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Unimolecular Cucurbit[7]uril-Based Indicator Displacement Assay with Dual Signal-Readout for the Detection of Drugs 基于葫芦[7]脲的单分子指示剂位移测定法与双信号读出法检测药物
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-05 DOI: 10.1002/anse.202400025
Pierre Picchetti, Maria Vittoria Balli, Seth Baker, Nilima Manoj Kumar, Patrick Gruhs, Luca Prodi, Frank Biedermann

Point-of-care diagnostics relies on optical and electrochemical sensors to develop devices that are both compact and cost-effective. Therefore, the search for new design principles for chemosensors that enable multiple signal outputs is a particularly interesting concept. In this work, we present an unimolecular chemosensor based on cucurbit[7]uril that combines two signal readouts - namely fluorescent and electrochemical signals - in a single chemosensor design. This is achieved by utilizing the tunable fluorescence and the electrochemical properties of the reporter molecule, which depend on whether or not it is engulfed by the cucurbit[7]uril cavity in the absence or presence of the analyte. By setting up an assay using the dual readout chemosensor, illicit drug formulations containing pancuronium bromide or nicotine can be detected at low micromolar concentrations (0–100 μM). This assay is compatible with standard fluorescence plate readers and electrochemical devices, including commercially available screen-printed electrodes. Overall, the chemosensor presented in this study represents a significant advance in the development of cucurbit[7]uril chemosensors, characterized by multimodal detection capabilities. It uniquely combines traditional optical and electrochemical detection methods in a single molecular design.

床旁诊断依赖于光学和电化学传感器,以开发结构紧凑、成本效益高的设备。因此,寻找能实现多信号输出的化学传感器的新设计原则是一个特别有趣的概念。在这项工作中,我们介绍了一种基于葫芦[7]脲的单分子化学传感器,它在单一化学传感器设计中结合了两种信号读出方式,即荧光信号和电化学信号。这是通过利用报告分子的可调荧光和电化学特性来实现的,这取决于报告分子是否被葫芦[7]脲空腔吞噬。通过使用双读出化学传感器建立检测方法,可以在低微摩尔浓度(0 - 100 μM)下检测含有泮库溴铵或尼古丁的非法药物制剂。这种检测方法与标准荧光平板阅读器和电化学装置兼容,包括市售的丝网印刷电极(SPE)。总之,本研究中介绍的化学传感器是葫芦素[7]脲化学传感器开发领域的一大进步,具有多模式检测能力。它在单一分子设计中独特地结合了传统的光学和电化学检测方法。
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引用次数: 0
In Situ pH Modulation for Enhanced Chemical Sensing: Strategies and Applications 用于增强化学传感的原位 pH 值调节:策略与应用
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-03 DOI: 10.1002/anse.202400013
Fabian Steininger, Klaus Koren

pH is one of the key parameters in chemistry and impacts almost all chemical and biological processes. Also, within analytical chemistry and sensing, pH plays a critical role. This review underscores the critical role of pH manipulation in overcoming analytical challenges posed by complex sample matrices and dynamic environmental conditions. It explores the available tools to control pH at a local scale and how those are or can be applied to improve sensor performance. We focus on four key areas where pH modulation has been or could be leveraged to advance chemical sensing capabilities: i) sensing alkalinity and buffer capacity, ii) sample pretreatment, iii) sensing pH dependent analytes and iv) reducing biofouling. We analyze existing strategies, but also try to identify unexplored possibilities which may have potential and can be exploited for sensing.

pH 值是化学中的关键参数之一,影响着几乎所有化学和生物过程。此外,在分析化学和传感领域,pH 值也起着至关重要的作用。本综述强调了 pH 值控制在克服复杂样品基质和动态环境条件带来的分析挑战中的关键作用。它探讨了在局部范围内控制 pH 值的可用工具,以及如何应用这些工具来提高传感器性能。我们将重点放在已经或可以利用 pH 值调节来提高化学传感能力的四个关键领域:i) 传感碱度和缓冲能力;ii) 样品预处理;iii) 传感 pH 值依赖性分析物;iv) 减少生物污损。我们分析了现有的策略,同时也试图找出尚未探索的、可能具有潜力并可用于传感的可能性。
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引用次数: 0
Bimetallic Nanoparticles as Electrochemical Labels in Immunosensors for the Detection of Biomarkers of Clinical Interest 双金属纳米粒子作为免疫传感器中的电化学标签,用于检测临床相关的生物标记物
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-05-17 DOI: 10.1002/anse.202400017
David Valero-Calvo, Francisco Javier García-Alonso, Alfredo de la Escosura-Muñiz

Electrochemical immunosensors have emerged in the last years as outstanding analytical systems for the detection of analytes of clinical interest. As alternative to the traditional enzymatic labels, the use of nanoparticles and especially bimetallic ones has gained increased attention thanks to their advantages related to the higher simplicity, stability and sensitivity offered. Main routes for the detection of such nanoparticle labels are based on i) dissolution of the nanoparticle into the corresponding metal ions followed by voltammetric detection; ii) taking advantage of the electrocatalytic effect of the metals towards secondary reactions; and iii) taking advantage of their electrochemiluminescence properties.

近年来,电化学免疫传感器已成为检测临床相关分析物的杰出分析系统。作为传统酶标记的替代品,纳米粒子,尤其是双金属纳米粒子的使用越来越受到关注,这是因为它们具有更简便、更稳定和更灵敏的优点。检测此类纳米粒子标签的主要方法有:i) 将纳米粒子溶解到相应的金属离子中,然后进行伏安检测;ii) 利用金属对二次反应的电催化效应;iii) 利用其电化学发光特性。在此背景下,本综述介绍了在免疫传感器中使用双金属纳米粒子作为电化学标签检测临床分析物的最新趋势。本综述介绍了在免疫传感器中使用双金属纳米粒子作为电化学标签检测临床感兴趣的分析物的最新趋势,并提供了分析性能和文献中发现的主要方法的重要概述,最后介绍了该领域的未来展望和前景。
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引用次数: 0
Small-Molecule Fluorescent Probes for Plant Hormones and their Receptors 植物激素及其受体的小分子荧光探针
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-05-14 DOI: 10.1002/anse.202400020
Zibo Lin, Junhao Xiong, Zihao Zhou, Prof. Qiong Chen, Prof. Jun Yin

Plant hormones and their receptors play a crucial role in regulating plant growth and adapting to the stress environment. The exploration of interaction between plant hormones and their receptors is significant to comprehend the molecular mechanisms of plant growth and development, the response mechanisms of adaptation to environmental changes, and to optimize the traits and stress-resistance of crops. Since the biosynthesis, transport, and metabolism of hormones in plants are closely relevant to spatio-temporal changes, and their content and distribution are highly dynamic, there is an urgent need for a qualitative and quantitative tool to accurately, real-time, and in situ monitor the dynamic changes of hormones in plants without injury. Fluorescent probes have been widely used in the sensing and imaging of plant hormones and their receptors, due to their high spatio-temporal resolution, high selectivity, non-invasive, high sensitivity, and tailored molecular structures. Here, this paper provides a systematical overview of the research progress in the sensing and imaging of plant hormones and their receptors using fluorescent probes. In addition, the potential prospects and remaining challenges are also discussed to design fluorescent probes with better performance and promote the development of this field.

植物激素及其受体在调节植物生长和适应胁迫环境方面起着至关重要的作用。探索植物激素及其受体之间的相互作用对于理解植物生长发育的分子机制、适应环境变化的响应机制以及优化作物性状和抗逆性具有重要意义。由于植物体内激素的生物合成、转运和代谢与时空变化密切相关,其含量和分布也高度动态,因此迫切需要一种定性和定量的工具来准确、实时和原位监测植物体内激素的动态变化而不受伤害。荧光探针具有高时空分辨率、高选择性、非侵入性、高灵敏度和定制分子结构等特点,已被广泛应用于植物激素及其受体的传感和成像。本文系统概述了利用荧光探针对植物激素及其受体进行传感和成像的研究进展。此外,还讨论了潜在的前景和仍然存在的挑战,以期设计出性能更优的荧光探针,推动该领域的发展。
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引用次数: 0
Synthesis of Stable 2D Conductive Lanthanide Organic Frameworks (Lu-HHTP) for High-Performance Humidity Sensors 为高性能湿度传感器合成稳定的二维导电镧系元素有机框架 (Lu-HHTP)
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-05-09 DOI: 10.1002/anse.202400024
Dr. Shan Jiang, Xichao Mo, Xuefei Zhao, Xiaohui Yan, Zhaorui Zhang, Jiahao Liu, Huashuai Hu, Nan Wang, Prof. Minghui Yang

Two-dimensional conductive metal-organic frameworks (MOFs) featuring structural diversity and high porosity represent promising platforms for chemiresistive humidity sensing. The precise control of the structure of lanthanide-based MOFs and an exploration of its impact on charge transport and sensing applications have consistently been focal points for researchers. In this study, we present the synthesis and characterization of Lu-HHTP (HHTP=2,3,6,7,10,11-hexahydroxytriphenylene) as highly crystalline and conductive porous materials. The polymeric framework of Lu-HHTP encompasses 1D hexagonal channels and exhibits interlayer π–π stacking, resulting in a material with a high surface area and uniform rod-like microstructure. Benefiting from its elevated electrical conductivity, the Lu-HHTP-based humidity sensor exhibited commendable sensing properties within the relative humidity range of 33 % to 95 % at room temperature (25 °C), achieving a response value as high as 19 at 95 % relative humidity. Furthermore, the sensor displayed superior repeatability, characterized by rapid response and recovery speeds in the presence of moisture. These findings indicate that Lu-HHTP holds substantial promise as a material for humidity sensors.

具有结构多样性和高孔隙率的二维导电金属有机框架(MOFs)是化学电阻湿度传感的理想平台。如何精确控制镧系元素基 MOF 的结构,并探索其对电荷传输和传感应用的影响,一直是研究人员关注的焦点。在本研究中,我们合成并表征了高结晶导电多孔材料 Lu-HHTP(HHTP = 2,3,6,7,10,11-六羟基三亚苯)。Lu-HHTP 的聚合物框架包括一维六边形通道,并呈现层间 π-π 堆积,从而形成了一种具有高表面积和均匀棒状微结构的材料。得益于其较高的导电性,基于 Lu-HHTP 的湿度传感器在室温(25°C)下 33% 至 95% 的相对湿度范围内表现出令人称道的传感性能,在 95% 的相对湿度下响应值高达 19。此外,该传感器还表现出优异的可重复性,其特点是在潮湿环境中响应和恢复速度快。这些研究结果表明,Lu-HHTP 很有希望成为湿度传感器的一种材料。
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引用次数: 0
Odor Biosensors Based on Cell Expressing Olfactory Receptor: Recent Advances 基于表达嗅觉受体细胞的气味生物传感器:最新进展
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-04-26 DOI: 10.1002/anse.202400006
Hongchao Deng, Takamichi Nakamoto

Inspired by the powerful biological olfaction, scientists extracted numerous materials such as olfactory sensory neuron, olfactory receptor (OR) protein, and odorant binding protein from animal olfactory systems, then combined them with transducers to form multiple odor biosensors. These biosensors, despite well inheriting the sensing ability of creatures, have several drawbacks, such as complex preparation process, unstable sensing material characteristics, and high cost. Unlike the biological materials listed above, cell expressing heterologous OR maintains a stable sensing performance after passaging for multiple generations, also its experimental operation is simple, and cost is low. Therefore, odor biosensors based on cell expressing OR have been well developed in recent years. In this review, we first listed several odor biosensors based on cell expressing OR, mainly focusing on fluorescent and electrophysiological measurement methods. Furthermore, we illustrated the techniques to improve the biosensor performance, e. g., wider detection range, longer lifetime, more OR types, and higher quantification efficiency. In addition, we explained the possible prospects such as big sensor array and predicting odor response.

受到强大的生物嗅觉的启发,科学家们从动物嗅觉系统中提取了嗅觉感觉神经元、嗅觉受体(OR)蛋白和气味结合蛋白等多种材料,然后将它们与传感器相结合,形成了多种气味生物传感器。这些生物传感器虽然很好地继承了生物的传感能力,但也存在一些缺点,如制备过程复杂、传感材料特性不稳定、成本高昂等。与上述生物材料不同,表达异源 OR 的细胞经过多代传代后仍能保持稳定的传感性能,而且实验操作简单、成本低。因此,基于细胞表达 OR 的气味生物传感器近年来得到了很好的发展。在这篇综述中,我们首先列举了几种基于细胞表达 OR 的气味生物传感器,主要集中在荧光和电生理测量方法上。此外,我们还介绍了提高生物传感器性能的技术,如更宽的检测范围、更长的寿命、更多的 OR 类型和更高的定量效率。此外,我们还解释了大型传感器阵列和预测气味反应等可能的前景。
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引用次数: 0
Flexible Dual-Channel Molecularly Imprinted Electrochemical Sensor for Simultaneously Monitoring Sweat Cortisol and Lactate Levels 用于同时监测汗液皮质醇和乳酸盐水平的柔性双通道分子印迹电化学传感器
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-04-23 DOI: 10.1002/anse.202400003
Siying Pei, Dr. Wenhui Ji, Ya Yang, Tianwei Liu, Shuo Yang, Prof. Dr. Jiayi Wu, Jiangxuan Dai, Dr. Xiyan Hou, Qiong Wu, Prof. Dr. Lin Li

While exercise offers significant potential to enhance overall well-being, unscientific exercise practices often cause exercise fatigue, posing a threat to human health. Flexible sweat sensors have garnered considerable attention owing to their ability to continuously, non-invasively, and dynamically monitor human health during exercise at the molecular level. Therefore, in this study, we constructed a flexible molecularly imprinted polymer (MIP) sensor for the real-time monitoring of cortisol and lactate levels in sweat using cortisol or lactate as template molecules and pyrrole (Py) as functional monomer. Prussian blue (PB) was embedded into the MIP as a built-in redox probe, eliminating the need for an additional probe and facilitating the simultaneous quantification of cortisol and lactate concentrations. Moreover, the MIP-doped platinum nanoparticles (PtNPs) ehanced the electron transfer capability, further improving the sensitivity of the sensors. The fabricated flexibile cortisol and lactate MIP sensors demonstrated low limits of detection (LOD; 1.07 nM and 1.09 mM, respectively), high sensitivity (0.09 μA lg[nM]−1 and 1.28 μA lg[nM]−1), and exceptional stability and selectivity. The flexible MIP sensors could continuously and dynamically monitor changes in sweat cortisol and lactate concentrations, thus contributing to the advancement of next-generation flexible sweat electrochemical sensors and providing a crucial tool for monitoring exercise fatigue.

虽然运动具有提高整体健康水平的巨大潜力,但不科学的运动方式往往会造成运动疲劳,对人体健康构成威胁。柔性汗液传感器能够在分子水平上连续、无创、动态地监测运动过程中的人体健康状况,因此备受关注。因此,在本研究中,我们以皮质醇或乳酸盐为模板分子,以吡咯(Py)为功能单体,构建了一种用于实时监测汗液中皮质醇和乳酸盐水平的柔性分子印迹聚合物(MIP)传感器。普鲁士蓝(PB)作为内置氧化还原探针被嵌入 MIP 中,从而无需额外的探针,便于同时量化皮质醇和乳酸盐的浓度。此外,掺杂铂纳米粒子(PtNPs)的 MIP 增强了电子传递能力,进一步提高了传感器的灵敏度。制造出的柔性皮质醇和乳酸盐 MIP 传感器具有低检测限(LOD,分别为 1.07 nM 和 1.09 mM)、高灵敏度(0.09 μA lg[nM]-1 和 1.28 μA lg[nM]-1)、优异的稳定性和选择性。柔性 MIP 传感器可以连续、动态地监测汗液中皮质醇和乳酸浓度的变化,从而推动了下一代柔性汗液电化学传感器的发展,并为监测运动疲劳提供了重要工具。
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引用次数: 0
Upconversion Luminescence Based Direct Hybridization Assay to Detect Subfemtomolar miR-20 a DNA Analogue in Plasma 基于上转换发光的直接杂交测定法检测血浆中的亚母摩尔 miR-20a DNA 类似物
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-04-22 DOI: 10.1002/anse.202400005
Saara Kuusinen, Satu Lahtinen, Tero Soukka

MicroRNAs (miRNAs) are promising biomarkers especially for early-stage cancer diagnostics, but the implementation of miRNA-based diagnostic tests is still hindered by the limitations of current analytical methods. The small size, low concentrations in biofluids and high sequence homology of miRNAs are challenges for assay development. Currently, most of the sensitive detection methods rely on enzymatic amplification steps, which complicate the analysis and can lead to biases in quantitation. Therefore, there is an increasing need to develop enzyme-free detection methods that are sensitive, specific and user-friendly. In this study, a simple direct hybridization assay for the DNA analogue of miR-20a was developed. The assay is based on upconverting nanoparticle labels, which enable ultrasensitive detection, and hairpin structured probes, which provide additional hybridization stability due to base stacking. The limit of detection was 0.73 fM with plasma recoveries between 76 % and 111 %, demonstrating that the assay could be used for direct detection of miRNAs from complex sample matrices without isolation of RNA. Due to the simplicity and the excellent sensitivity for an amplification-free method, the assay has a great potential for miRNA-based clinical applications.

微小核糖核酸(miRNA)是很有前途的生物标志物,尤其是在早期癌症诊断方面,但基于 miRNA 的诊断测试的实施仍然受到目前分析方法局限性的阻碍。miRNA 体积小、在生物流体中浓度低、序列同源性高,这些都是检测方法开发所面临的挑战。目前,大多数灵敏的检测方法都依赖于酶扩增步骤,这使分析变得复杂,并可能导致定量出现偏差。因此,人们越来越需要开发灵敏、特异且操作简便的无酶检测方法。本研究开发了一种简单的直接杂交检测 miR-20a DNA 类似物的方法。该检测方法基于上转换纳米粒子标签和发夹结构探针,前者可实现超灵敏检测,后者则可通过碱基堆叠提供额外的杂交稳定性。检测限为 0.73 fM,血浆回收率在 76% 至 111% 之间,这表明该测定可用于直接检测复杂样品基质中的 miRNA,而无需分离 RNA。由于无扩增方法简便、灵敏度高,该测定在基于 miRNA 的临床应用中具有巨大潜力。
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引用次数: 0
Simultaneous Detection of Multiple Biomarkers by Peptide Nucleic Acids-Based Triplex Molecular Beacon in a Nanopore 通过纳米孔中基于多肽核酸的三重分子信标同时检测多种生物标记物
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-04-17 DOI: 10.1002/anse.202400002
Dr. Bingyuan Guo, Dr. Yun Zhang, Qianyuan Ren, Dr. Ke Zhou, Dr. Lei Liu, Prof. Hai-Chen Wu

In this study, we propose an enhanced nanopore sensing strategy that utilizes a peptide nucleic acid (PNA)-based triplex molecular beacon sensor to achieve the simultaneous detection of multiple biomarkers with a high degree of sensitivity. The sensor is a triplex switch composed of a triplex-forming DNA strand and an oligo-arginine-tagged PNA strand, serving as the target recognition moiety and signal output element, respectively. Upon target binding to the recognition element of the sensor, the PNA signal output strand is released and a hybrid complex of the target-DNA recognition strand is formed simultaneously. Due to the positive charges carried by the PNA-Arg strands, they could be driven through the nanopore under positive electric field, effectively eliminating interferences from co-existing target-DNA complexes. This approach enables label-free, one-step detection of targets without requiring complex treatments and procedures. Leveraging the modular properties of DNA recognition strand, this method can be applied universally, and here, we successfully demonstrate its application using three SARS-CoV-2 related biomarkers.

在本研究中,我们提出了一种增强型纳米孔传感策略,利用基于肽核酸(PNA)的三重分子信标传感器,实现高灵敏度地同时检测多种生物标记物。该传感器是一个三重开关,由三重形成的 DNA 链和寡精氨酸标记的 PNA 链组成,分别作为目标识别分子和信号输出元件。当目标物与传感器的识别元件结合时,PNA 信号输出链被释放,同时形成目标物-DNA 识别链的杂交复合物。由于 PNA-Arg 链带有正电荷,它们可以在正电场的作用下通过纳米孔,从而有效地消除了同时存在的靶标-DNA 复合物的干扰。这种方法无需复杂的处理和程序,就能实现无标记、一步到位的目标检测。利用 DNA 识别链的模块化特性,这种方法可以普遍应用,在此,我们利用三种与 SARS-CoV-2 相关的生物标记物成功地展示了这种方法的应用。
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引用次数: 0
MRI Probes for In Vivo Aldehyde Sensing 用于体内醛感应的核磁共振探针
IF 3.4 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-04-10 DOI: 10.1002/anse.202300087
Alexia Kirby, Mojmír Suchý, Adam J. Shuhendler

Endogenous aldehydes are produced via tightly regulated metabolic processes and are rapidly cleared by aldehyde dehydrogenases. However, dysregulation of these processes leads to accumulation of toxic aldehydes in affected tissues, resulting in electrophilic stress forming pathogenic DNA- and protein-adducts. The highly reactive aldehydes contribute to numerous pathologies including traumatic brain injury, cancer, cardiovascular diseases, and fibrosis. Due to their transient nature and electrophilicity, the development of molecular imaging probes with the ability to trap and detect aldehydes in vivo remains a challenge. Herein, two classes of aldehyde-mapping MRI probes are discussed: (1) gadolinium and manganese-containing macrocyclic MRI agents targeting extracellular aldehydes produced during active tissue fibrosis, and (2) metal-free hydrazoCEST-MRI agents for total intracellular aldehyde detection. This comprehensive review outlines the development, mechanisms, and potential applications of diverse MRI probes targeting aldehydes, aiming to advance non-invasive diagnostic tools, disease staging, and therapeutic interventions in multiple pathologies.

内源性醛通过严格调节的代谢过程产生,并通过醛脱氢酶迅速清除。然而,这些过程的失调会导致有毒醛类在受影响的组织中积累,从而产生亲电压力,形成致病的 DNA 和蛋白质加合物。高活性醛类物质会导致多种病症,包括创伤性脑损伤、癌症、心血管疾病和纤维化。由于醛的瞬时性和亲电性,开发能够捕获和检测体内醛的分子成像探针仍是一项挑战。本文讨论了两类醛映射 MRI 探针:(1) 针对活跃组织纤维化过程中产生的细胞外醛的含钆和含锰大环 MRI 探针;(2) 用于细胞内总体醛检测的不含金属的 hydrazoCEST-MRI 探针。本综述概述了针对醛类的各种磁共振成像探针的开发、机制和潜在应用,旨在推进多种病症的无创诊断工具、疾病分期和治疗干预。
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引用次数: 0
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