Pub Date : 2025-01-01Epub Date: 2024-10-05DOI: 10.1016/j.talanta.2024.126985
Giorgia La Barbera, Marshal Spenser Shuler, Søren Hammershøj Beck, Per Holger Ibsen, Lars Joachim Lindberg, John Gásdal Karstensen, Lars Ove Dragsted
Genotoxicants originating from inflammation, diet, and environment can covalently modify DNA, possibly initiating the process of carcinogenesis. DNA adducts have been known for long, but the old methods allowed to target only a few known DNA adducts at a time, not providing a global picture of the "DNA adductome". DNA adductomics is a new research field, aiming to screen for unknown DNA adducts by high resolution mass spectrometry (HRMS). However, DNA adductomics presents several analytical challenges such as the need for high sensitivity and for the development of effective screening approaches to identify novel DNA adducts. In this work, a sensitive untargeted DNA adductomics method was developed by using ultra-high performance liquid chromatography (UHPLC) coupled via an ESI source to a quadrupole-time of flight mass spectrometric instrumentation. Mobile phases with ammonium bicarbonate gave the best signal enhancement. The MS capillary voltage, cone voltage, and detector voltage had most effect on the response of the DNA adducts. A low adsorption vial was selected for reducing analyte loss. Hybrid surface-coated analytical columns were tested for reducing adsorption of the DNA adducts. The optimized method was applied to analyse DNA adducts in calf thymus, cat colon, and human colon DNA by performing a MSE acquisition (all-ion fragmentation acquisition) and screening for the loss of deoxyribose and the nucleobase fragment ions. Fifty-four DNA adducts were tentatively identified, hereof 38 never reported before. This is the first untargeted DNA adductomics study on human colon tissue, and one of the few untargeted DNA adductomics studies in the literature reporting the identification of such a high number of unknowns. This demonstrates promising results for the application of this sensitive method in future human studies for investigating novel potential cancer-causing factors.
源于炎症、饮食和环境的基因毒性物质可对 DNA 进行共价修饰,从而可能引发致癌过程。人们对 DNA 加合物的了解由来已久,但以往的方法一次只能针对几种已知的 DNA 加合物,无法提供 "DNA 加合物组 "的全貌。DNA 加合物组学是一个新的研究领域,旨在通过高分辨质谱(HRMS)筛选未知的 DNA 加合物。然而,DNA加合物组学面临着一些分析挑战,如需要高灵敏度和开发有效的筛选方法来识别新型DNA加合物。本研究采用超高效液相色谱(UHPLC),通过ESI源与四极杆飞行时间质谱仪联用,开发了一种灵敏的非靶向DNA加合物组学方法。碳酸氢铵流动相的信号增强效果最佳。质谱毛细管电压、锥体电压和检测器电压对 DNA 加合物的反应影响最大。为减少分析物的损失,选择了低吸附瓶。测试了混合表面涂层分析柱,以减少 DNA 加合物的吸附。将优化后的方法应用于分析小牛胸腺、猫结肠和人类结肠 DNA 中的 DNA 加合物,方法是进行 MSE 采集(全离子碎片采集)并筛选脱氧核糖和核碱基碎片离子的损失。初步鉴定出 54 种 DNA 加合物,其中 38 种以前从未报道过。这是首次对人体结肠组织进行的非靶向DNA加合物组学研究,也是文献中少数几项非靶向DNA加合物组学研究之一,报告了如此多未知加合物的鉴定结果。这表明,在未来的人体研究中应用这种灵敏的方法来调查新的潜在致癌因素前景广阔。
{"title":"Development of an untargeted DNA adductomics method by ultra-high performance liquid chromatography coupled to high-resolution mass spectrometry.","authors":"Giorgia La Barbera, Marshal Spenser Shuler, Søren Hammershøj Beck, Per Holger Ibsen, Lars Joachim Lindberg, John Gásdal Karstensen, Lars Ove Dragsted","doi":"10.1016/j.talanta.2024.126985","DOIUrl":"10.1016/j.talanta.2024.126985","url":null,"abstract":"<p><p>Genotoxicants originating from inflammation, diet, and environment can covalently modify DNA, possibly initiating the process of carcinogenesis. DNA adducts have been known for long, but the old methods allowed to target only a few known DNA adducts at a time, not providing a global picture of the \"DNA adductome\". DNA adductomics is a new research field, aiming to screen for unknown DNA adducts by high resolution mass spectrometry (HRMS). However, DNA adductomics presents several analytical challenges such as the need for high sensitivity and for the development of effective screening approaches to identify novel DNA adducts. In this work, a sensitive untargeted DNA adductomics method was developed by using ultra-high performance liquid chromatography (UHPLC) coupled via an ESI source to a quadrupole-time of flight mass spectrometric instrumentation. Mobile phases with ammonium bicarbonate gave the best signal enhancement. The MS capillary voltage, cone voltage, and detector voltage had most effect on the response of the DNA adducts. A low adsorption vial was selected for reducing analyte loss. Hybrid surface-coated analytical columns were tested for reducing adsorption of the DNA adducts. The optimized method was applied to analyse DNA adducts in calf thymus, cat colon, and human colon DNA by performing a MS<sup>E</sup> acquisition (all-ion fragmentation acquisition) and screening for the loss of deoxyribose and the nucleobase fragment ions. Fifty-four DNA adducts were tentatively identified, hereof 38 never reported before. This is the first untargeted DNA adductomics study on human colon tissue, and one of the few untargeted DNA adductomics studies in the literature reporting the identification of such a high number of unknowns. This demonstrates promising results for the application of this sensitive method in future human studies for investigating novel potential cancer-causing factors.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"282 ","pages":"126985"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455148","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-09-19DOI: 10.1016/j.talanta.2024.126920
Zan Gong, Panpan Yuan, Yuqing Gan, Xi Long, Zhiwei Deng, Yalan Tang, Yanjing Yang, Shian Zhong
The capability to detect a small number of miRNAs in clinical samples with simplicity, selectivity, and sensitivity is immensely valuable, yet it remains a daunting task. Here, we described a novel Mango II aptamers-based sensor for the one-pot, sensitive and specific detection of miRNAs. Target miRNA-initiated mediated catalyzed hairpin assembly (CHA) would allow for the production of plenty of DNA duplexes and the formation of the complete T7 promoter, motivating the rolling circle transcription (RCT). Then, the subsequent RCT process efficiently generates a huge number of repeating RNA Mango II aptamers, brightened by the incorporation of fluorescent dye TO1-B for miRNA quantification, realizing label-free and high signal-to-background ratio. Moreover, this assay possesses a remarkable ability to confer high selectivity, enabling the distinction of miRNAs among family members with mere 1- or 2- nucleotide (nt) differences. By employing the proposed assay, we have successfully achieved a sensitive evaluation of miR-21 content in diverse cell lines and clinical serum samples. This offers a versatile approach for the sensitive assay of miRNA biomarkers in molecular diagnosis.
{"title":"A one-pot isothermal Fluorogenic Mango II arrays-based assay for label-free detection of miRNA.","authors":"Zan Gong, Panpan Yuan, Yuqing Gan, Xi Long, Zhiwei Deng, Yalan Tang, Yanjing Yang, Shian Zhong","doi":"10.1016/j.talanta.2024.126920","DOIUrl":"10.1016/j.talanta.2024.126920","url":null,"abstract":"<p><p>The capability to detect a small number of miRNAs in clinical samples with simplicity, selectivity, and sensitivity is immensely valuable, yet it remains a daunting task. Here, we described a novel Mango II aptamers-based sensor for the one-pot, sensitive and specific detection of miRNAs. Target miRNA-initiated mediated catalyzed hairpin assembly (CHA) would allow for the production of plenty of DNA duplexes and the formation of the complete T7 promoter, motivating the rolling circle transcription (RCT). Then, the subsequent RCT process efficiently generates a huge number of repeating RNA Mango II aptamers, brightened by the incorporation of fluorescent dye TO1-B for miRNA quantification, realizing label-free and high signal-to-background ratio. Moreover, this assay possesses a remarkable ability to confer high selectivity, enabling the distinction of miRNAs among family members with mere 1- or 2- nucleotide (nt) differences. By employing the proposed assay, we have successfully achieved a sensitive evaluation of miR-21 content in diverse cell lines and clinical serum samples. This offers a versatile approach for the sensitive assay of miRNA biomarkers in molecular diagnosis.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126920"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142278327","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-09-20DOI: 10.1016/j.talanta.2024.126909
Qing Liu, Si Chen, Yiming Nie, Qian Li, Fang Chen
4-n-butylresorcinol (4nBR) is a frequently utilized as whitening ingredients in skincare cosmetics. Compared with other whitening ingredients, it can effectively inhibit tyrosinase with lower toxicity and superior inhibition efficacy. Under alkaline conditions, an induced oxidative coupling reaction can occur between 4nBR and dopamine (DA) to generate strong fluorescent substance azamonardine with an intense emission band centering at 476 nm when excited at 440 nm. This phenomenon can be used to establish a fluorescence analysis method for 4nBR. The results indicated that the linear range of the method was 1.0-24.0 nmol L-1, and the detection limit was as low as 0.25 nmol L-1. The method showed high sensitivity, good selectivity, mild experimental conditions and low cost. The proposed method was successfully used to detect 4nBR in cosmetics, and the results were consistent with those of HPLC. The spiking recoveries were between 98.2% and 108 %.
{"title":"Determination of 4-n-butylresorcinol by fluorescence derivatization based on dopamine.","authors":"Qing Liu, Si Chen, Yiming Nie, Qian Li, Fang Chen","doi":"10.1016/j.talanta.2024.126909","DOIUrl":"10.1016/j.talanta.2024.126909","url":null,"abstract":"<p><p>4-n-butylresorcinol (4nBR) is a frequently utilized as whitening ingredients in skincare cosmetics. Compared with other whitening ingredients, it can effectively inhibit tyrosinase with lower toxicity and superior inhibition efficacy. Under alkaline conditions, an induced oxidative coupling reaction can occur between 4nBR and dopamine (DA) to generate strong fluorescent substance azamonardine with an intense emission band centering at 476 nm when excited at 440 nm. This phenomenon can be used to establish a fluorescence analysis method for 4nBR. The results indicated that the linear range of the method was 1.0-24.0 nmol L<sup>-1</sup>, and the detection limit was as low as 0.25 nmol L<sup>-1</sup>. The method showed high sensitivity, good selectivity, mild experimental conditions and low cost. The proposed method was successfully used to detect 4nBR in cosmetics, and the results were consistent with those of HPLC. The spiking recoveries were between 98.2% and 108 %.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126909"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338752","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01DOI: 10.1016/j.talanta.2024.127514
Susanne E Woodward, Stefan A Pieczonka, Jasmine Hertzog, Richard Haydock, Mary J Thomas, Chloé Roullier-Gall, Ciaran O'Flynn, Jenny Uhl, Michael Rychlik, Philippe Schmitt-Kopplin, James W Marshall
Non-targeted chemical analysis is a powerful tool for exploration of the unknown chemistry of complex matrices such as food, biological, geochemical, environmental and even extra-terrestrial samples. It allows researchers to ask open, unbiased questions about their system chemistry. Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FT-ICR-MS) offers these options and has been widely used to study complex mixtures, with its unmatched mass resolution enabling direct infusion methods and eliminating the challenges of chromatographic alignment in large-scale longitudinal projects. In this article, we demonstrate the use of FT-ICR-MS for generating a dataset for hundreds of complex samples with diverse chemistries over a period of 6 years and 32 batches, allowing confident comparison of data between samples from different batches. The resulting chemical database will be continuously expanded in future and retrospectively interrogated to test new hypotheses utilizing data of past projects and new knowledge of coming projects. We discuss the experimental setup and how other researchers could apply the same approaches, which is relevant for wide ranging applications and research fields.
{"title":"Continuum of non-targeted data for long term study of complex samples generated by direct infusion ultra-high resolution mass spectrometry.","authors":"Susanne E Woodward, Stefan A Pieczonka, Jasmine Hertzog, Richard Haydock, Mary J Thomas, Chloé Roullier-Gall, Ciaran O'Flynn, Jenny Uhl, Michael Rychlik, Philippe Schmitt-Kopplin, James W Marshall","doi":"10.1016/j.talanta.2024.127514","DOIUrl":"https://doi.org/10.1016/j.talanta.2024.127514","url":null,"abstract":"<p><p>Non-targeted chemical analysis is a powerful tool for exploration of the unknown chemistry of complex matrices such as food, biological, geochemical, environmental and even extra-terrestrial samples. It allows researchers to ask open, unbiased questions about their system chemistry. Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FT-ICR-MS) offers these options and has been widely used to study complex mixtures, with its unmatched mass resolution enabling direct infusion methods and eliminating the challenges of chromatographic alignment in large-scale longitudinal projects. In this article, we demonstrate the use of FT-ICR-MS for generating a dataset for hundreds of complex samples with diverse chemistries over a period of 6 years and 32 batches, allowing confident comparison of data between samples from different batches. The resulting chemical database will be continuously expanded in future and retrospectively interrogated to test new hypotheses utilizing data of past projects and new knowledge of coming projects. We discuss the experimental setup and how other researchers could apply the same approaches, which is relevant for wide ranging applications and research fields.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127514"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142963355","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ferrous ion (Fe2+) can indicate the redox situation of water and also plays an important role in maintaining the ecological balance of water bodies. However, due to the redox-active property of Fe2+, it is still a huge challenge to sensitively and accurately determine Fe2+ especially in interstitial water. Herein, we prepared a ferrozine gel rod for valence fixation during sampling and subsequent smartphone-based detection of Fe2+. The electrode potential of the redox pair can be varied through the formation of Fe2+-ligand complexes, and when Ecomplex was higher than [Formula: see text] , the oxidation of Fe2+ by O2 was hindered, thus achieving the valence fixation of Fe2+. Six ligands were screened, and it was found that ferrozine could effectively increase the redox potential after complexing with Fe2+, and also exhibits an obvious color change while fixing the valence of Fe2+. To facilitate Fe2+ detection, a cross-linked porous polymer gel rod prepared by acrylamide and sodium alginate was used to encapsulate the ferrozine molecules. The ferrozine gel rod enabled fixation the valence of Fe2+ longer than 30 days, and the resulted purple-red color was pictured and analyzed by a smartphone. Ultimately, the developed ferrozine gel rod sensing system was able to achieve sensitive and linear detection of Fe2+ in the range of 1-200 μM with the limit of detection as low as 0.33 μM, and it also exhibited excellent selectivity and anti-interference ability. The accuracy and reliability of the method was verified by the determination of Fe2+ in spiked water samples and certified standard reference water samples. Finally, the ferrozine gel rod sensing system was successfully applied to in-situ detection of Fe2+ in interstitial water, overlying water and upper water of lake and river. This facile system that enabled valence fixation and fast detection is promising for detection of Fe2+ in environmental waters.
{"title":"Valence fixable ferrozine gel rod combined with smartphone for facile determination of redox-active Fe<sup>2+</sup> in environmental water.","authors":"Peng'an Zhu, Jiangle Zhang, Jingjing Jin, Xing Huang, Xinfeng Zhang","doi":"10.1016/j.talanta.2024.126933","DOIUrl":"10.1016/j.talanta.2024.126933","url":null,"abstract":"<p><p>Ferrous ion (Fe<sup>2+</sup>) can indicate the redox situation of water and also plays an important role in maintaining the ecological balance of water bodies. However, due to the redox-active property of Fe<sup>2+</sup>, it is still a huge challenge to sensitively and accurately determine Fe<sup>2+</sup> especially in interstitial water. Herein, we prepared a ferrozine gel rod for valence fixation during sampling and subsequent smartphone-based detection of Fe<sup>2+</sup>. The electrode potential of the redox pair can be varied through the formation of Fe<sup>2+</sup>-ligand complexes, and when E<sub>complex</sub> was higher than [Formula: see text] , the oxidation of Fe<sup>2+</sup> by O<sub>2</sub> was hindered, thus achieving the valence fixation of Fe<sup>2+</sup>. Six ligands were screened, and it was found that ferrozine could effectively increase the redox potential after complexing with Fe<sup>2+</sup>, and also exhibits an obvious color change while fixing the valence of Fe<sup>2+</sup>. To facilitate Fe<sup>2+</sup> detection, a cross-linked porous polymer gel rod prepared by acrylamide and sodium alginate was used to encapsulate the ferrozine molecules. The ferrozine gel rod enabled fixation the valence of Fe<sup>2+</sup> longer than 30 days, and the resulted purple-red color was pictured and analyzed by a smartphone. Ultimately, the developed ferrozine gel rod sensing system was able to achieve sensitive and linear detection of Fe<sup>2+</sup> in the range of 1-200 μM with the limit of detection as low as 0.33 μM, and it also exhibited excellent selectivity and anti-interference ability. The accuracy and reliability of the method was verified by the determination of Fe<sup>2+</sup> in spiked water samples and certified standard reference water samples. Finally, the ferrozine gel rod sensing system was successfully applied to in-situ detection of Fe<sup>2+</sup> in interstitial water, overlying water and upper water of lake and river. This facile system that enabled valence fixation and fast detection is promising for detection of Fe<sup>2+</sup> in environmental waters.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126933"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
An ultrasensitive electrochemical sensor is constructed by electrostatically adsorbing negatively charged hourglass-shape Cu-Polyoxometalate (POM) onto a positively charged CoO nanowires modified carbon cloth. The petaloid CoO nanowires have a large specific surface area that can well disperse open-structured Cu-POM to form Cu-POM@CoONWs@CC, which can maximumly expose catalytic active centers (Co2+ and Cu2+) and accelerate mass/charge transfer. In addition to the above advantages, the excellent electron exchange ability of Cu-POM and good conductivity of CoONWs@CC endow the sensor with good detection capability to H2O2 including a linear detection range of 0.05-1.4 μA μM-1, a low detection limit of 0.022 μM, high sensitivity of 110.48 μA μM-1, good selectivity and long-term stability. Due to the fast transformation of superoxide anion (O2∙-) to H2O2, the sensor can indirectly monitor the electron leakage resulting in the formation of O2∙- via detecting H2O2. Afterwards, Hela cell mitochondria were extracted from the living cells that cultured with different mitochondrial inhibitors and the release of O2∙- from the corresponding mitochondrial complexes was monitored by the sensor. Through comparing the current signals, we determined that complex I is probably the main electron leakage site. This work could provide meaningful information for the diagnosis of certain oxidative stress diseases.
{"title":"Fabrication of polyoxometalate dispersed cobalt oxide nanowires for electrochemically monitoring superoxide radicals from Hela cell mitochondria.","authors":"Chaoyao Geng, Xiujuan Zhang, Xinyao Zhu, Bingjie Li, Zhenhua Ren, Xiuhua Liu, Jadranka Travas-Sejdic, Xiaoqiang Liu","doi":"10.1016/j.talanta.2024.127037","DOIUrl":"10.1016/j.talanta.2024.127037","url":null,"abstract":"<p><p>An ultrasensitive electrochemical sensor is constructed by electrostatically adsorbing negatively charged hourglass-shape Cu-Polyoxometalate (POM) onto a positively charged CoO nanowires modified carbon cloth. The petaloid CoO nanowires have a large specific surface area that can well disperse open-structured Cu-POM to form Cu-POM@CoONWs@CC, which can maximumly expose catalytic active centers (Co<sup>2+</sup> and Cu<sup>2+</sup>) and accelerate mass/charge transfer. In addition to the above advantages, the excellent electron exchange ability of Cu-POM and good conductivity of CoONWs@CC endow the sensor with good detection capability to H<sub>2</sub>O<sub>2</sub> including a linear detection range of 0.05-1.4 μA μM<sup>-1</sup>, a low detection limit of 0.022 μM, high sensitivity of 110.48 μA μM<sup>-1</sup>, good selectivity and long-term stability. Due to the fast transformation of superoxide anion (O<sub>2</sub><sup>∙-</sup>) to H<sub>2</sub>O<sub>2</sub>, the sensor can indirectly monitor the electron leakage resulting in the formation of O<sub>2</sub><sup>∙-</sup> via detecting H<sub>2</sub>O<sub>2</sub>. Afterwards, Hela cell mitochondria were extracted from the living cells that cultured with different mitochondrial inhibitors and the release of O<sub>2</sub><sup>∙-</sup> from the corresponding mitochondrial complexes was monitored by the sensor. Through comparing the current signals, we determined that complex I is probably the main electron leakage site. This work could provide meaningful information for the diagnosis of certain oxidative stress diseases.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"282 ","pages":"127037"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dimethyl methylphosphonate (DMMP) is commonly used as an alternative for demonstrating to detect sarin, which is one of the most toxic but odorless chemical nerve agents. Among various types of DMMP sensors, those utilizing surface acoustic wave (SAW) technology provide notable advantages such as wireless/passive monitoring, digital output, and a compact, portable design. However, key challenges for SAW-based DMMP sensors operated at room temperature lies in simultaneous enhancement of sensitivities and reduction of detection limits. In this study, we developed a binary material strategy by combining reduced graphene oxide (rGO) and tin disulfide (SnS2) with (100)-facets orientation as sensing layers of SAW device for DMMP detection utilized at room temperature. Ultraviolet (UV) light was applied to activate the sensitive film and reduce the sensor's response time. The developed SAW DMMP sensor demonstrated a superior sensitivity (-1298.82 Hz/ppm), a low detection limit of 50 ppb, and a hysteresis below 1.5%, along with fast response/recovery time (39.2 s/28.4 s), excellent selectivity, long-term stability and repeatability. The formation of shrub-like rGO-SnS2 heterojunctions with abundant surface defects and large specific surface areas, high-energy (100) crystalline surfaces of SnS2, and photogenerated carriers generated by UV irradiation were pinpointed as the crucial sensing mechanisms. These factors collectively enhanced adsorption and reaction dynamics of DMMP molecules.
{"title":"Surface acoustic wave platform integrated with ultraviolet activated rGO-SnS<sub>2</sub> nanocomposites to achieve ppb-level dimethyl methylphosphonate detection at room-temperature.","authors":"Jinbo Zhang, Jian Zhou, Hui Chen, Yihao Guo, Qikun Tian, Yanhong Xia, Guangzhao Qin, Jianfei Xie, Yongqing Fu","doi":"10.1016/j.talanta.2024.127063","DOIUrl":"10.1016/j.talanta.2024.127063","url":null,"abstract":"<p><p>Dimethyl methylphosphonate (DMMP) is commonly used as an alternative for demonstrating to detect sarin, which is one of the most toxic but odorless chemical nerve agents. Among various types of DMMP sensors, those utilizing surface acoustic wave (SAW) technology provide notable advantages such as wireless/passive monitoring, digital output, and a compact, portable design. However, key challenges for SAW-based DMMP sensors operated at room temperature lies in simultaneous enhancement of sensitivities and reduction of detection limits. In this study, we developed a binary material strategy by combining reduced graphene oxide (rGO) and tin disulfide (SnS<sub>2</sub>) with (100)-facets orientation as sensing layers of SAW device for DMMP detection utilized at room temperature. Ultraviolet (UV) light was applied to activate the sensitive film and reduce the sensor's response time. The developed SAW DMMP sensor demonstrated a superior sensitivity (-1298.82 Hz/ppm), a low detection limit of 50 ppb, and a hysteresis below 1.5%, along with fast response/recovery time (39.2 s/28.4 s), excellent selectivity, long-term stability and repeatability. The formation of shrub-like rGO-SnS<sub>2</sub> heterojunctions with abundant surface defects and large specific surface areas, high-energy (100) crystalline surfaces of SnS<sub>2</sub>, and photogenerated carriers generated by UV irradiation were pinpointed as the crucial sensing mechanisms. These factors collectively enhanced adsorption and reaction dynamics of DMMP molecules.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"282 ","pages":"127063"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142455173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-09-18DOI: 10.1016/j.talanta.2024.126900
Ziwang Liu, Rihui Su, Xiaohua Xiao, Gongke Li
Rapid and selective separation, enrichment and detection of trace residue all-in-one in complex samples is a major challenge. Hydrogels with molecular sieve properties can selectively separate and enrich target analytes, and the combination with high sensitivity detection of surface-enhanced Raman scattering (SERS) is expected to achieve the above all-in-one detection. Herein, the core-shell structured Au@poly(N-isopropylacrylamide)-phenylboronic acid hydrogel (Au@PNIP-VBA) with boronic acid ester groups was prepared by thermally initiated polymerization. The boronic acid ester groups in hydrogel are selectively hydrolyzed by hydrogen peroxide (H2O2) to hydroxyl structures, leading to a reduction in SERS signals. The Au@PNIP-VBA hydrogel has molecular sieve properties and high SERS activity, making it suitable for separation, enrichment, hydrolysis and detection of H2O2 all-in-one. A rapid SERS method was developed for analysis of H2O2 based on the Au@PNIP-VBA hydrogel with the linear range of 8.5 × 10-2-6.8 mg L-1 and the detection limit of 33 μg L-1. The method was successfully applied to the determination of H2O2 residue in fresh milk, pure milk, yogurt and camel milk, with the recoveries were in the range of 82.2%-109.3% and the relative standard deviations were 2.8%-8.3%. This efficient all-in-one strategy has the advantages of simple sample pre-treatment, rapid analysis (30 min) and high sensitivity, making it highly promising for food quality and safety analysis.
{"title":"Boronic acid ester-based hydrogel as surface-enhanced Raman scattering substrates for separation, enrichment, hydrolysis and detection of hydrogen peroxide residue in dairy product all-in-one.","authors":"Ziwang Liu, Rihui Su, Xiaohua Xiao, Gongke Li","doi":"10.1016/j.talanta.2024.126900","DOIUrl":"10.1016/j.talanta.2024.126900","url":null,"abstract":"<p><p>Rapid and selective separation, enrichment and detection of trace residue all-in-one in complex samples is a major challenge. Hydrogels with molecular sieve properties can selectively separate and enrich target analytes, and the combination with high sensitivity detection of surface-enhanced Raman scattering (SERS) is expected to achieve the above all-in-one detection. Herein, the core-shell structured Au@poly(N-isopropylacrylamide)-phenylboronic acid hydrogel (Au@PNIP-VBA) with boronic acid ester groups was prepared by thermally initiated polymerization. The boronic acid ester groups in hydrogel are selectively hydrolyzed by hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) to hydroxyl structures, leading to a reduction in SERS signals. The Au@PNIP-VBA hydrogel has molecular sieve properties and high SERS activity, making it suitable for separation, enrichment, hydrolysis and detection of H<sub>2</sub>O<sub>2</sub> all-in-one. A rapid SERS method was developed for analysis of H<sub>2</sub>O<sub>2</sub> based on the Au@PNIP-VBA hydrogel with the linear range of 8.5 × 10<sup>-2</sup>-6.8 mg L<sup>-1</sup> and the detection limit of 33 μg L<sup>-1</sup>. The method was successfully applied to the determination of H<sub>2</sub>O<sub>2</sub> residue in fresh milk, pure milk, yogurt and camel milk, with the recoveries were in the range of 82.2%-109.3% and the relative standard deviations were 2.8%-8.3%. This efficient all-in-one strategy has the advantages of simple sample pre-treatment, rapid analysis (30 min) and high sensitivity, making it highly promising for food quality and safety analysis.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126900"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142278350","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-01-01Epub Date: 2024-09-18DOI: 10.1016/j.talanta.2024.126902
Todd Cowen, Sotirios Grammatikos, Michael Cheffena
A simple gas sensor consisting of a molecularly imprinted polymer-carbon nanotube composite cast onto a screen-printed electrode has been developed with extremely high selectivity for ethanol vapour over methanol vapour. Ethanol gas sensors typically display selectivity for ethanol over methanol in the range 2-4 times, while the mean ratio of ethanol to methanol response observed with the described device was 672. This selectivity was achieved under ambient conditions. Additionally, the molecularly imprinted polymer was produced using reagents previously applied in the development of a device selective for methanol, with only the template being changed. This demonstrates the versatility of molecular imprinting and provides a foundation for their greater integration into future gas sensors.
{"title":"Highly selective ethanol vapour sensing materials for a new generation of gas sensors based on molecularly imprinted polymers.","authors":"Todd Cowen, Sotirios Grammatikos, Michael Cheffena","doi":"10.1016/j.talanta.2024.126902","DOIUrl":"10.1016/j.talanta.2024.126902","url":null,"abstract":"<p><p>A simple gas sensor consisting of a molecularly imprinted polymer-carbon nanotube composite cast onto a screen-printed electrode has been developed with extremely high selectivity for ethanol vapour over methanol vapour. Ethanol gas sensors typically display selectivity for ethanol over methanol in the range 2-4 times, while the mean ratio of ethanol to methanol response observed with the described device was 672. This selectivity was achieved under ambient conditions. Additionally, the molecularly imprinted polymer was produced using reagents previously applied in the development of a device selective for methanol, with only the template being changed. This demonstrates the versatility of molecular imprinting and provides a foundation for their greater integration into future gas sensors.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126902"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142278356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
On-site quantitative detection of organophosphorus pesticides (OPs) is crucial for safeguarding food and public safety. This study presents a novel acetylcholinesterase (AChE)-mediated paper-based Au3+-etching of gold nanobipyramids (AuNBPs) system. The system employs a long-term storable AuNBPs-deposited nylon membrane embedded within a portable and temperature-controlled paper-based analytical device. This system, coupled with a colorimeter-based quantitative method, enables the development of a practical paper-based multicolor sensor (PMS) for on-site quantitative detection of three common OPs (paraoxon, dichlorvos, and trichlorfon). In the absence of OPs, AChE hydrolyzes acetylthiocholine to thiocholine, which reduces Au3+ to Au+. The presence of OPs inhibits AChE activity, thereby preserving Au3+ to etch AuNBPs on nylon membranes, accompanied by multicolor changes. These color changes can be simply quantified by measuring the a∗ parameter of the CIELab color space using a portable colorimeter. Under optimal conditions, the PMS displayed eight OPs-corresponding color changes with a minimum detectable concentration of 1.0-10 μg/L (visual observation) and limits of detection of 0.8-7.2 μg/L (colorimeter) and 0.2-3.4 μg/L (UV-vis spectrometry). The PMS successfully determined the OPs in vegetable and rice samples with recoveries of 89.0-109 % and RSDs (n = 5) of <6 %. These results were consistent with those obtained using the HPLC-MS method. The PMS demonstrates excellent portability, AuNBPs stability, detection sensitivity, and reproducibility, making it a promising tool for the on-site quantitative detection of OPs residues in food. Furthermore, the paper-based etching system coupled with the colorimeter-based quantitative method provides a valuable reference to develop practical PMSs for various targets in diverse fields.
{"title":"Paper-based multicolor sensor for on-site quantitative detection of organophosphate pesticides based on acetylcholinesterase-mediated paper-based Au<sup>3+</sup>-etching of gold nanobipyramids and CIELab color space.","authors":"Feng Zhang, Yu Gao, Enxi Ren, Ling Fang, Weijuan Yang, Liaoyuan Zhang, Zongwen Wang","doi":"10.1016/j.talanta.2024.126925","DOIUrl":"10.1016/j.talanta.2024.126925","url":null,"abstract":"<p><p>On-site quantitative detection of organophosphorus pesticides (OPs) is crucial for safeguarding food and public safety. This study presents a novel acetylcholinesterase (AChE)-mediated paper-based Au<sup>3+</sup>-etching of gold nanobipyramids (AuNBPs) system. The system employs a long-term storable AuNBPs-deposited nylon membrane embedded within a portable and temperature-controlled paper-based analytical device. This system, coupled with a colorimeter-based quantitative method, enables the development of a practical paper-based multicolor sensor (PMS) for on-site quantitative detection of three common OPs (paraoxon, dichlorvos, and trichlorfon). In the absence of OPs, AChE hydrolyzes acetylthiocholine to thiocholine, which reduces Au<sup>3+</sup> to Au<sup>+</sup>. The presence of OPs inhibits AChE activity, thereby preserving Au<sup>3+</sup> to etch AuNBPs on nylon membranes, accompanied by multicolor changes. These color changes can be simply quantified by measuring the a∗ parameter of the CIELab color space using a portable colorimeter. Under optimal conditions, the PMS displayed eight OPs-corresponding color changes with a minimum detectable concentration of 1.0-10 μg/L (visual observation) and limits of detection of 0.8-7.2 μg/L (colorimeter) and 0.2-3.4 μg/L (UV-vis spectrometry). The PMS successfully determined the OPs in vegetable and rice samples with recoveries of 89.0-109 % and RSDs (n = 5) of <6 %. These results were consistent with those obtained using the HPLC-MS method. The PMS demonstrates excellent portability, AuNBPs stability, detection sensitivity, and reproducibility, making it a promising tool for the on-site quantitative detection of OPs residues in food. Furthermore, the paper-based etching system coupled with the colorimeter-based quantitative method provides a valuable reference to develop practical PMSs for various targets in diverse fields.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126925"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142278357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}