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Advances and Perspectives of Responsive Probes for Measuring γ-Glutamyl Transpeptidase γ-谷氨酰转肽酶响应探针的研究进展与展望
Q3 Chemistry Pub Date : 2023-12-04 DOI: 10.1021/acsmeasuresciau.3c00045
Yiming Zhang, Zexi Zhang, Miaomiao Wu and Run Zhang*, 

Gamma-glutamyltransferase (GGT) is a plasma-membrane-bound enzyme that is involved in the γ-glutamyl cycle, like metabolism of glutathione (GSH). This enzyme plays an important role in protecting cells from oxidative stress, thus being tested as a key biomarker for several medical conditions, such as liver injury, carcinogenesis, and tumor progression. For measuring GGT activity, a number of bioanalytical methods have emerged, such as chromatography, colorimetric, electrochemical, and luminescence analyses. Among these approaches, probes that can specifically respond to GGT are contributing significantly to measuring its activity in vitro and in vivo. This review thus aims to highlight the recent advances in the development of responsive probes for GGT measurement and their practical applications. Responsive probes for fluorescence analysis, including “off–on”, near-infrared (NIR), two-photon, and ratiometric fluorescence response probes, are initially summarized, followed by discussing the advances in the development of other probes, such as bioluminescence, chemiluminescence, photoacoustic, Raman, magnetic resonance imaging (MRI), and positron emission tomography (PET). The practical applications of the responsive probes in cancer diagnosis and treatment monitoring and GGT inhibitor screening are then highlighted. Based on this information, the advantages, challenges, and prospects of responsive probe technology for GGT measurement are analyzed.

γ-谷氨酰转移酶(GGT)是一种质膜结合酶,参与γ-谷氨酰循环,如谷胱甘肽(GSH)的代谢。这种酶在保护细胞免受氧化应激方面起着重要作用,因此被测试为几种医学状况的关键生物标志物,如肝损伤、致癌和肿瘤进展。为了测量GGT活性,出现了许多生物分析方法,如色谱法、比色法、电化学和发光分析。在这些方法中,能够特异性响应GGT的探针在体外和体内测量其活性方面做出了重大贡献。因此,本综述旨在强调用于GGT测量的响应探针的发展及其实际应用的最新进展。本文首先总结了用于荧光分析的响应探针,包括“开关”、近红外(NIR)、双光子和比例荧光响应探针,然后讨论了其他探针的发展进展,如生物发光、化学发光、光声、拉曼、磁共振成像(MRI)和正电子发射断层扫描(PET)。然后重点介绍了反应性探针在癌症诊断和治疗监测以及GGT抑制剂筛选中的实际应用。在此基础上,分析了响应式探针技术在GGT测量中的优势、挑战和前景。
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引用次数: 0
The Growing Influence of Mass Spectrometry in Measurement Science 质谱法在测量科学中日益增长的影响
Q3 Chemistry Pub Date : 2023-11-30 DOI: 10.1021/acsmeasuresciau.3c00065
Abraham K. Badu-Tawiah*, 
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引用次数: 0
Interfacing Aptamer-Modified Nanopipettes with Neuronal Media and Ex Vivo Brain Tissue 适配体修饰的纳米吸管与神经元介质和离体脑组织的连接
Q3 Chemistry Pub Date : 2023-11-22 DOI: 10.1021/acsmeasuresciau.3c00047
Annina Stuber, Anna Cavaccini, Andreea Manole, Anna Burdina, Yassine Massoud, Tommaso Patriarchi, Theofanis Karayannis and Nako Nakatsuka*, 

Aptamer-functionalized biosensors exhibit high selectivity for monitoring neurotransmitters in complex environments. We translated nanoscale aptamer-modified nanopipette sensors to detect endogenous dopamine release in vitro and ex vivo. These sensors employ quartz nanopipettes with nanoscale pores (ca. 10 nm diameter) that are functionalized with aptamers that enable the selective capture of dopamine through target-specific conformational changes. The dynamic behavior of aptamer structures upon dopamine binding leads to the rearrangement of surface charge within the nanopore, resulting in measurable changes in ionic current. To assess sensor performance in real time, we designed a fluidic platform to characterize the temporal dynamics of nanopipette sensors. We then conducted differential biosensing by deploying control sensors modified with nonspecific DNA alongside dopamine-specific sensors in biological milieu. Our results confirm the functionality of aptamer-modified nanopipettes for direct measurements in undiluted complex fluids, specifically in the culture media of human-induced pluripotent stem cell-derived dopaminergic neurons. Moreover, sensor implantation and repeated measurements in acute brain slices was possible, likely owing to the protected sensing area inside nanoscale DNA-filled orifices, minimizing exposure to nonspecific interferents and preventing clogging. Further, differential recordings of endogenous dopamine released through electrical stimulation in the dorsolateral striatum demonstrate the potential of aptamer-modified nanopipettes for ex vivo recordings with unprecedented spatial resolution and reduced tissue damage.

适配体功能化的生物传感器在复杂环境中监测神经递质具有高选择性。我们翻译了纳米级适配体修饰的纳米吸管传感器来检测内源性多巴胺的体外和体外释放。这些传感器采用带有纳米级孔(直径约10纳米)的石英纳米吸管,这些孔被适体功能化,能够通过靶向特异性构象变化选择性捕获多巴胺。多巴胺结合后适配体结构的动态行为导致纳米孔内表面电荷的重排,导致离子电流的可测量变化。为了实时评估传感器的性能,我们设计了一个流体平台来表征纳米吸管传感器的时间动态。然后,我们通过在生物环境中部署用非特异性DNA修饰的控制传感器和多巴胺特异性传感器来进行差异生物传感。我们的研究结果证实了适配体修饰的纳米吸管在未稀释的复杂液体中直接测量的功能,特别是在人类诱导的多能干细胞衍生的多巴胺能神经元的培养基中。此外,在急性脑切片中植入传感器和重复测量是可能的,这可能是由于纳米级dna填充孔内受保护的传感区域,最大限度地减少了暴露于非特异性干扰物并防止堵塞。此外,通过电刺激在背侧纹状体释放内源性多巴胺的差异记录表明,适体修饰的纳米管具有前所未有的空间分辨率和减少组织损伤的离体记录潜力。
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引用次数: 0
MXene Nanosheets-Decorated Paper as a Green Electronics Material for Biosensing 作为生物传感用绿色电子材料的 MXene 纳米片装饰纸
Q3 Chemistry Pub Date : 2023-11-09 DOI: 10.1021/acsmeasuresciau.3c00043
Shan-Chu Yu, Tzu-Yen Huang and Tzu-En Lin*, 

This research delves into the development and optimization of MXene nanosheet-based paper electrodes, emphasizing their adaptability in green electronics and diverse applications. Xuan paper, a cellulose-based material, was identified as an ideal substrate for its mechanical attributes and capacity to accommodate MXene, further yielding outstanding electrical conductivity. The MXene paper electrode demonstrated consistent performance under various conditions, showing its potential in the field of wearable electronics and medical devices. Notably, its impressive electrothermal capabilities and environmentally conscious decomposition mechanism make it a promising candidate for future green electronic applications. Overall, this study underscores the electrode’s harmonization of performance and environmental sustainability, paving the way for its integration into futuristic electronic solutions.

本研究深入探讨了基于 MXene 纳米片的纸电极的开发和优化,强调了其在绿色电子和各种应用中的适应性。宣纸是一种纤维素基材料,因其机械属性和容纳 MXene 的能力而被确定为理想的基底,并进一步产生了出色的导电性。MXene 纸电极在各种条件下均表现出稳定的性能,显示出其在可穿戴电子设备和医疗设备领域的潜力。值得注意的是,它令人印象深刻的电热能力和环保型分解机制使其成为未来绿色电子应用的理想候选材料。总之,这项研究强调了这种电极在性能和环境可持续性方面的协调性,为其融入未来的电子解决方案铺平了道路。
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引用次数: 0
Electrochemical Visualization of Single-Molecule Thiol Substitution with Nanopore Measurement 通过纳米孔测量实现单分子硫醇置换的电化学可视化
Q3 Chemistry Pub Date : 2023-11-09 DOI: 10.1021/acsmeasuresciau.3c00046
Chao-Nan Yang, Wei Liu, Hao-Tian Liu, Ji-Chang Zhang, Ru-Jia Yu, Yi-Lun Ying* and Yi-Tao Long, 

Reactions involving sulfhydryl groups play a critical role in maintaining the structure and function of proteins. However, traditional mechanistic studies have mainly focused on reaction rates and the efficiency in bulk solutions. Herein, we have designed a cysteine-mutated nanopore as a biological protein nanoreactor for electrochemical visualization of the thiol substitute reaction. Statistical analysis of characteristic current signals shows that the apparent reaction rate at the single-molecule level in this confined nanoreactor reached 1400 times higher than that observed in bulk solution. This substantial acceleration of thiol substitution reactions within the nanopore offers promising opportunities for advancing the design and optimization of micro/nanoreactors. Moreover, our results could shed light on the understanding of sulfhydryl reactions and the thiol-involved signal transduction mechanisms in biological systems.

涉及巯基的反应在维持蛋白质的结构和功能方面起着至关重要的作用。然而,传统的机理研究主要关注的是反应速率和大量溶液中的效率。在此,我们设计了一种半胱氨酸突变纳米孔,作为生物蛋白质纳米反应器,用于硫醇替代反应的电化学可视化。对特征电流信号的统计分析表明,在这种封闭的纳米反应器中,单分子水平的表观反应速率比在大体积溶液中观察到的速率高出 1400 倍。硫醇置换反应在纳米孔内的这种大幅加速为推进微/纳米反应器的设计和优化提供了大有可为的机会。此外,我们的研究结果还可以帮助人们了解生物系统中的巯基反应以及巯基参与的信号转导机制。
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引用次数: 0
Abiotic, Hybrid, and Biological Electrocatalytic Materials Applied in Microfluidic Fuel Cells: A Comprehensive Review 应用于微流控燃料电池的非生物、混合和生物电催化材料:全面综述
Q3 Chemistry Pub Date : 2023-11-06 DOI: 10.1021/acsmeasuresciau.3c00044
D. V. Estrada-Osorio, Ricardo A. Escalona-Villalpando, M. P. Gurrola, Ricardo Chaparro-Sánchez, J. A. Rodríguez-Morales, L. G. Arriaga and J. Ledesma-García*, 

This article provides an overview of the work reported in the past decade in the field of microfluidic fuel cells. To develop appropriate research, the most commonly used electrocatalytic materials were considered and a new classification was proposed based on their nature: abiotic, hybrid, or biological. This classification allowed the authors to discern the information collected. In this sense, the types of electrocatalysts used for the oxidation of the most common fuels in different environments, such as glucose, ethanol, methanol, glycerol, and lactate, were presented. There are several phenomena presented in this article. This information gives an overview of where research is heading in the field of materials for electrocatalysis, regardless of the fuel used in the microfluidic fuel cell: the synthesis of abiotic and biological materials to obtain hybrid materials that allow the use of the best properties of each material.

本文概述了过去十年中微流体燃料电池领域的研究成果。为了开展适当的研究,作者考虑了最常用的电催化材料,并根据其性质提出了新的分类方法:非生物、混合或生物。通过这种分类,作者可以对收集到的信息进行鉴别。从这个意义上说,作者介绍了在不同环境中用于氧化葡萄糖、乙醇、甲醇、甘油和乳酸盐等最常见燃料的电催化剂类型。本文介绍了几种现象。这些信息概述了电催化材料领域的研究方向,无论微流体燃料电池使用何种燃料:合成非生物和生物材料,以获得混合材料,从而利用每种材料的最佳特性。
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引用次数: 0
Nanosensor Chemical Cytometry: Advances and Opportunities in Cellular Therapy and Precision Medicine 纳米传感器化学细胞测量法:细胞疗法和精准医学的进步与机遇
Q3 Chemistry Pub Date : 2023-11-01 DOI: 10.1021/acsmeasuresciau.3c00038
Youngho Song, Changyu Tian, Yullim Lee, Minyeong Yoon, Sang Eun Yoon and Soo-Yeon Cho*, 

With the definition of therapeutics now encompassing transplanted or engineered cells and their molecular products, there is a growing scientific necessity for analytics to understand this new category of drugs. This Perspective highlights the recent development of new measurement science on label-free single cell analysis, nanosensor chemical cytometry (NCC), and their potential for cellular therapeutics and precision medicine. NCC is based on microfluidics integrated with fluorescent nanosensor arrays utilizing the optical lensing effect of a single cell to real-time extract molecular properties and correlate them with physical attributes of single cells. This new class of cytometry can quantify the heterogeneity of the multivariate physicochemical attributes of the cell populations in a completely label-free and nondestructive way and, thus, suggest the vein-to-vein conditions for the safe therapeutic applications. After the introduction of the NCC technology, we suggest the technological development roadmap for the maturation of the new field: from the sensor/chip design perspective to the system/software development level based on hardware automation and deep learning data analytics. The advancement of this new single cell sensing technology is anticipated to aid rich and multivariate single cell data setting and support safe and reliable cellular therapeutics. This new measurement science can lead to data-driven personalized precision medicine.

随着治疗学的定义已涵盖移植或工程细胞及其分子产物,科学界越来越需要通过分析来了解这一新的药物类别。本视角重点介绍无标记单细胞分析、纳米传感器化学细胞仪(NCC)等新型测量科学的最新发展及其在细胞疗法和精准医疗方面的潜力。NCC 基于集成了荧光纳米传感器阵列的微流体技术,利用单细胞的光学透镜效应实时提取分子特性,并将其与单细胞的物理属性相关联。这种新型细胞测量技术可以完全无标记和无损的方式量化细胞群的多元物理化学属性的异质性,从而为安全的治疗应用提供静脉到静脉条件的建议。在介绍了 NCC 技术之后,我们为新领域的成熟提出了技术发展路线图:从传感器/芯片设计角度到基于硬件自动化和深度学习数据分析的系统/软件开发层面。预计这种新型单细胞传感技术的进步将有助于丰富的多变量单细胞数据设置,并为安全可靠的细胞疗法提供支持。这一新的测量科学可实现数据驱动的个性化精准医疗。
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引用次数: 0
Aiming for Maximized and Reproducible Enhancements in the Obstacle Race of SERS 在 SERS 的障碍赛中追求最大化和可重复的增强效果
Q3 Chemistry Pub Date : 2023-10-31 DOI: 10.1021/acsmeasuresciau.3c00037
Priyanka Dey*, 

Surface enhanced Raman scattering (SERS), since its discovery in the mid-1970s, has taken on many roles in the world of analytical measurement science. From identifying known and unknown chemicals in mixtures such as pharmaceutical and environmental samples to enabling qualitative and quantitative analysis of biomolecules and biomedical disease markers (or biomarkers), furthermore expanding to tracking nanostructures in vivo for medical diagnosis and therapy. This is because SERS combines the inherent power of Raman scattering capable of molecular species identification, topped with tremendous amplification in the Raman signal intensity when the molecule of interest is positioned near plasmonic nanostructures. The higher the SERS signal amplification, the lower the limit of detection (LOD) that could be achieved for the above applications. Therefore, improving SERS sensing efficiencies is vital. The signal reproducibility and SERS enhancement factor (EF) heavily rely on plasmonic nanostructure design, which has led to tremendous work in the field. But SERS signal and EF reproducibility remain key limitations for its wider market usability. This Review will scrutinize factors, some recognized and some often overlooked, that dictate the SERS signal and are of utmost importance to enable reproducible SERS EFs. Most of the factors pertain to colloidal labeled SERS. Some critically reviewed factors include the nanostructure’s surface area as a limiting factor, SERS hot-spots including optimizing the SERS EF within the hot-spot volume and positioning labels, properties of label molecules governing molecule orientation in hot-spots, and resonance effects. A better understanding of these factors will enable improved optimization and control of the experimental SERS, enabling extremely sensitive LODs without overestimating the SERS EFs. These are crucial steps toward identification and reproducible quantification in SERS sensing.

自 20 世纪 70 年代中期发现表面增强拉曼散射(SERS)以来,它在分析测量科学领域发挥了许多作用。从识别医药和环境样品等混合物中的已知和未知化学物质,到对生物大分子和生物医学疾病标志物(或生物标记物)进行定性和定量分析,再到追踪体内纳米结构以进行医学诊断和治疗。这是因为 SERS 结合了拉曼散射固有的分子物种识别能力,当感兴趣的分子靠近等离子纳米结构时,拉曼信号强度会被极大放大。SERS 信号放大率越高,上述应用所能达到的检测限(LOD)就越低。因此,提高 SERS 传感效率至关重要。信号重现性和 SERS 增强因子(EF)在很大程度上依赖于等离子纳米结构的设计,这也导致了该领域的大量研究工作。但是,SERS 信号和 EF 可重复性仍然是其广泛市场应用的关键限制因素。本综述将仔细研究决定 SERS 信号的因素,其中有些是公认的,有些则经常被忽视,而这些因素对于实现 SERS EF 的可重复性至关重要。大多数因素都与胶体标记 SERS 有关。一些重要因素包括作为限制因素的纳米结构表面积、SERS 热点(包括优化热点体积内的 SERS EF 和定位标签)、标签分子在热点中的取向特性以及共振效应。更好地了解这些因素将有助于改进对 SERS 实验的优化和控制,从而在不高估 SERS EF 的情况下实现极其灵敏的 LOD。这些都是在 SERS 传感中实现识别和可重复量化的关键步骤。
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引用次数: 0
Advances in Bioelectrode Design for Developing Electrochemical Biosensors 开发电化学生物传感器的生物电极设计进展
Q3 Chemistry Pub Date : 2023-10-27 DOI: 10.1021/acsmeasuresciau.3c00034
Nabajyoti Kalita, Sudarshan Gogoi, Shelley D. Minteer* and Pranab Goswami*, 

The critical performance factors such as selectivity, sensitivity, operational and storage stability, and response time of electrochemical biosensors are governed mainly by the function of their key component, the bioelectrode. Suitable design and fabrication strategies of the bioelectrode interface are essential for realizing the requisite performance of the biosensors for their practical utility. A multifaceted attempt to achieve this goal is visible from the vast literature exploring effective strategies for preparing, immobilizing, and stabilizing biorecognition elements on the electrode surface and efficient transduction of biochemical signals into electrical ones (i.e., current, voltage, and impedance) through the bioelectrode interface with the aid of advanced materials and techniques. The commercial success of biosensors in modern society is also increasingly influenced by their size (and hence portability), multiplexing capability, and coupling in the interface of the wireless communication technology, which facilitates quick data transfer and linked decision-making processes in real-time in different areas such as healthcare, agriculture, food, and environmental applications. Therefore, fabrication of the bioelectrode involves careful selection and control of several parameters, including biorecognition elements, electrode materials, shape and size of the electrode, detection principles, and various fabrication strategies, including microscale and printing technologies. This review discusses recent trends in bioelectrode designs and fabrications for developing electrochemical biosensors. The discussions have been delineated into the types of biorecognition elements and their immobilization strategies, signal transduction approaches, commonly used advanced materials for electrode fabrication and techniques for fabricating the bioelectrodes, and device integration with modern electronic communication technology for developing electrochemical biosensors of commercial interest.

电化学生物传感器的选择性、灵敏度、操作和存储稳定性以及响应时间等关键性能因素主要受其关键部件生物电极功能的影响。生物电极界面的适当设计和制造策略对于实现生物传感器的必要性能和实际用途至关重要。为实现这一目标,人们进行了多方面的尝试,从大量文献中可以看出,这些文献探讨了在电极表面制备、固定和稳定生物识别元件的有效策略,并借助先进的材料和技术,通过生物电极界面将生化信号有效地转化为电信号(即电流、电压和阻抗)。生物传感器在现代社会中的商业成功也日益受到其尺寸(因此便携性)、多路复用能力和无线通信技术接口耦合的影响,无线通信技术有利于在医疗保健、农业、食品和环境应用等不同领域快速传输数据和实时联动决策过程。因此,生物电极的制造涉及对多个参数的精心选择和控制,包括生物识别元件、电极材料、电极形状和尺寸、检测原理以及各种制造策略,包括微尺度和打印技术。本综述讨论了用于开发电化学生物传感器的生物电极设计和制造的最新趋势。讨论内容包括生物识别元件的类型及其固定策略、信号转导方法、电极制造常用的先进材料和生物电极制造技术,以及为开发具有商业价值的电化学生物传感器而将设备与现代电子通信技术相结合。
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引用次数: 0
Analyzer-to-Analyzer Variations in Assaying Ultralow Concentrated Biomarkers Associated with Neurodegenerative Diseases Using Immunomagnetic Reduction 利用免疫磁性还原法检测与神经退行性疾病相关的超低浓度生物标记物时分析仪之间的差异
Q3 Chemistry Pub Date : 2023-10-23 DOI: 10.1021/acsmeasuresciau.3c00029
Kun-Hung Lee, Ming-Hung Hsu, Hsin-Hsien Chen and Shieh-Yueh Yang*, 

By utilizing a high-temperature superconducting quantum interference device (high-Tc SQUID) magnetometer, an alternating current (AC) magnetosusceptometer, referred to as an analyzer, was developed for ultrasensitive immunoassays. The analyzer has been applied to assay biomarkers in human plasma associated with Alzheimer’s disease (AD) and Parkinson’s disease (PD). The involved assay methodology is the so-called immunomagnetic reduction (IMR). Such an analyzer has been approved for clinical use in Taiwan and Europe. The mass production of the analyzer is needed for clinical utilities. The issue of exploring analyzer-to-analyzer variations in the performances becomes critical. Unfortunately, there is no standard characterization to determine the variations in performances among analyzers. In this study, key characterizations, such as output signal stability, signal-to-noise ratio, measured concentrations of a control sample, etc., are proposed. In total, three analyzers are characterized in this work. The detected biomarkers include amyloid peptides, total tau protein, phosphorylated tau protein, and α-synuclein protein for AD and PD. Through one-way ANOVA for any of the characterizations among the three analyzers, it was found that there was no significant difference in any of these characterizations among the analyzers (p > 0.05). Furthermore, the three analyzers are applied to assay biomolecules for AD and PD in reference samples. High correlations (r > 0.8) in measured concentrations of any of these biomarkers in reference samples were obtained among the three analyzers. The results demonstrate that the proposed characterizations are feasible for achieving consistent performance among high-Tc SQUID-based AC magnetosusceptometers for assaying biomolecules.

通过利用高温超导量子干涉装置(high-Tc SQUID)磁力计,开发出了一种用于超灵敏免疫测定的交流(AC)磁感测器,称为分析仪。该分析仪已被用于检测人体血浆中与阿尔茨海默病(AD)和帕金森病(PD)相关的生物标记物。其中涉及的检测方法是所谓的免疫磁还原法(IMR)。这种分析仪已在台湾和欧洲获准用于临床。临床应用需要大量生产这种分析仪。探索分析仪之间的性能差异成为关键问题。遗憾的是,目前还没有标准的表征方法来确定分析仪之间的性能差异。在本研究中,我们提出了一些关键特性,如输出信号稳定性、信噪比、对照样本的测量浓度等。本研究共对三种分析仪进行了表征。检测的生物标记物包括淀粉样肽、总tau蛋白、磷酸化tau蛋白和α-突触核蛋白(AD和PD)。通过对三种分析仪的任何特征进行单因素方差分析,发现分析仪之间的任何特征均无显著差异(p > 0.05)。此外,这三种分析仪还被用于检测参考样本中的AD和PD生物大分子。三台分析仪在参考样本中测得的这些生物标记物的浓度具有很高的相关性(r > 0.8)。结果表明,所提出的特征描述是可行的,可以使基于高锝 SQUID 的交流磁差计在检测生物大分子时获得一致的性能。
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引用次数: 0
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