Pub Date : 2025-02-27DOI: 10.1007/s00604-025-07051-x
Yutong Wang, Yizhi Liu, Xiao Liang, Zhiyuan Liu, Yaling Yang
This study successfully developed a colorimetric/SERS dual-mode sensor for determining acrylamide in baked goods based on the excellent peroxidase-like activity and Raman activity of Fe-PHS@Au–Ag-Au Janus NPs. In colorimetric mode, the thiol-ene Michael addition between acrylamide (AA) and glutathione (GSH) efficiently eliminates GSH-induced peroxidase-like activity inhibition. The peroxidase-like activity of Fe-PHS@Au–Ag-Au Janus NPs gradually recovered, and the blue color of the solution gradually deepened with the increase in AA dosage. In surface-enhanced Raman spectroscopy (SERS), Apt-Fe-PHS@Au–Ag-Au Janus NPs can selectively capture AA and bind specifically, leading to the dissociation of Apt and Fe-PHS@Au–Ag-Au Janus NPs. The Raman activity of Apt-Fe-PHS@Au–Ag-Au Janus NPs decreases due to the dissociation of Apt. The dual-mode sensor was utilized for the determination of acrylamide in the concentrations range from 0.05 to 20 µg·L−1 with detection limits of 0.06 µg·L−1 (SERS) and 0.01 µg·L−1 (colorimetric). The recovery in baked samples was between 91.0 and 108.0%.
Graphical Abstract
{"title":"A colorimetric/SERS dual-mode sensor based on ferric ion-dopamine@Au–Ag-Au Janus NPs for acrylamide determination in baked goods","authors":"Yutong Wang, Yizhi Liu, Xiao Liang, Zhiyuan Liu, Yaling Yang","doi":"10.1007/s00604-025-07051-x","DOIUrl":"10.1007/s00604-025-07051-x","url":null,"abstract":"<div><p>This study successfully developed a colorimetric/SERS dual-mode sensor for determining acrylamide in baked goods based on the excellent peroxidase-like activity and Raman activity of Fe-PHS@Au–Ag-Au Janus NPs. In colorimetric mode, the thiol-ene Michael addition between acrylamide (AA) and glutathione (GSH) efficiently eliminates GSH-induced peroxidase-like activity inhibition. The peroxidase-like activity of Fe-PHS@Au–Ag-Au Janus NPs gradually recovered, and the blue color of the solution gradually deepened with the increase in AA dosage. In surface-enhanced Raman spectroscopy (SERS), Apt-Fe-PHS@Au–Ag-Au Janus NPs can selectively capture AA and bind specifically, leading to the dissociation of Apt and Fe-PHS@Au–Ag-Au Janus NPs. The Raman activity of Apt-Fe-PHS@Au–Ag-Au Janus NPs decreases due to the dissociation of Apt. The dual-mode sensor was utilized for the determination of acrylamide in the concentrations range from 0.05 to 20 µg·L<sup>−1</sup> with detection limits of 0.06 µg·L<sup>−1</sup> (SERS) and 0.01 µg·L<sup>−1</sup> (colorimetric). The recovery in baked samples was between 91.0 and 108.0%.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496947","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-27DOI: 10.1007/s00604-025-07054-8
Sameera Sh. Mohammed Ameen, Faisal Algethami, Khalid M. Omer
The development is shown of rod-shaped manganese-based metal–organic frameworks (Mn-MOFs) as hot- and cold-adapted oxidase-like nanozymes, with strong magnetic properties. These Mn-MOFs enable highly sensitive detection of nitrite ions, utilizing both convenient colorimetric ratio analysis and a visual instrument-free-based approach compatible with smartphone-based detection. The Mn-MOF showed multi-functional activity, such as cold/hot-adapted and magnetic oxidase-like activity, catalyzing the oxidation of chromogenic substrates 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxidized TMB (oxTMB). Mn-MOF shows high oxidase activity with Vmax of 1.39 × 10−8 M/s and Km of 0.068 mM for TMB oxidation. Nitrite ions further react with oxTMB to form a yellow color via diazotization resulting in the ratiometric change in absorbance (A652/A461). The color ratio is also quantified through the naked eye and/or smartphone app by analyzing RGB values, providing a rapid, portable, and cost-effective method for on-site detection. When applying Mn-MOF for smartphone-based nitrite detection, it performs excellent detection, with a linear range of 5.0–55.0 µM and a limit of detection of 0.18 µM, superior to most of the oxidase nanozyme-based nitrite sensing platforms. The detection platforms develop sensing probes using a reusable nanozyme that enables highly sensitive and selective detection of nitrite, featuring a broad linear range and a low limit of detection.
Graphical Abstract
{"title":"Magnetic rod-shaped Mn-based MOF as a multi-functional and recyclable platform for dual-mode ratiometric-based nitrite detection","authors":"Sameera Sh. Mohammed Ameen, Faisal Algethami, Khalid M. Omer","doi":"10.1007/s00604-025-07054-8","DOIUrl":"10.1007/s00604-025-07054-8","url":null,"abstract":"<div><p>The development is shown of rod-shaped manganese-based metal–organic frameworks (Mn-MOFs) as hot- and cold-adapted oxidase-like nanozymes, with strong magnetic properties. These Mn-MOFs enable highly sensitive detection of nitrite ions, utilizing both convenient colorimetric ratio analysis and a visual instrument-free-based approach compatible with smartphone-based detection. The Mn-MOF showed multi-functional activity, such as cold/hot-adapted and magnetic oxidase-like activity, catalyzing the oxidation of chromogenic substrates 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxidized TMB (oxTMB). Mn-MOF shows high oxidase activity with <i>V</i>max of 1.39 × 10<sup>−8</sup> M/s and <i>K</i>m of 0.068 mM for TMB oxidation. Nitrite ions further react with oxTMB to form a yellow color via diazotization resulting in the ratiometric change in absorbance (A<sub>652</sub>/A<sub>461</sub>). The color ratio is also quantified through the naked eye and/or smartphone app by analyzing RGB values, providing a rapid, portable, and cost-effective method for on-site detection. When applying Mn-MOF for smartphone-based nitrite detection, it performs excellent detection, with a linear range of 5.0–55.0 µM and a limit of detection of 0.18 µM, superior to most of the oxidase nanozyme-based nitrite sensing platforms. The detection platforms develop sensing probes using a reusable nanozyme that enables highly sensitive and selective detection of nitrite, featuring a broad linear range and a low limit of detection.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496948","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-26DOI: 10.1007/s00604-025-07040-0
Danni Sun, Tao Liu, Yiran Yao, Dezhao Kong, Chang Liu, Hua Ye, Qi Zhang, Shijie Li, Yaqi Li, Qiaoqiao Shi
A surface-enhanced Raman scattering (SERS) aptasensor was developed using gold nanostars (Au NSs) and Fe3O4@Au nanoparticles (NPs) for the highly sensitive detection of aflatoxin B1 (AFB1). Au NSs were modified by the Raman reporter 4-aminothiophenol (PATP) and then coupled with cDNA to act as the capture probes (Au NSs@PATP-cDNA). Fe3O4@Au NPs were modified with the AFB1 aptamer (AFB1 Apt) and used as signal probes (Fe3O4@Au NPs-AFB1 Apt). The SERS peak of PATP at 1078 cm−1 was used for quantitative analysis. When the core-satellite nanostructures (Fe3O4@Au NPs-AFB1 Apt/cDNA-Au NSs@PATP) were self-assembled by oligonucleotide hybridization, the SERS intensity was significantly enhanced. When AFB1 was present, AFB1 Apt specifically binds to AFB1, causing the Fe3O4@Au NPs-AFB1 Apt and Au NSs@PATP-cDNA to dissociate, resulting in a decrease in the SERS intensity measured after magnetic separation. Under optimal conditions, the limit of detection (LOD) of AFB1 can be reduced to 0.24 pg/mL. This is attributed to the high affinity of AFB1 Apt, excellent magnetic separation characteristics, and multiple SERS hotspots. The assay has been validated to perform well in recovery and accuracy by evaluating spiked samples (rice, corn, and wheat) and positive samples (corn, brown rice, and wheat).
Graphical Abstract
{"title":"A core-satellite self-assembled SERS aptasensor used for ultrasensitive detection of AFB1","authors":"Danni Sun, Tao Liu, Yiran Yao, Dezhao Kong, Chang Liu, Hua Ye, Qi Zhang, Shijie Li, Yaqi Li, Qiaoqiao Shi","doi":"10.1007/s00604-025-07040-0","DOIUrl":"10.1007/s00604-025-07040-0","url":null,"abstract":"<div><p>A surface-enhanced Raman scattering (SERS) aptasensor was developed using gold nanostars (Au NSs) and Fe<sub>3</sub>O<sub>4</sub>@Au nanoparticles (NPs) for the highly sensitive detection of aflatoxin B<sub>1</sub> (AFB<sub>1</sub>). Au NSs were modified by the Raman reporter 4-aminothiophenol (PATP) and then coupled with cDNA to act as the capture probes (Au NSs@PATP-cDNA). Fe<sub>3</sub>O<sub>4</sub>@Au NPs were modified with the AFB<sub>1</sub> aptamer (AFB<sub>1</sub> Apt) and used as signal probes (Fe<sub>3</sub>O<sub>4</sub>@Au NPs-AFB<sub>1</sub> Apt). The SERS peak of PATP at 1078 cm<sup>−1</sup> was used for quantitative analysis. When the core-satellite nanostructures (Fe<sub>3</sub>O<sub>4</sub>@Au NPs-AFB<sub>1</sub> Apt/cDNA-Au NSs@PATP) were self-assembled by oligonucleotide hybridization, the SERS intensity was significantly enhanced. When AFB<sub>1</sub> was present, AFB<sub>1</sub> Apt specifically binds to AFB<sub>1</sub>, causing the Fe<sub>3</sub>O<sub>4</sub>@Au NPs-AFB<sub>1</sub> Apt and Au NSs@PATP-cDNA to dissociate, resulting in a decrease in the SERS intensity measured after magnetic separation. Under optimal conditions, the limit of detection (LOD) of AFB<sub>1</sub> can be reduced to 0.24 pg/mL. This is attributed to the high affinity of AFB<sub>1</sub> Apt, excellent magnetic separation characteristics, and multiple SERS hotspots. The assay has been validated to perform well in recovery and accuracy by evaluating spiked samples (rice, corn, and wheat) and positive samples (corn, brown rice, and wheat).</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496817","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The preparation of UiO-66@CdTe@AuNPs composites is presented for the first time, which function as a photoelectrochemical (PEC) sensing matrix and are conjugated to a three-way junction (TWJ). We propose an antibody-based specific recognition-induced neighbor-joining reaction that initiates the assembly of two molecularly designed nucleic acid enzymes (MNAzymes), to release an oligonucleotide that hydrolyzes TWJ through the mechanism of a toehold-mediated strand displacement reaction (TSDR). Subsequently, a hybridization chain reaction application (HRCA)-based dendrimer is formed, which immobilizes a large number of quantum dots to generate a burst effect that reduces the photocurrent signal. As anticipated, the developed PEC biosensor showed excellent analytical performance for both m6A-RNA and m5C-RNA, with detection limits of 0.309 fM and 6.918 aM, respectively. The successful fabrication of this ultrasensitive and simultaneous PEC biosensor provides new insights for epigenetic research and the bioassay, mechanism investigation and clinical diagnosis of diseases associated with RNA methylation.
Graphical Abstract
{"title":"A novel photoelectrochemical strategy for ultrasensitive and simultaneous detection of 5-methylcytosine and N6-methyladenosine based on proximity binding-triggered assembly MNAzyme -mediated HRCA","authors":"Yue Hu, Mengshi Xia, Mimi Li, Lulu Li, Chenghong Li, Yi Liu, Lina Wang, Hui Huang, Lichao Fang, Kexing Peng, Huamin Liu, Xiaolong Wang, Junsong Zheng","doi":"10.1007/s00604-025-07033-z","DOIUrl":"10.1007/s00604-025-07033-z","url":null,"abstract":"<div><p> The preparation of UiO-66@CdTe@AuNPs composites is presented for the first time, which function as a photoelectrochemical (PEC) sensing matrix and are conjugated to a three-way junction (TWJ). We propose an antibody-based specific recognition-induced neighbor-joining reaction that initiates the assembly of two molecularly designed nucleic acid enzymes (MNAzymes), to release an oligonucleotide that hydrolyzes TWJ through the mechanism of a toehold-mediated strand displacement reaction (TSDR). Subsequently, a hybridization chain reaction application (HRCA)-based dendrimer is formed, which immobilizes a large number of quantum dots to generate a burst effect that reduces the photocurrent signal. As anticipated, the developed PEC biosensor showed excellent analytical performance for both m<sup>6</sup>A-RNA and m<sup>5</sup>C-RNA, with detection limits of 0.309 fM and 6.918 aM, respectively. The successful fabrication of this ultrasensitive and simultaneous PEC biosensor provides new insights for epigenetic research and the bioassay, mechanism investigation and clinical diagnosis of diseases associated with RNA methylation. </p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-26DOI: 10.1007/s00604-025-07041-z
Gleidson Thiago Sá Araújo, Lucas Costa Faustino, Rejane Maria Pereira Silva, Welter Cantanhêde, Everson Thiago Santos Gerôncio
A simple and cost-effective methodology for manufacturing a portable electroanalytical device is reported. The device is based on a graphite/polyvinyl chloride (PVC) paper-based electrode coupled to a miniaturized 3D-printed electrochemical cell (3DEC). The 3DEC was designed to ensure the reproducibility of the system by delimitating the paper-based graphite electrode (PGE) area. The disposable PGE was fabricated by paint-brushing a conductive ink based on graphite powder and toluene-free PVC glue, onto a kraft paper. Different weight proportions (wt%) of graphite/PVC were evaluated regarding mechanical stability and electrochemical behavior. Cyclic voltammetric (CV) analysis in the presence of the [Fe(CN)6]3−/4− redox probe has shown that as the wt% of graphite in the ink increased from 50 to 90%, a clear decrease in peak potential separation (ΔEp) and increase in current are observed, indicating an improvement in charge transfer kinetics. However, 90 wt% graphite electrodes have shown poor adhesion to the substrate and easy leaching due to the small amount of PVC (binder). Therefore, the best PGE was achieved using 80:20 wt% graphite/PVC ink (PGE8020). Moreover, scanning electron microscopy (SEM) images and energy dispersive spectroscopy (EDS) mapping revealed a rugous and more uniform deposition of the conductive ink containing 80 wt% graphite. As a proof of concept, the graphite/PVC ink-based disposable electrodes were employed for the detection of 3-nitro-L-tyrosine (3-NLT) in synthetic urine samples, showing a detection limit of 2.85 μmol L−1, and %recovery in synthetic urine between 97 and 109%, highlighting the reliability and applicability of the proposed approach.
Graphical Abstract
{"title":"Simple graphite/PVC ink-designed paper-based electrodes integrated with a 3D-printed electrochemical device for affordable analyses","authors":"Gleidson Thiago Sá Araújo, Lucas Costa Faustino, Rejane Maria Pereira Silva, Welter Cantanhêde, Everson Thiago Santos Gerôncio","doi":"10.1007/s00604-025-07041-z","DOIUrl":"10.1007/s00604-025-07041-z","url":null,"abstract":"<div><p> A simple and cost-effective methodology for manufacturing a portable electroanalytical device is reported. The device is based on a graphite/polyvinyl chloride (PVC) paper-based electrode coupled to a miniaturized 3D-printed electrochemical cell (3DEC). The 3DEC was designed to ensure the reproducibility of the system by delimitating the paper-based graphite electrode (PGE) area. The disposable PGE was fabricated by paint-brushing a conductive ink based on graphite powder and toluene-free PVC glue, onto a kraft paper. Different weight proportions (wt%) of graphite/PVC were evaluated regarding mechanical stability and electrochemical behavior. Cyclic voltammetric (CV) analysis in the presence of the [Fe(CN)<sub>6</sub>]<sup>3−/4−</sup> redox probe has shown that as the wt% of graphite in the ink increased from 50 to 90%, a clear decrease in peak potential separation (Δ<i>E</i><sub>p</sub>) and increase in current are observed, indicating an improvement in charge transfer kinetics. However, 90 wt% graphite electrodes have shown poor adhesion to the substrate and easy leaching due to the small amount of PVC (binder). Therefore, the best PGE was achieved using 80:20 wt% graphite/PVC ink (PGE8020). Moreover, scanning electron microscopy (SEM) images and energy dispersive spectroscopy (EDS) mapping revealed a rugous and more uniform deposition of the conductive ink containing 80 wt% graphite. As a proof of concept, the graphite/PVC ink-based disposable electrodes were employed for the detection of 3-nitro-L-tyrosine (3-NLT) in synthetic urine samples, showing a detection limit of 2.85 μmol L<sup>−1</sup>, and %recovery in synthetic urine between 97 and 109%, highlighting the reliability and applicability of the proposed approach.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A ratiometric fluorescence sensor for detecting Escherichia coli (E. coli) was fabricated based on the fluorescein isothiocyanate (FITC)–labeled zirconium (Zr)–tetraphenylporphyrin tetrasulfonic acid (TPPS) hydrate metal–organic frameworks (ZTMs@FITC). The ZTMs have strong red fluorescence emission at 683 nm, which can be quenched by Cu2+. E. coli can capture and convert external Cu2+ into Cu+ through its distinctive metabolic activities. To minimize environmental and instrumental influences and enhance detection precision, green FITC with an emission peak at 515 nm was utilized as the fluorescence labeling agent to fabricate the ratiometric fluorescence probe (ZTMs@FITC). The prepared ZTMs@FITC probe showed excellent performance in the detection of E. coli. As the concentration of E. coli increased, the fluorescence intensity at 683 nm (ZTMs, F683) increased considerably, while the fluorescence intensity at 515 nm (FITC, F515) decreased. By monitoring the increase in the ratio of F683 to F515, this sensor achieved rapid and sensitive detection of E. coli within the concentration range from 1.0 × 101 to 5.0 × 105 CFU/mL. The limit of detection was 6 CFU/mL. When observed under a 365 nm ultraviolet lamp, the fluorescence color of the solution changed from yellow to red. Additionally, the dual-signal ratiometric fluorescence method exhibited high selectivity for E. coli and was successfully utilized to detect E. coli in juice samples, demonstrating its practical application potential in food analysis.
Graphical Abstract
{"title":"Ratiometric fluorescence sensor for Escherichia coli detection using fluorescein isothiocyanate–labeled metal–organic frameworks","authors":"Duoduo Zhang, Xinyu Zhang, Mingshuang Liang, Xiuxiu Li, Heping Xiao, Dawei Cao, Xiubo Zhao","doi":"10.1007/s00604-025-07053-9","DOIUrl":"10.1007/s00604-025-07053-9","url":null,"abstract":"<div><p> A ratiometric fluorescence sensor for detecting <i>Escherichia coli (E. coli)</i> was fabricated based on the fluorescein isothiocyanate (FITC)–labeled zirconium (Zr)–tetraphenylporphyrin tetrasulfonic acid (TPPS) hydrate metal–organic frameworks (ZTMs@FITC). The ZTMs have strong red fluorescence emission at 683 nm, which can be quenched by Cu<sup>2+</sup>. <i>E. coli</i> can capture and convert external Cu<sup>2+</sup> into Cu<sup>+</sup> through its distinctive metabolic activities. To minimize environmental and instrumental influences and enhance detection precision, green FITC with an emission peak at 515 nm was utilized as the fluorescence labeling agent to fabricate the ratiometric fluorescence probe (ZTMs@FITC). The prepared ZTMs@FITC probe showed excellent performance in the detection of <i>E. coli.</i> As the concentration of <i>E. coli</i> increased, the fluorescence intensity at 683 nm (ZTMs, F<sub>683</sub>) increased considerably, while the fluorescence intensity at 515 nm (FITC, F<sub>515</sub>) decreased. By monitoring the increase in the ratio of F<sub>683</sub> to F<sub>515</sub>, this sensor achieved rapid and sensitive detection of <i>E. coli</i> within the concentration range from 1.0 × 10<sup>1</sup> to 5.0 × 10<sup>5</sup> CFU/mL. The limit of detection was 6 CFU/mL. When observed under a 365 nm ultraviolet lamp, the fluorescence color of the solution changed from yellow to red. Additionally, the dual-signal ratiometric fluorescence method exhibited high selectivity for <i>E. coli</i> and was successfully utilized to detect <i>E. coli</i> in juice samples, demonstrating its practical application potential in food analysis.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1007/s00604-025-07002-6
Adrián Sánchez-Visedo, Patricia Alcázar-González, Luis José Royo, Ana Soldado, Francisco Javier Ferrero, José Manuel Costa-Fernández, María Teresa Fernández-Argüelles
A novel and simple methodology is introduced that allows accurate and highly sensitive detection of microRNAs (miRNAs), taking advantage of an amplification strategy based on multicomponent nucleic acid enzymes (MNAzymes), combined with a fluorescence resonance energy transfer (FRET) phenomenon. For this purpose, a fluorescent dye (FAM) has been selected as an energy donor, while gold nanoparticles (AuNPs) are employed as energy acceptors, located close to each other through hybridisation with the substrate. The research object was miR146a, which is a biomarker whose overexpression in milk is associated with inflammation in bovine mammary glands caused by bovine mastitis. The presence of a genetic target activates the MNAzyme cleavage capability, splitting the substrate into two parts. Hence, the presence of the target increases the distance between donor and acceptor, recovering the quenched fluorescence. Experimental parameters have been optimised, achieving a limit of detection (LOD) of only 2.3 fM (highly competitive as compared to other similar approaches) and a wide linear response range between 15.9 fM and 10 nM. In addition, the proposed methodology allows discriminating miR146a from other similar miRNAs differing in a single base mismatch. Detection of miR146a has been successfully carried out in spiked raw milk samples.
Graphical Abstract
{"title":"Multicomponent nucleic acid enzymes as signal amplification strategy for the detection of microRNA based on fluorescence resonance energy transfer","authors":"Adrián Sánchez-Visedo, Patricia Alcázar-González, Luis José Royo, Ana Soldado, Francisco Javier Ferrero, José Manuel Costa-Fernández, María Teresa Fernández-Argüelles","doi":"10.1007/s00604-025-07002-6","DOIUrl":"10.1007/s00604-025-07002-6","url":null,"abstract":"<div><p>A novel and simple methodology is introduced that allows accurate and highly sensitive detection of microRNAs (miRNAs), taking advantage of an amplification strategy based on multicomponent nucleic acid enzymes (MNAzymes), combined with a fluorescence resonance energy transfer (FRET) phenomenon. For this purpose, a fluorescent dye (FAM) has been selected as an energy donor, while gold nanoparticles (AuNPs) are employed as energy acceptors, located close to each other through hybridisation with the substrate. The research object was miR146a, which is a biomarker whose overexpression in milk is associated with inflammation in bovine mammary glands caused by bovine mastitis. The presence of a genetic target activates the MNAzyme cleavage capability, splitting the substrate into two parts. Hence, the presence of the target increases the distance between donor and acceptor, recovering the quenched fluorescence. Experimental parameters have been optimised, achieving a limit of detection (LOD) of only 2.3 fM (highly competitive as compared to other similar approaches) and a wide linear response range between 15.9 fM and 10 nM. In addition, the proposed methodology allows discriminating miR146a from other similar miRNAs differing in a single base mismatch. Detection of miR146a has been successfully carried out in spiked raw milk samples.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s00604-025-07002-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143481051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25DOI: 10.1007/s00604-024-06932-x
Jianghua Liu, Yu Wang, Xinyue Zhang, Mingquan Huang, Guoliang Li
A novel direct lysis method combined with amplification-free CRISPR/Cas12a-SERS genosensor was for the first time developed to rapidly and sensitively identify meat adulteration. Notably, polystyrene (PS) microspheres, with distinct shrinking and swelling properties, were dexterously employed to encapsulate biological-silent Raman reporter 4-mercaptobenzonitrile (4-MBN) and act as a controlled-release signal probe. Target DNA activated the trans-cleavage activity of CRISPR/Cas12a towards ssDNA linked with PS microsphere to liberate the signal probe, which was able to release numerous Raman reporters after treatment with THF solution, resulting in high signal amplification. Through this platform, trace target DNA was deftly transformed into a sensitive Raman signal and could be on-site determined through a portable Raman equipment. Under optimized conditions, this strategy displayed good linearity in the range 1–450 ng/μL (R2 = 0.9943) and favorable sensitivity with limit of detection as low as 0.23 ng/μL without any pre-amplification. Moreover, it exhibited good applicability to on-site identification of commercial meat samples in complicated food matrix. In addition, DNA extraction by direct lysis and amplification-free detection realized ultrafast meat adulteration determination within 35 min from sampling to result. This method possessed great potential in rapid and on-site accurate determination of meat authenticity.
Graphical abstract
我们首次开发了一种新颖的直接裂解方法，结合无扩增的CRISPR/Cas12a-SERS基因传感器，可快速灵敏地识别肉类掺假。值得注意的是，该研究巧妙地利用了具有独特收缩和膨胀特性的聚苯乙烯（PS）微球来封装生物无声拉曼报告物 4-巯基苯甲腈（4-MBN），并将其作为可控释放信号探针。靶DNA激活了CRISPR/Cas12a对与PS微球相连的ssDNA的反式裂解活性，从而释放出信号探针，信号探针经四氢呋喃溶液处理后能够释放出大量拉曼报告物，从而实现高信号放大。通过这一平台，痕量目标 DNA 被巧妙地转化为灵敏的拉曼信号，并可通过便携式拉曼设备进行现场测定。在优化条件下，该方法在 1-450 ng/μL 范围内具有良好的线性关系（R2 = 0.9943），灵敏度高，检测限低至 0.23 ng/μL，无需任何预放大。此外，该方法还非常适用于在复杂的食品基质中对商用肉类样品进行现场鉴定。此外，通过直接裂解提取 DNA 和免扩增检测，实现了超快速肉类掺假检测，从取样到检测结果出来仅需 35 分钟。该方法在快速、现场准确测定肉类真伪方面具有巨大潜力。
{"title":"Direct lysis combined with amplification-free CRISPR/Cas12a-SERS genosensor for ultrafast and on-site identification of meat authenticity","authors":"Jianghua Liu, Yu Wang, Xinyue Zhang, Mingquan Huang, Guoliang Li","doi":"10.1007/s00604-024-06932-x","DOIUrl":"10.1007/s00604-024-06932-x","url":null,"abstract":"<div><p> A novel direct lysis method combined with amplification-free CRISPR/Cas12a-SERS genosensor was for the first time developed to rapidly and sensitively identify meat adulteration. Notably, polystyrene (PS) microspheres, with distinct shrinking and swelling properties, were dexterously employed to encapsulate biological-silent Raman reporter 4-mercaptobenzonitrile (4-MBN) and act as a controlled-release signal probe. Target DNA activated the <i>trans</i>-cleavage activity of CRISPR/Cas12a towards ssDNA linked with PS microsphere to liberate the signal probe, which was able to release numerous Raman reporters after treatment with THF solution, resulting in high signal amplification. Through this platform, trace target DNA was deftly transformed into a sensitive Raman signal and could be on-site determined through a portable Raman equipment. Under optimized conditions, this strategy displayed good linearity in the range 1–450 ng/μL (<i>R</i><sup>2</sup> = 0.9943) and favorable sensitivity with limit of detection as low as 0.23 ng/μL without any pre-amplification. Moreover, it exhibited good applicability to on-site identification of commercial meat samples in complicated food matrix. In addition, DNA extraction by direct lysis and amplification-free detection realized ultrafast meat adulteration determination within 35 min from sampling to result. This method possessed great potential in rapid and on-site accurate determination of meat authenticity.</p><h3>Graphical abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A fluorescent/colorimetric dual-mode biosensor was designed using CdTe QDs and CRISPR/Cas for the efficient and ultrasensitive detection of microcystin-leucine-arginine (MC-LR). The biosensor mainly activates the trans-cleavage activity of Cas12a through nucleic acid amplification technology, such as bidirectional rolling circle amplification (B-RCA), to perform signal conversion, release Ag+ from the cleaving hairpin, quench QD fluorescence, and perform signal presentation. The biosensor can perform fluorometric and colorimetric detection, enabling rapid field assays. It exhibits enhanced selectivity, increased sensitivity, and greater accuracy. The optimal conditions yield a detection range from 0.05 to 500 nM, with a minimum detectable concentration of 2.137 pM, surpassing the performance of traditional methods. The biosensor can effectively detect MC-LR in actual environmental samples. Overall, this study provided a general detection approach for the application of nucleic acid detection technology to detect trace pollutants in the environment.
{"title":"Fluorescent/colorimetric dual-mode for detecting of MC-LR using bidirectional RCA coupled with CdTe QDs","authors":"Weiqing Sun, Xinru Ren, Yijing Xiao, Bowen Li, Qing-ao Pang, Meili Yang, Rui Zhu, Zhiqiang Guo, Jinghua Yu, Jiadong Huang, Yu Wang, Su Liu","doi":"10.1007/s00604-025-06991-8","DOIUrl":"10.1007/s00604-025-06991-8","url":null,"abstract":"<div><p> A fluorescent/colorimetric dual-mode biosensor was designed using CdTe QDs and CRISPR/Cas for the efficient and ultrasensitive detection of microcystin-leucine-arginine (MC-LR). The biosensor mainly activates the trans-cleavage activity of Cas12a through nucleic acid amplification technology, such as bidirectional rolling circle amplification (B-RCA), to perform signal conversion, release Ag<sup>+</sup> from the cleaving hairpin, quench QD fluorescence, and perform signal presentation. The biosensor can perform fluorometric and colorimetric detection, enabling rapid field assays. It exhibits enhanced selectivity, increased sensitivity, and greater accuracy. The optimal conditions yield a detection range from 0.05 to 500 nM, with a minimum detectable concentration of 2.137 pM, surpassing the performance of traditional methods. The biosensor can effectively detect MC-LR in actual environmental samples. Overall, this study provided a general detection approach for the application of nucleic acid detection technology to detect trace pollutants in the environment.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143489415","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-24DOI: 10.1007/s00604-025-07045-9
Xiaoying Zhu, Qi Zhang, Xiaohua Qi, Yibo Feng, Mingqiang Zou, Qingbian Ma, Lin Zhang, Qiang Ma, Cong Wang
Peroxynitrite (ONOO−) plays a pivotal role in environmental pollution and ecosystem health, necessitating its detection for assessing ecological impacts and risks. Surface-enhanced Raman scattering (SERS) offers high sensitivity but is often limited by narrow Raman cross sections of analytes. Specialized molecules can aid SERS detection, but are complex to design and may cause nonspecific reactions in biological systems. Therefore, developing new SERS strategies is crucial for simpler, more accurate ONOO− detection. Herein, the shape instability of Ag nanomaterials in the hotspots, due to oxidation and dissolution of Ag atoms at the edges and corners, is investigated, and the detection of ONOO− is performed by SERS probes. ONOO− reacts first with the (111) facet, especially at the edges and corners. Consequently, the SERS signal of the adsorbed probe, Rhodamine 6G in hotspots can be used to monitor edge and corner dissolution that positively related to the ONOO− concentration. As a result, ONOO− concentration from 0.1 to 25 μM was detected, achieving a coefficient of determination of R2 = 0.9896. The method exhibits good reproducibility (RSD < 3.25%) and stability (> 7 days), and quantitative detection of ONOO− was achieved in bovine serum samples. Ag nanocubes exhibited an eightfold stronger response and higher precision compared to Ag nanoparticles in ONOO− detection. This simple detection technique offers a promising method for the accurate, quantitative detection of ONOO− in wide range of biological systems.
Graphical Abstract
{"title":"Unraveling the structural evolution of silver plasmonic hotspots for the detection of oxidative ONOO− radicals via SERS probe decay","authors":"Xiaoying Zhu, Qi Zhang, Xiaohua Qi, Yibo Feng, Mingqiang Zou, Qingbian Ma, Lin Zhang, Qiang Ma, Cong Wang","doi":"10.1007/s00604-025-07045-9","DOIUrl":"10.1007/s00604-025-07045-9","url":null,"abstract":"<div><p>Peroxynitrite (ONOO<sup>−</sup>) plays a pivotal role in environmental pollution and ecosystem health, necessitating its detection for assessing ecological impacts and risks. Surface-enhanced Raman scattering (SERS) offers high sensitivity but is often limited by narrow Raman cross sections of analytes. Specialized molecules can aid SERS detection, but are complex to design and may cause nonspecific reactions in biological systems. Therefore, developing new SERS strategies is crucial for simpler, more accurate ONOO<sup>−</sup> detection. Herein, the shape instability of Ag nanomaterials in the hotspots, due to oxidation and dissolution of Ag atoms at the edges and corners, is investigated, and the detection of ONOO<sup>−</sup> is performed by SERS probes. ONOO<sup>−</sup> reacts first with the (111) facet, especially at the edges and corners. Consequently, the SERS signal of the adsorbed probe, Rhodamine 6G in hotspots can be used to monitor edge and corner dissolution that positively related to the ONOO<sup>−</sup> concentration. As a result, ONOO<sup>−</sup> concentration from 0.1 to 25 μM was detected, achieving a coefficient of determination of <i>R</i><sup>2</sup> = 0.9896. The method exhibits good reproducibility (RSD < 3.25%) and stability (> 7 days), and quantitative detection of ONOO<sup>−</sup> was achieved in bovine serum samples. Ag nanocubes exhibited an eightfold stronger response and higher precision compared to Ag nanoparticles in ONOO<sup>−</sup> detection. This simple detection technique offers a promising method for the accurate, quantitative detection of ONOO<sup>−</sup> in wide range of biological systems.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 3","pages":""},"PeriodicalIF":5.3,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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