3)from 0 to 5000 mmol/L with the limit of detection of 6.4 mmol/L.This method was successfully applied to the detection of simulated air polluted by NH_(3),indicating its practical applicability for environmental monitoring.This method shows great potential for on-site NH_(3)detection particularly in remote area,where a simple,fast,low-cost,and easy-to-handle method is highly desirable.
基金supported by the National Natural Science Foundation of China(No.21876206)the Key Fundamental Project of Shandong Natural Science Foundation(No.ZR2020ZD13)+1 种基金the Science and Technology Projects of Qingdao(No.21–1–4-sf-7-nsh)the Youth Innovation and Technology project of Universities in Shandong Province(No.2020KJC007)。
文摘Although many plasmonic nanosenosrs have been established for the detection of mercury(Ⅱ)(Hg^(2+)),few of them is feasible for analyzing natural samples with very complex matrices because of insufficient method selectivity.To address this challenge,we propose an epitaxial and lattice-mismatch approach to the synthesis of a unique Au/Ag_(2)S dimeric nanostructure,which consists of an Au segment with excellent plasmonic characteristics,and a highly stable Ag_(2)S portion with minimum solubility product (K_(sp)(Ag_(2)S)=6.3×10^(-50)).The detection relies on the chemical conversion of Ag_(2)S to HgS when reacting with Hg^(2+),resulting in a red shift in the absorption band of the connecting Au NPs.The concurrent color changes of the solution from gray purple to dark green and finally to navy correlate well with Hg^(2+)concentration,thus enables UV-vis quantitation and a naked-eye readout of the Hg^(2+)concentration.This method exhibits superior selectivity towards Hg^(2+) over other interfering ions tested because Hg^(2+) is the only ion that can react with Ag_(2)S to form HgS with even smaller solubility product (K_(sp)(HgS)=4×10^(-53)).The detection limit of this method is 1.21μmol/L,calculated by the signal-to-noise of 3.The practicability of the method was verified by analyzing the Hg^(2+)in sewage water samples without sample pretreatment with satisfactory recoveries (93.1%-102.8%) and relative standard deviations (1.38%-2.89%).We believe this method holds great potential for on-the-spot detection of Hg^(2+) in environmental water samples with complex matrices.