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Development of an untargeted DNA adductomics method by ultra-high performance liquid chromatography coupled to high-resolution mass spectrometry. 利用超高效液相色谱法和高分辨质谱法开发非靶向 DNA 加合物组学方法。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-05 DOI: 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。
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引用次数: 0
A one-pot isothermal Fluorogenic Mango II arrays-based assay for label-free detection of miRNA. 基于等温荧光芒果 II 阵列的单次无标记检测 miRNA 方法。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-19 DOI: 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.

以简单、选择性和灵敏度检测临床样本中少量 miRNA 的能力具有极大的价值,但这仍然是一项艰巨的任务。在这里,我们介绍了一种基于芒果 II 合体的新型传感器,它能对 miRNA 进行一次性、灵敏而特异的检测。由目标 miRNA 引发的催化发夹组装(CHA)可产生大量 DNA 双链并形成完整的 T7 启动子,从而推动滚圆转录(RCT)。随后的 RCT 过程有效地生成了大量重复的 RNA 芒果 II 合体,并通过加入荧光染料 TO1-B 进行 miRNA 定量,实现了无标记和高信噪比。此外,这种检测方法还具有显著的高选择性,能够区分仅有 1 或 2 个核苷酸(nt)差异的 miRNA 家族成员。通过采用所提出的检测方法,我们成功地实现了对不同细胞系和临床血清样本中 miR-21 含量的灵敏评估。这为分子诊断中敏感地检测 miRNA 生物标记物提供了一种多功能方法。
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引用次数: 0
Determination of 4-n-butylresorcinol by fluorescence derivatization based on dopamine. 基于多巴胺的荧光衍生法测定 4-正丁基间苯二酚。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-20 DOI: 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 %.

4-正丁基间苯二酚(4nBR)是护肤化妆品中常用的美白成分。与其他美白成分相比,它能有效抑制酪氨酸酶,毒性较低,抑制效果显著。在碱性条件下,4nBR 与多巴胺(DA)之间会发生诱导氧化偶联反应,生成强荧光物质氮杂萘啶,在 440 纳米波长下激发时,以 476 纳米波长为中心形成一条强发射带。这一现象可用于建立 4nBR 的荧光分析方法。结果表明,该方法的线性范围为1.0-24.0 nmol L-1,检出限低至0.25 nmol L-1。该方法灵敏度高、选择性好、实验条件温和、成本低。该方法成功用于化妆品中4nBR的检测,结果与高效液相色谱法一致。加标回收率为98.2%~108%。
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引用次数: 0
Continuum of non-targeted data for long term study of complex samples generated by direct infusion ultra-high resolution mass spectrometry.
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 DOI: 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.

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引用次数: 0
Valence fixable ferrozine gel rod combined with smartphone for facile determination of redox-active Fe2+ in environmental water. Valence fixable ferrozine gel rod 与智能手机相结合,轻松测定环境水体中具有氧化还原活性的 Fe2+。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-22 DOI: 10.1016/j.talanta.2024.126933
Peng'an Zhu, Jiangle Zhang, Jingjing Jin, Xing Huang, Xinfeng Zhang

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.

亚铁离子(Fe2+)可指示水体的氧化还原情况,在维持水体生态平衡方面也发挥着重要作用。然而,由于Fe2+具有氧化还原活性,如何灵敏准确地测定Fe2+,尤其是间隙水中的Fe2+,仍然是一个巨大的挑战。在此,我们制备了一种铁嗪凝胶棒,用于在采样过程中进行价态固定,然后基于智能手机检测 Fe2+。通过形成 Fe2+-配体复合物,可改变氧化还原对的电极电位,当 Ecomplex 大于[式中:见正文]时,Fe2+ 被 O2 氧化受阻,从而实现了 Fe2+ 的价固定。筛选了六种配体,发现铁嗪与 Fe2+络合后能有效地提高氧化还原电位,在固定 Fe2+的价态时还能表现出明显的颜色变化。为了便于检测 Fe2+,研究人员使用丙烯酰胺和海藻酸钠制备的交联多孔聚合物凝胶杆来包裹铁嗪分子。这种铁嗪凝胶棒可固定 Fe2+ 的价态超过 30 天,所产生的紫红色可通过智能手机进行拍照和分析。最终,所开发的铁嗪凝胶棒传感系统能够在 1-200 μM 的范围内灵敏、线性地检测 Fe2+,检测限低至 0.33 μM,并且具有良好的选择性和抗干扰能力。该方法的准确性和可靠性得到了加标水样和标准参考水样中 Fe2+ 含量测定的验证。最后,铁嗪凝胶棒传感系统被成功应用于湖泊和河流的间隙水、上覆水和上层水中 Fe2+ 的原位检测。这种简便的系统可实现价态固定和快速检测,有望用于环境水体中 Fe2+ 的检测。
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引用次数: 0
Fabrication of polyoxometalate dispersed cobalt oxide nanowires for electrochemically monitoring superoxide radicals from Hela cell mitochondria. 制备聚氧化铝分散氧化钴纳米线,用于电化学监测 Hela 细胞线粒体中的超氧自由基。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-18 DOI: 10.1016/j.talanta.2024.127037
Chaoyao Geng, Xiujuan Zhang, Xinyao Zhu, Bingjie Li, Zhenhua Ren, Xiuhua Liu, Jadranka Travas-Sejdic, Xiaoqiang Liu

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.

通过静电吸附带负电荷的沙漏形聚氧乙烯醚铜(POM)到带正电荷的 CoO 纳米线修饰碳布上,构建了一种超灵敏电化学传感器。花瓣状 CoO 纳米线具有很大的比表面积,可以很好地分散开放结构的 Cu-POM,形成 Cu-POM@CoONWs@CC ,从而最大限度地暴露催化活性中心(Co2+ 和 Cu2+),加速质量/电荷转移。除上述优点外,Cu-POM 优异的电子交换能力和 CoONWs@CC 良好的导电性赋予了该传感器良好的 H2O2 检测能力,包括 0.05-1.4 μA μM-1 的线性检测范围、0.022 μM 的低检测限、110.48 μA μM-1 的高灵敏度、良好的选择性和长期稳定性。由于超氧阴离子(O2∙-)可快速转化为 H2O2,该传感器可通过检测 H2O2 间接监测形成 O2∙- 的电子泄漏。随后,从使用不同线粒体抑制剂培养的活细胞中提取 Hela 细胞线粒体,用传感器监测相应线粒体复合物释放 O2∙- 的情况。通过比较电流信号,我们确定复合体 I 可能是主要的电子泄漏点。这项工作可为某些氧化应激疾病的诊断提供有意义的信息。
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引用次数: 0
Surface acoustic wave platform integrated with ultraviolet activated rGO-SnS2 nanocomposites to achieve ppb-level dimethyl methylphosphonate detection at room-temperature. 表面声波平台与紫外线激活的 rGO-SnS2 纳米复合材料集成,实现室温下 ppb 级甲基膦酸二甲酯检测。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-17 DOI: 10.1016/j.talanta.2024.127063
Jinbo Zhang, Jian Zhou, Hui Chen, Yihao Guo, Qikun Tian, Yanhong Xia, Guangzhao Qin, Jianfei Xie, Yongqing Fu

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.

甲基膦酸二甲酯(DMMP)通常用作检测沙林的替代品,沙林是毒性最强但无味的化学神经毒剂之一。在各种类型的 DMMP 传感器中,利用表面声波(SAW)技术的传感器具有显著的优势,如无线/被动监测、数字输出以及紧凑便携的设计。然而,基于声表面波的 DMMP 传感器在室温下工作时面临的主要挑战是如何同时提高灵敏度和降低检测限。在这项研究中,我们开发了一种二元材料策略,将还原氧化石墨烯(rGO)和具有(100)-面方向的二硫化锡(SnS2)结合起来,作为声表面波器件的传感层,用于室温下的 DMMP 检测。紫外线(UV)光可激活敏感薄膜并缩短传感器的响应时间。所开发的声表面波 DMMP 传感器具有极高的灵敏度(-1298.82 Hz/ppm)、50 ppb 的低检测限和低于 1.5% 的滞后,以及快速响应/恢复时间(39.2 s/28.4 s)、优异的选择性、长期稳定性和可重复性。具有丰富表面缺陷和大比表面积的灌木状 rGO-SnS2 异质结的形成、SnS2 的高能(100)结晶表面以及紫外线照射产生的光生载流子被认为是关键的传感机制。这些因素共同增强了 DMMP 分子的吸附和反应动力学。
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引用次数: 0
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. 将硼酸酯基水凝胶作为表面增强拉曼散射基底,用于乳制品中过氧化氢残留的分离、富集、水解和检测一体化。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-18 DOI: 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.

快速、选择性地分离、富集和检测复杂样品中的痕量残留物是一项重大挑战。具有分子筛特性的水凝胶可以选择性地分离和富集目标分析物,结合表面增强拉曼散射(SERS)的高灵敏度检测,有望实现上述一体化检测。本文采用热引发聚合法制备了具有硼酸酯基团的核壳结构 Au@聚(N-异丙基丙烯酰胺)-苯硼酸水凝胶(Au@PNIP-VBA)。水凝胶中的硼酸酯基团会被过氧化氢(H2O2)选择性地水解为羟基结构,从而导致 SERS 信号减弱。Au@PNIP-VBA 水凝胶具有分子筛特性和高 SERS 活性,适用于 H2O2 的分离、富集、水解和检测于一体。建立了基于Au@PNIP-VBA水凝胶的H2O2快速SERS分析方法,其线性范围为8.5×10-2-6.8 mg L-1,检出限为33 μg L-1。该方法成功地应用于鲜牛奶、纯牛奶、酸奶和骆驼奶中H2O2残留量的测定,回收率为82.2%~109.3%,相对标准偏差为2.8%~8.3%。这种高效的一体化策略具有样品前处理简单、分析速度快(30 分钟)和灵敏度高等优点,在食品质量和安全分析中具有广阔的应用前景。
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引用次数: 0
Highly selective ethanol vapour sensing materials for a new generation of gas sensors based on molecularly imprinted polymers. 基于分子印迹聚合物的新一代气体传感器的高选择性乙醇蒸汽传感材料。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-18 DOI: 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.

我们开发出了一种简单的气体传感器,由分子印迹聚合物-碳纳米管复合材料浇铸在丝网印刷电极上组成,对乙醇蒸气的选择性极高。乙醇气体传感器对乙醇和甲醇的选择性通常在 2-4 倍之间,而使用所述装置观察到的乙醇和甲醇反应的平均比率为 672。这种选择性是在环境条件下实现的。此外,分子印迹聚合物是利用以前用于开发甲醇选择性装置的试剂生产的,只改变了模板。这证明了分子印迹技术的多功能性,并为其进一步融入未来的气体传感器奠定了基础。
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引用次数: 0
Paper-based multicolor sensor for on-site quantitative detection of organophosphate pesticides based on acetylcholinesterase-mediated paper-based Au3+-etching of gold nanobipyramids and CIELab color space. 基于乙酰胆碱酯酶介导的纸基 Au3+-蚀刻金纳米双锥体和 CIELab 色彩空间的有机磷农药现场定量检测纸基多色传感器。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-19 DOI: 10.1016/j.talanta.2024.126925
Feng Zhang, Yu Gao, Enxi Ren, Ling Fang, Weijuan Yang, Liaoyuan Zhang, Zongwen Wang

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.

现场定量检测有机磷农药(OPs)对保障食品和公共安全至关重要。本研究提出了一种新型乙酰胆碱酯酶(AChE)介导的纸基 Au3+ 蚀刻金纳米双金字塔(AuNBPs)系统。该系统采用了一种可长期保存的 AuNBPs 沉积尼龙膜,嵌入到一个便携式温控纸基分析装置中。该系统与基于色度计的定量方法相结合,开发出一种实用的纸质多色传感器(PMS),用于现场定量检测三种常见的 OPs(对硫磷、敌敌畏和敌百虫)。在没有 OPs 的情况下,AChE 会将乙酰硫代胆碱水解为硫代胆碱,从而将 Au3+ 还原为 Au+。OPs 的存在抑制了 AChE 的活性,从而保留了 Au3+,使其能够蚀刻尼龙膜上的 AuNBPs,并伴随着多种颜色的变化。这些颜色变化可通过使用便携式色度计测量 CIELab 色彩空间的 a∗ 参数进行简单量化。在最佳条件下,PMS 显示了八种 OPs 对应的颜色变化,最低检测浓度为 1.0-10 μg/L(目测),检测限为 0.8-7.2 μg/L(色度计)和 0.2-3.4 μg/L(紫外-可见光谱法)。PMS 成功地测定了蔬菜和大米样品中的 OPs,回收率为 89.0-109%,RSD(n = 5)为
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