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Development of 3D printed microchips with encapsulated channels as miniaturized separation devices for bioanalysis 具有封装通道的3D打印微芯片作为小型生物分析分离装置的开发
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-12-01 DOI: 10.1016/j.aca.2025.344971
Christopher T. Desire , R. Dario Arrua , Billy Michalatos , Jing Zhang , Xanthe L. Venn , Michael Breadmore , Zlatko Kopecki , Neil McMillan , Robert Fitridge , Emily F. Hilder , Allison J. Cowin

Background

3D printing has emerged as an attractive alternative for the fabrication of microfluidic devices offering the ability for rapid prototyping and a high degree of customization, in contrast to conventional microfabrication techniques. Despite its potential, the size of internal features (such as microfluidic channels) has been limited to larger cross-sectional areas and shorter lengths. Advances in 3D printing technology and the development of custom resins have allowed for smaller features to be obtained, moving the field closer to genuine microfluidic devices. However, not all researchers can readily perform the customization or resin development required.

Results

In this work, we obtained channels with smaller cross-sections (∼100–200 μm) and longer channel lengths (up to 96 mm) using a commercial printer and resin, by optimizing several printing parameters as well as aspects of the microfluidic design. A chip array and custom 3D printed manifold was used to develop a workflow for high throughput post-processing, enabling facile removal of uncured resin from enclosed channels. Using a rectangular channel geometry, a layer height of 50 μm, and a single layer cover, channels with specified dimensions of 150 × 150 μm and 6 mm total length were obtained with a high success rate (>98 %). Channels up to 96 mm could be printed using dimensions of 200 × 200 μm. The potential for these microchips for the pre-concentration and separation of proteins was also demonstrated, by fabricating polyacrylamide separation gels within the channels.

Significance

This work presents an alternative workflow for fabrication of enclosed channels that does not rely on the use of custom printers or resins. Implementation of this workflow with pre-existing 3D printing technology is expected to allow future research progress facilitating smaller channel dimensions of longer lengths more readily. If coupled with emerging 3D printing technology, this could open the door for the development of truly microfluidic devices for bioanalysis and point-of-care devices in healthcare settings.
与传统的微制造技术相比,3d打印已经成为制造微流体装置的一种有吸引力的替代方案,提供了快速原型设计和高度定制的能力。尽管具有潜力,但内部特征(如微流控通道)的尺寸仅限于较大的横截面积和较短的长度。3D打印技术的进步和定制树脂的开发已经允许获得更小的特征,使该领域更接近真正的微流体装置。然而,并不是所有的研究人员都能轻松地进行所需的定制或树脂开发。在这项工作中,我们使用商用打印机和树脂,通过优化几个打印参数以及微流体设计的各个方面,获得了更小的横截面(~ 100-200 μm)和更长的通道长度(高达96 mm)。芯片阵列和定制的3D打印歧管用于开发高通量后处理的工作流程,可以方便地从封闭通道中去除未固化的树脂。采用矩形通道几何形状,层高50 μm,单层覆盖,可获得指定尺寸为150 × 150 μm,总长度为6 mm的通道,成功率高达98%。使用200 × 200 μm的尺寸可以打印最大为96 mm的通道。通过在通道内制造聚丙烯酰胺分离凝胶,这些微芯片在蛋白质预浓缩和分离方面的潜力也得到了证明。意义:这项工作提出了一种不依赖于使用定制打印机或树脂的封闭通道制造的替代工作流程。利用现有的3D打印技术实现这一工作流程,有望使未来的研究进展更容易地促进更小尺寸、更长的通道尺寸。如果与新兴的3D打印技术相结合,这可能为开发真正的微流体设备打开大门,用于医疗保健环境中的生物分析和护理点设备。
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引用次数: 0
Biopolymer-based ultrasound extraction of parabens: Functionalized polyvinylpyrrolidone –alginate beads with a natural eutectic solvent 基于生物聚合物的超声波提取对羟基苯甲酸酯:用天然共熔溶剂功能化聚乙烯吡咯烷酮-海藻酸酯珠
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-12-01 DOI: 10.1016/j.aca.2025.344978
J. Mabel Luna-Díaz , Luz O. Leal-Quezada , Laura Ferrer , Edwin Palacio
Parabens, widely used as preservatives in pharmaceuticals and personal care products, are considered emerging contaminants due to their endocrine-disrupting properties and frequent detection in aquatic environments. Their trace-level concentrations (μg L−1 to ng L−1) and moderate polarity pose significant challenges for effective monitoring using conventional preconcentration techniques. To address these limitations, a green ultrasound-assisted extraction method was developed employing polyvinylpyrrolidone–alginate beads functionalized with a hydrophobic natural eutectic solvent composed of menthol and camphor (2:1 M ratio). The sorbent facilitates selective interaction with parabens through hydrogen bonding and hydrophobic effects, significantly improving extraction efficiency over non-functionalized materials. The method utilises only 125 mg of biodegradable sorbent and 3 % ammonia in water as desorption solvent, per analysis, minimising the use of hazardous reagent and aligning with Green Analytical Chemistry principles. Under optimised conditions, four parabens i.e., methylparaben, ethylparaben, propylparaben and butylparaben, were simultaneously extracted and analysed by UHPLC-DAD, achieving enrichment factors ranged from 8 to 13.9, with limits of detection and quantification between 0.056 and 0.222 μg L−1 and 0.186–0.744 μg L−1, respectively. Precision (RSD) remained below 10 % for both intra- and inter-day analyses, with excellent linearity (R2 ≥ 0.9943) across a working range of 5–10,000 μg L−1. The method was successfully applied to wastewater samples from various treatment stages, achieving recoveries between 81 and 114 %, confirming its suitability for routine environmental monitoring of parabens.
对羟基苯甲酸酯被广泛用作药品和个人护理产品的防腐剂,由于其内分泌干扰特性和在水生环境中经常被检测到,被认为是新兴污染物。它们的痕量浓度(μg - L-1至ng - L-1)和中等极性对传统预富集技术的有效监测提出了重大挑战。为了解决这些局限性,我们开发了一种绿色超声辅助提取方法,使用由薄荷醇和脑组成的疏水天然共晶溶剂(摩尔比为2:1)对聚乙烯吡咯烷酮海藻酸酯珠进行功能化。该吸附剂通过氢键和疏水效应促进与对羟基苯甲酸酯的选择性相互作用,显著提高了非功能化材料的萃取效率。该方法每次分析仅使用125毫克可生物降解的吸附剂和3%的氨水作为解吸溶剂,最大限度地减少了有害试剂的使用,并符合绿色分析化学原则。在优化条件下,同时提取对羟基苯甲酸甲酯、对羟基苯甲酸乙酯、对羟基苯甲酸丙酯和对羟基苯甲酸丁酯4种对羟基苯甲酸酯,富集因子范围为8 ~ 13.9,检测限和定量限分别为0.056 ~ 0.222 μg -1和0.186 ~ 0.744 μg -1。日内和日间分析的精密度(RSD)均低于10%,在5-10,000 μg L-1的工作范围内具有良好的线性(R2≥0.9943)。该方法成功地应用于不同处理阶段的废水样品,回收率在81 ~ 114%之间,证实了对羟基苯甲酸酯的常规环境监测的适用性。
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引用次数: 0
Bisulfite-triggered AIEgens release from metal–organic cages for bioimaging 亚硫酸氢盐触发的生物成像金属有机笼中氧气释放
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-12-01 DOI: 10.1016/j.aca.2025.344966
Zhihui Zhong , Qinglei Cui , Tangsheng Guan , Hongyu Wen , Yu-xin Chen , Yu-Xin Ye , Jianqiao Xu , Gangfeng Ouyang

Background

Aggregation-induced emission luminogens (AIEgens) exhibit efficient fluorescence in the aggregated state, making them promising candidates for bioimaging applications. However, their inherently hydrophobic structures often lead to uncontrollable aggregation, hindering their delivery to target sites for imaging. Researchers have developed strategies to enhance the water solubility of AIEgens through either structural modification or carrier-based encapsulation. However structural modification methods involve complicated synthesis and macrocycles often show low encapsulation efficiency toward AIEgens. Improving the water solubility of AIEgens for bioimaging requires simple yet effective strategies.

Results

We report a novel supramolecular encapsulation approach utilizing water-soluble metal–organic cages (MOCs) as host carriers for AIEgens. Encapsulation significantly prevented the aggregation of AIEgens, enabling their uniform dispersion in aqueous matrices. The AIEgens@MOC complex exhibited excellent structural stability across broad ranges of pH (5.0–9.0), temperature (10°C–80 °C), and time (over 14 days) prior to bisulfite (HSO3) stimulation, confirming the stable host–guest interaction. Upon stimulation with HSO3, the disassembly of MOC led to the release of AIEgens, which subsequently aggregated and exhibited significantly enhanced fluorescence within 60 s. The new AIEgens@MOC complex enabled the succeeded visualization of abnormal intracellular HSO3 fluctuations (>20 μM). Moreover, the low cytotoxicity of AIEgens@MOC facilitated its application as an intracellular imaging probe for HSO3, with the capability of specific lysosomal localization.

Significance

We have developed a simple and effective strategy to improve the water solubility of AIEgens for bioimaging of important biomarkers in live cells. This method avoided complex chemical modifications, and enabled efficient detection of HSO3 in biological systems. By selecting MOCs with appropriate cavity sizes, this strategy is promising to accommodate various AIEgens in the future, offering a generalizable solution to facilitate their bioimaging applications.
聚集诱导发射发光原(AIEgens)在聚集状态下表现出高效的荧光,使其成为生物成像应用的有希望的候选者。然而,它们固有的疏水结构经常导致不可控的聚集,阻碍了它们递送到靶部位进行成像。研究人员已经开发出通过结构修饰或基于载体的包封来提高AIEgens水溶性的策略。但结构修饰方法合成复杂,大环对AIEgens的包封效率往往较低。提高用于生物成像的AIEgens的水溶性需要简单而有效的策略。结果我们报道了一种利用水溶性金属有机笼(MOCs)作为宿主载体的新型超分子包封方法。包封显著地阻止了aigens的聚集,使其在水性基质中均匀分散。AIEgens@MOC配合物在亚硫酸氢盐(HSO3−)刺激前的广泛pH(5.0-9.0)、温度(10°C - 80°C)和时间(超过14天)范围内均表现出优异的结构稳定性,证实了稳定的主客体相互作用。在HSO3−刺激下,MOC的分解导致AIEgens的释放,这些AIEgens随后聚集并在60 s内表现出显著增强的荧光。新的AIEgens@MOC配合物使细胞内异常HSO3−波动(>20 μM)成功可视化。此外,AIEgens@MOC的低细胞毒性有助于其作为HSO3−的细胞内成像探针,具有特异性溶酶体定位的能力。我们已经开发了一种简单有效的策略来提高AIEgens的水溶性,用于活细胞中重要生物标志物的生物成像。该方法避免了复杂的化学修饰,能够有效地检测生物系统中的HSO3−。通过选择具有适当腔尺寸的moc,该策略有望在未来适应各种AIEgens,为促进其生物成像应用提供一种通用的解决方案。
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引用次数: 0
A smartphone-assisted dual-mode sensor for synchronous detection of Microcystin-LR in environmental water via Temperature–Multicolour dual signals 采用温度-多色双信号同步检测环境水中微囊藻毒素lr的智能手机辅助双模传感器
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-12-01 DOI: 10.1016/j.aca.2025.344977
Hongjian Lin , Yiwen Zhu , Xiaoya Chen, Huilian Sun, Xinyu Cao, Mengyu Tao, Jingqi Zhou, Hong Huang, Bingyong Lin, Longhua Guo

Background

The direct reading of a signal is one of the essential requirements for field testing. However, quantitative analysis based on a single signal is prone to false positives and false negatives, compromising monitoring reliability. Therefore, there is an urgent need for a method that can enhance the reliability of detection achieved through simple quantitative signal readings. In this work, a temperature–multicolour dual-mode sensor was fabricated based on the localized surface plasmon resonance and photothermal effects of gold nanorods (Au NRs) to enable synchronous dual-signal detection of microcystin-LR (MC-LR) in environmental water.

Results

The proposed sensor offers the advantages of sensitive, synchronous, and simple dual-signal reading with the aid of a smartphone equipped with an infrared temperature probe. Both the temperature signal (ΔT) and the multicolour signal (R/G) exhibit strong linear correlations with the concentration of MC-LR. To evaluate the sensor's environmental monitoring performance, environmental water samples from different areas were analysed. Compared with the commercial enzyme-linked immunosorbent assay method, the proposed sensor achieved a lower limit of detection and produced comparable results using only signal readings obtained with a smartphone equipped with an infrared temperature probe, without the need for additional professional equipment. Moreover, excellent recoveries were obtained in the detection of spiked environmental water samples.

Significance

Two independent signals can be used to validate each other, thereby improving the reliability of detection. Therefore, the proposed smartphone-assisted temperature–multicolour dual-mode sensor shows strong potential for point-of-care testing, particularly in water quality monitoring.
直接读取信号是现场测试的基本要求之一。然而,基于单一信号的定量分析容易出现假阳性和假阴性,影响监测的可靠性。因此,迫切需要一种方法,可以提高通过简单的定量信号读数实现的检测的可靠性。本文基于金纳米棒(Au NRs)的局部表面等离子体共振和光热效应,制备了一种温度多色双模传感器,实现了环境水中微囊藻毒素lr (MC-LR)的同步双信号检测。结果该传感器具有双信号读取灵敏、同步、简单等优点,可借助配备红外温度探头的智能手机进行读取。温度信号(ΔT)和多色信号(R/G)均与MC-LR浓度呈较强的线性相关。为了评估传感器的环境监测性能,对不同地区的环境水样进行了分析。与商用酶联免疫吸附测定方法相比,该传感器实现了较低的检测极限,并且仅使用配备红外温度探头的智能手机获得的信号读数就可以产生可比的结果,而无需额外的专业设备。此外,该方法在加标环境水样的检测中具有良好的回收率。意义两个独立的信号可以相互验证,从而提高检测的可靠性。因此,提出的智能手机辅助温度多色双模传感器在即时检测方面具有强大的潜力,特别是在水质监测方面。
{"title":"A smartphone-assisted dual-mode sensor for synchronous detection of Microcystin-LR in environmental water via Temperature–Multicolour dual signals","authors":"Hongjian Lin ,&nbsp;Yiwen Zhu ,&nbsp;Xiaoya Chen,&nbsp;Huilian Sun,&nbsp;Xinyu Cao,&nbsp;Mengyu Tao,&nbsp;Jingqi Zhou,&nbsp;Hong Huang,&nbsp;Bingyong Lin,&nbsp;Longhua Guo","doi":"10.1016/j.aca.2025.344977","DOIUrl":"10.1016/j.aca.2025.344977","url":null,"abstract":"<div><h3>Background</h3><div>The direct reading of a signal is one of the essential requirements for field testing. However, quantitative analysis based on a single signal is prone to false positives and false negatives, compromising monitoring reliability. Therefore, there is an urgent need for a method that can enhance the reliability of detection achieved through simple quantitative signal readings. In this work, a temperature–multicolour dual-mode sensor was fabricated based on the localized surface plasmon resonance and photothermal effects of gold nanorods (Au NRs) to enable synchronous dual-signal detection of microcystin-LR (MC-LR) in environmental water.</div></div><div><h3>Results</h3><div>The proposed sensor offers the advantages of sensitive, synchronous, and simple dual-signal reading with the aid of a smartphone equipped with an infrared temperature probe. Both the temperature signal (ΔT) and the multicolour signal (R/G) exhibit strong linear correlations with the concentration of MC-LR. To evaluate the sensor's environmental monitoring performance, environmental water samples from different areas were analysed. Compared with the commercial enzyme-linked immunosorbent assay method, the proposed sensor achieved a lower limit of detection and produced comparable results using only signal readings obtained with a smartphone equipped with an infrared temperature probe, without the need for additional professional equipment. Moreover, excellent recoveries were obtained in the detection of spiked environmental water samples.</div></div><div><h3>Significance</h3><div>Two independent signals can be used to validate each other, thereby improving the reliability of detection. Therefore, the proposed smartphone-assisted temperature–multicolour dual-mode sensor shows strong potential for point-of-care testing, particularly in water quality monitoring.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1384 ","pages":"Article 344977"},"PeriodicalIF":6.0,"publicationDate":"2025-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145691639","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}
引用次数: 0
Cholesterol affinity recognition for extracellular vesicle isolation and metabolomics analysis in liver disease 肝脏疾病细胞外囊泡分离和代谢组学分析中的胆固醇亲和力识别
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-30 DOI: 10.1016/j.aca.2025.344950
Shilong Zhao, Luxi Chen, Aixiang Bu, Guangyao Wu, Wenjing Yu, Lianghai Hu

Background

Extracellular vesicles (EVs), abundant in bodily fluids such as blood, urine, and saliva, have emerged as promising biomarker sources for disease diagnosis due to their rich content of metabolites, proteins, and nucleic acids. Efficient isolation of EVs remains a significant challenge. Currently, commonly used EV enrichment methods include ultracentrifugation (UC), size exclusion chromatography (SEC), antibody-based affinity methods, and polymer precipitation. These methods face limitations such as high costs, complex operations, and contamination risks. Consequently, there is an urgent need for the development of rapid and efficient methods for EV isolation.

Results

In this study, we developed a strategy for synthesizing cholesterol-imprinted polymers via a one-pot reverse microemulsion approach, enabling rapid and high-yield enrichment of urinary EVs. Notably, this approach requires only a minimal amount of sample (4 mg) to achieve rapid separation (50 min) with high recovery rate (79 %), demonstrating significant improvements in both efficiency and practicality compared to conventional techniques. Ultra-performance liquid chromatography-ion mobility-mass spectrometry, we achieved high-resolution separation and detection of EV metabolites. The analytical system demonstrated excellent sensitivity, with a signal-to-noise ratio >2000:1 for 1 pg of reserpine, and high mass accuracy (resolution ≥80,000 FWHM). Metabolomic analysis of EVs from clinical samples (9 Cirrhosis, 12 Liver cancer, and 10 Healthy controls) successfully differentiated the groups. Receiver operating characteristic (ROC) analysis of four representative metabolites yielded area under the curve (AUC) values greater than 0.7, indicating promising diagnostic potential.

Significance

In conclusion, the cholesterol-imprinted polymer developed in this study enables high-yield enrichment and isolation of EVs from 2 mL of urine within 50 min. Metabolomic analysis of the enriched urinary EVs from clinical samples successfully classified and predicted different pathological conditions. This approach provides an efficient strategy for urinary EV enrichment and offers a promising platform for broader liquid biopsy applications.
胞外囊泡(EVs)大量存在于血液、尿液和唾液等体液中,由于其丰富的代谢物、蛋白质和核酸含量,已成为疾病诊断的有前途的生物标志物来源。有效隔离电动汽车仍然是一个重大挑战。目前,常用的EV富集方法包括超离心(UC)、粒径排除色谱(SEC)、基于抗体的亲和法和聚合物沉淀法。这些方法面临成本高、操作复杂和污染风险等限制。因此,迫切需要开发快速有效的EV分离方法。结果在本研究中,我们开发了一种通过一锅反相微乳法合成胆固醇印迹聚合物的策略,实现了尿液ev的快速、高产富集。值得注意的是,这种方法只需要少量的样品(4mg)就可以实现快速分离(50分钟),回收率高(79%),与传统技术相比,在效率和实用性方面都有显着提高。采用超高效液相色谱-离子迁移质谱技术,实现了EV代谢物的高分辨率分离检测。该分析系统具有良好的灵敏度,对1 pg利血平的信噪比为2000:1,质量精度高(分辨率≥80000 FWHM)。临床样本(9例肝硬化、12例肝癌和10例健康对照)的ev代谢组学分析成功区分了各组。四种代表性代谢物的受试者工作特征(ROC)分析结果显示,曲线下面积(AUC)值大于0.7,具有良好的诊断潜力。总之,本研究开发的胆固醇印迹聚合物可以在50分钟内从2ml尿液中高效富集和分离EVs。对临床样本中富集的尿液ev进行代谢组学分析,成功地分类并预测了不同的病理状况。该方法为尿液EV富集提供了有效的策略,并为更广泛的液体活检应用提供了一个有前途的平台。
{"title":"Cholesterol affinity recognition for extracellular vesicle isolation and metabolomics analysis in liver disease","authors":"Shilong Zhao,&nbsp;Luxi Chen,&nbsp;Aixiang Bu,&nbsp;Guangyao Wu,&nbsp;Wenjing Yu,&nbsp;Lianghai Hu","doi":"10.1016/j.aca.2025.344950","DOIUrl":"10.1016/j.aca.2025.344950","url":null,"abstract":"<div><h3>Background</h3><div>Extracellular vesicles (EVs), abundant in bodily fluids such as blood, urine, and saliva, have emerged as promising biomarker sources for disease diagnosis due to their rich content of metabolites, proteins, and nucleic acids. Efficient isolation of EVs remains a significant challenge. Currently, commonly used EV enrichment methods include ultracentrifugation (UC), size exclusion chromatography (SEC), antibody-based affinity methods, and polymer precipitation. These methods face limitations such as high costs, complex operations, and contamination risks. Consequently, there is an urgent need for the development of rapid and efficient methods for EV isolation.</div></div><div><h3>Results</h3><div>In this study, we developed a strategy for synthesizing cholesterol-imprinted polymers via a one-pot reverse microemulsion approach, enabling rapid and high-yield enrichment of urinary EVs. Notably, this approach requires only a minimal amount of sample (4 mg) to achieve rapid separation (50 min) with high recovery rate (79 %), demonstrating significant improvements in both efficiency and practicality compared to conventional techniques. Ultra-performance liquid chromatography-ion mobility-mass spectrometry, we achieved high-resolution separation and detection of EV metabolites. The analytical system demonstrated excellent sensitivity, with a signal-to-noise ratio &gt;2000:1 for 1 pg of reserpine, and high mass accuracy (resolution ≥80,000 FWHM). Metabolomic analysis of EVs from clinical samples (9 Cirrhosis, 12 Liver cancer, and 10 Healthy controls) successfully differentiated the groups. Receiver operating characteristic (ROC) analysis of four representative metabolites yielded area under the curve (AUC) values greater than 0.7, indicating promising diagnostic potential.</div></div><div><h3>Significance</h3><div>In conclusion, the cholesterol-imprinted polymer developed in this study enables high-yield enrichment and isolation of EVs from 2 mL of urine within 50 min. Metabolomic analysis of the enriched urinary EVs from clinical samples successfully classified and predicted different pathological conditions. This approach provides an efficient strategy for urinary EV enrichment and offers a promising platform for broader liquid biopsy applications.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1384 ","pages":"Article 344950"},"PeriodicalIF":6.0,"publicationDate":"2025-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145619402","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}
引用次数: 0
Hydrogel-based electrochemical microneedles biosensor for sensitive monitoring of lactic acid in interstitial fluid 基于水凝胶的电化学微针生物传感器用于间质液乳酸的灵敏监测
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-30 DOI: 10.1016/j.aca.2025.344965
Yiyue Qu , Ran Chen , Jie Chen , Qian Li , Mostafa R. Abukhadra , Ahmed M. ElSherbeeny , Lili Jin , Qingwei Jiang , Shilun Feng , Shengtai Bian

Background

Lactic acid is a critical biomarker for pathology and physiological status in health and sports. Current monitoring relies on invasive blood tests performed by professionals in clinical settings, limiting accessibility, frequency, and real-time insight. This creates a significant barrier to personalized health and performance management. There is a clear need for a painless, portable, user-operable method to enable continuous lactic acid monitoring outside the lab.

Results

We present a portable hydrogel microneedle (MN) biosensor for rapid, continuous, and painless lactic acid detection in interstitial fluid (ISF). The device features a detachable electrode integrated into a MN patch, enabling both in-home and mobile use. It achieves real-time data transmission for user health management. Key performance metrics include a wide linear detection range up to 2 mM, high sensitivity of 19.45 μA mM−1 cm−2, and a low limit of detection of 3.6 μM, demonstrating its capability for accurate physiological monitoring.

Significance

This work provides a minimally invasive, cost-effective alternative to blood-based lactic acid testing, significantly improving patient compliance and accessibility. Its portability and real-time data capabilities empower individuals to proactively manage health and athletic performance. This technology represents a paradigm shift towards user-friendly point-of-care monitoring, with transformative potential for personalized healthcare and sports science applications.
乳酸是健康和运动中病理和生理状态的重要生物标志物。目前的监测依赖于临床环境中由专业人员进行的侵入性血液检查,限制了可及性、频率和实时洞察力。这对个性化运行状况和性能管理造成了重大障碍。显然需要一种无痛、便携、用户可操作的方法来实现实验室外的连续乳酸监测。结果我们提出了一种便携式水凝胶微针生物传感器,用于快速、连续、无痛地检测间质液(ISF)中的乳酸。该设备具有集成在MN贴片中的可拆卸电极,可在家庭和移动中使用。实现了用户健康管理的实时数据传输。主要性能指标为线性检测范围宽达2mm,灵敏度高达19.45 μA mM−1 cm−2,检测下限为3.6 μM,具有准确的生理监测能力。这项工作提供了一种微创的、具有成本效益的血液乳酸检测替代方法,显著提高了患者的依从性和可及性。它的便携性和实时数据功能使个人能够主动管理健康和运动表现。这项技术代表了向用户友好的护理点监测的范式转变,具有个性化医疗保健和运动科学应用的变革潜力。
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引用次数: 0
Ultrafast response recovery room temperature triethylamine sensor based on La2(WO4)3/SnO2 heterojunction 基于La2(WO4)3/SnO2异质结的超快速响应恢复室温三乙胺传感器
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-29 DOI: 10.1016/j.aca.2025.344949
Zhihua Zhao , Bingbing Wang , Zhiyi Zhang , Huiqin Li , Jingjing Tang , Peijuan Wu , Lan Wu , Qilin Zou

Background

Triethylamine (TEA), a volatile chemical marker released during seafood spoilage, not only indicates food freshness but also poses respiratory hazards, underscoring the need for reliable gas sensing. Current TEA detection technologies are often constrained by high operating temperatures, limited sensitivity in the ppb range, and sluggish response/recovery behavior, leading to excessive energy use and restricted real-world applicability. To overcome these limitations, this study focuses on developing a room-temperature TEA sensor capable of ultrasensitive and rapid detection, supporting both energy-efficient operation and sustainable monitoring solutions.

Results

We successfully synthesized SnO2 hollow spheres and La2(WO4)3 nanoparticles via a solvothermal method and constructed La2(WO4)3/SnO2 (LSO) nanocomposites with the aim of developing a highly efficient sensor for triethylamine (TEA) detection. The results show that the LSO exhibited a notable enhancement in TEA gas sensing properties at room temperature. Specifically, it was observed that the LSO-4 heterojunctions exhibited response to 100 ppm TEA could reach to 5.24, which was approximately 3.14 times better than that of pure SnO2. Density functional theory (DFT) calculations confirmed the enhanced TEA adsorption capacity of the LSO heterojunction, while clarifying the underlying electron transfer mechanism. Practical application tests showed that the sensor could effectively detect TEA, demonstrating excellent sensitivity, stability, and repeatability, thereby providing feasibility for its application in monitoring of harmful gases in the environment.

Significance

This work reports the first example of fabrication La2(WO4)3/SnO2 heterojunctions for gas sensors. The sensors can detect ppb level TEA gas at room temperature, and meanwhile, the sensors have the advantage of ultrafast response and recovery, which is not normal for the room temperature gas sensor, which thus support their practical application in the field of food quality monitoring and harmful gas control.
三乙胺(TEA)是一种挥发性化学标志物,在海鲜变质过程中释放,不仅表明食物新鲜,而且对呼吸系统造成危害,因此需要可靠的气体传感。目前的TEA检测技术通常受到高工作温度、ppb范围内有限的灵敏度以及缓慢的响应/恢复行为的限制,导致过度的能量消耗和限制了实际应用。为了克服这些限制,本研究的重点是开发一种能够超灵敏和快速检测的室温TEA传感器,支持节能操作和可持续监测解决方案。结果采用溶剂热法成功合成了SnO2空心球和La2(WO4)3纳米粒子,构建了La2(WO4)3/SnO2 (LSO)纳米复合材料,旨在开发一种高效的三乙胺(TEA)检测传感器。结果表明,LSO在室温下显著提高了TEA的气敏性能。具体而言,LSO-4异质结对100 ppm TEA的响应可达5.24,约为纯SnO2的3.14倍。密度泛函理论(DFT)计算证实了LSO异质结的TEA吸附能力增强,同时阐明了潜在的电子转移机制。实际应用测试表明,该传感器能够有效检测到TEA,具有良好的灵敏度、稳定性和重复性,为其在环境有害气体监测中的应用提供了可行性。本工作报道了用于气体传感器的La2(WO4)3/SnO2异质结的第一个例子。该传感器可以在室温下检测ppb级的TEA气体,同时具有常温气体传感器所不具备的超快响应和超快恢复的优点,支持其在食品质量监测和有害气体控制领域的实际应用。
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引用次数: 0
Sensor array based on Co-based nanozymes for rapid identification of multiple synthetic phenolic antioxidants 基于co基纳米酶的传感器阵列快速识别多种合成酚类抗氧化剂
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-29 DOI: 10.1016/j.aca.2025.344969
Xuan Xu, Baoquan Chen, Xufei Liu, Chunmeng Deng, Guanghua Mao, Dali Wei, Xiangyang Wu
Synthetic phenolic antioxidants are a class of compounds with phenolic structure prepared by chemical synthesis, which are mainly used in foods, plastics, and rubbers to slow down the oxidation process, but excessive consumption may pose a threat to human health. However, it is difficult to achieve rapid and efficient detection of multiple synthetic phenolic antioxidants by existing methods. To circumvent this issue, we prepared a novel nanozyme sensor array based on two cobalt-based nanozymes (Co-MOFs and CoOOH) with high oxidase-like activity for rapid differentiation of six synthetic phenolic antioxidants, including propyl gallate (PG), tertiary butylhydroquinone (TBHQ), butylated hydroxyanisole (BHA), butylated hydroxytoluene (BHT), 2,6-Di-tert-butyl-4-hydroxymethylphenol (BHT-OH) and 3,5-Di-tert-butyl-4-hydroxybenzoic acid (BHT-COOH). Wherein, the obtained Co-MOFs and CoOOH nanozymes showed good oxidase-like activity and exhibited high stability. Of interest, the synthetic phenolic antioxidants could differentially modulate the oxidase-like activities of Co-MOFs and CoOOH nanozymes, which could be converted into colorimetric signals. The proposed nanozyme sensor array can characterize six synthetic phenolic antioxidants and their multi-component mixtures in the concentration range of 0.015–1 mM. Our findings present a straightforward and efficient approach for identifying and quantifying synthetic phenolic antioxidants, advancing the development of sensor array technologies for detecting diverse contaminants in environmental monitoring and food safety applications.
合成酚类抗氧化剂是一类通过化学合成制备的具有酚类结构的化合物,主要用于食品、塑料、橡胶中,以减缓氧化过程,但过量食用可能对人体健康构成威胁。然而,现有方法难以实现对多种合成酚类抗氧化剂的快速高效检测。为了解决这一问题,我们基于两种具有高氧化酶活性的钴基纳米酶(Co-MOFs和CoOOH)制备了一种新型纳米酶传感器阵列,用于快速分化6种合成酚类抗氧化剂,包括没食子酸丙酯(PG)、叔丁基对苯二酚(TBHQ)、丁基羟基异醇醚(BHA)、丁基羟基甲苯(BHT)、2,6-二叔丁基-4-羟基甲基苯酚(BHT- oh)和3,5-二叔丁基-4-羟基苯甲酸(BHT- cooh)。其中,得到的co - mof和CoOOH纳米酶表现出良好的类氧化酶活性和较高的稳定性。值得注意的是,合成的酚类抗氧化剂可以不同地调节co - mof和CoOOH纳米酶的类氧化酶活性,并将其转化为比色信号。所提出的纳米酶传感器阵列可以表征六种合成酚类抗氧化剂及其浓度范围为0.015-1 mM的多组分混合物。我们的研究结果为识别和定量合成酚类抗氧化剂提供了一种简单有效的方法,推动了传感器阵列技术在环境监测和食品安全应用中检测各种污染物的发展。
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引用次数: 0
Carbon dot-enhanced nanobody-based fluorescence immunoassay for ultrasensitive Listeria monocytogenes detection in dairy products 基于碳点增强纳米体的荧光免疫分析法用于乳制品中单核细胞增生李斯特菌的超灵敏检测
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-29 DOI: 10.1016/j.aca.2025.344954
Xuan Liu , Shurong Li , Juan Wei , Xueyi Fan , Kai Zheng , Qinkai Yang , Xiaohui Du , Ruixue Feng , Peixiang Wang , Jianlong Wang , Yanru Wang
Listeria monocytogenes (L. monocytogenes), a psychrophilic Gram-positive bacterium, causes severe foodborne listeriosis outbreaks. However, rapid, accurate diagnostic assays for this pathogen in complex food matrices remain limited. Herein, we established a phage-displayed nanobody (Nb) library by immunizing a bactrian camel with inactivated L. monocytogenes. After biopanning, four specific Nbs were obtained with good specificity and thermal stability. Using soluble Nbs as capture antibodies and phage-displayed nanobodies as detecting antibodies, a fluorescent ELISA for L. monocytogenes was constructed by employing carbon dots as fluorescent probes based on the inner filter effect-mediated quenching. The developed assay exhibited a limit of detection of 3.21 × 103 CFU/mL, demonstrating a 144-fold enhancement over conventional ELISA, enabling highly sensitive and specific pathogen detection. In real sample analysis, the average recoveries ranged from 97.6 to 119.6 % and the relative standard deviation below 6.3 %, showcasing significant potential in food analysis applications.
单核增生李斯特菌(L. monocytogenes)是一种嗜冷的革兰氏阳性细菌,可引起严重的食源性李斯特菌病暴发。然而,在复杂的食物基质中快速、准确地诊断这种病原体的方法仍然有限。在此,我们用灭活的单核细胞增生乳杆菌免疫双峰驼,建立了噬菌体展示纳米体(Nb)文库。经过生物筛选,获得了4种特异性的Nbs,具有良好的特异性和热稳定性。以可溶性Nbs作为捕获抗体,噬菌体展示纳米体作为检测抗体,利用碳点作为荧光探针,基于内过滤效应介导猝灭,构建了单核细胞增生性乳杆菌的荧光酶联免疫吸附测定(ELISA)。该方法的检出限为3.21 × 103 CFU/mL,比传统ELISA提高了144倍,具有较高的灵敏度和特异性。在实际样品分析中,平均加样回收率为97.6% ~ 119.6%,相对标准偏差小于6.3%,在食品分析中具有较大的应用潜力。
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引用次数: 0
Photoelectrochemical detection of epigenetic 5-hydroxymethylcytosine based on Cu2O@CuO@Ag and self-triggered isothermal amplification 基于Cu2O@CuO@Ag和自触发等温扩增的表观遗传5-羟甲基胞嘧啶的光电化学检测
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-29 DOI: 10.1016/j.aca.2025.344968
Huamin Liu , Ziyi Zheng , Can Zhou , Zixin Chen , Kexing Peng , Chenghong Li , Hui Huang , Lina Wang , Yi Liu , Lulu Li , Shuang Xu , Yimei Li , Yiyuqing Yang , Yang Xiang , Junsong Zheng

Background

Epigenetic DNA hydroxymethylation, particularly 5-hydroxymethylcytosine (5hmC), has emerged as a promising biomarker for early and specific tumor diagnosis. This modification serves as a critical regulator of gene expression, and its aberrant levels correlate directly with tumor initiation, metastasis, and therapeutic resistance. Quantitative analysis of sequence-specific 5hmC modifications offers valuable insights into dynamic epigenetic patterns associated with disease progression. Consequently, developing highly sensitive methods for quantitative detection of 5hmC is crucial for advancing epigenetic detection and diagnosis.

Results

In this study, we engineered a novel photoelectrochemical (PEC) biosensor for ultrasensitive detection of the epigenetic biomarker 5hmC. The sensor utilized a ternary heterojunction Cu2O@CuO@Ag as the photoactive material, whose unique band structure facilitated efficient charge separation and generated a stable initial photocurrent. The detection mechanism initiated with a click chemistry-mediated azide reaction targeting 5hmC, forming Y-shaped DNA scaffolds. These scaffolds activated a self-triggered isothermal amplification cascade, enzymatically recycling trace targets into abundant trigger P sequences. Subsequently, alkaline phosphatase (ALP)-conjugated probes catalyzed the hydrolysis of ascorbic acid phosphate (AAP), producing ascorbic acid (AA) as an electron donor. The amplified AA significantly enhanced electron transfer to the photoanode, enabling quantification of 5hmC DNA in buffer down to 0.56 fM with high specificity. This integrated signal amplification strategy provides a powerful platform for epigenetic analysis in clinical diagnostics.

Significance

In conclusion, this strategy offers a novel approach for ultrasensitive quantification of natural DNA base modifications (e.g., 5hmC). By integrating ternary Cu2O@CuO@Ag heterojunction photoanodes with self-triggered isothermal amplification, it achieved 0.56 fM detection limit, opening avenues for clinical epigenetics, early cancer screening, and liquid biopsy applications in complex samples.
去遗传DNA羟甲基化,特别是5-羟甲基胞嘧啶(5hmC),已成为早期和特异性肿瘤诊断的有前景的生物标志物。这种修饰是基因表达的关键调控因子,其异常水平与肿瘤的发生、转移和治疗耐药性直接相关。序列特异性5hmC修饰的定量分析为与疾病进展相关的动态表观遗传模式提供了有价值的见解。因此,开发高灵敏度的5hmC定量检测方法对于推进表观遗传检测和诊断至关重要。结果本研究设计了一种新型的光电化学(PEC)生物传感器,用于超灵敏检测表观遗传生物标志物5hmC。该传感器采用三元异质结Cu2O@CuO@Ag作为光活性材料,其独特的能带结构有利于有效的电荷分离,并产生稳定的初始光电流。检测机制以靶向5hmC的点击化学介导的叠氮化物反应开始,形成y形DNA支架。这些支架激活了一个自触发的等温扩增级联,酶循环痕量靶标成丰富的触发P序列。随后,碱性磷酸酶(ALP)偶联探针催化抗坏血酸磷酸(AAP)的水解,产生抗坏血酸(AA)作为电子供体。扩增的AA显着增强了电子向光阳极的转移,使缓冲液中的5hmC DNA的定量降低到0.56 fM,具有高特异性。这种集成的信号放大策略为临床诊断中的表观遗传分析提供了一个强大的平台。总之,该策略为天然DNA碱基修饰(如5hmC)的超灵敏定量提供了一种新方法。通过将三元Cu2O@CuO@Ag异质结光阳极与自触发等温扩增相结合,达到了0.56 fM的检测限,为临床表观遗传学、早期癌症筛查和复杂样品的液体活检应用开辟了道路。
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引用次数: 0
期刊
Analytica Chimica Acta
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