Electrochemical analysis

电化学分析
  • 文章类型: Journal Article
    能够连续监测指示健康状况的生理参数的可穿戴感测平台的出现已经导致临床医学的范式转变。这种便携式的可访问性和适应性,不显眼的设备可以实现主动,基于实时生理见解的个性化护理。虽然可穿戴传感平台展示了持续监测生理参数的强大功能,器件制造通常需要专门的设施和技术专长,限制部署机会和创新潜力。最近出现的传感器制造的快速原型方法,如激光诱导石墨烯(LIG),提供了通过低成本规避这些障碍的途径,可扩展的制造。然而,激光加工的固有限制将基于LIG的柔性电子设备的空间分辨率限制为最小激光光斑尺寸。对于CO2激光器-通常报道的用于设备生产的激光器-这对应于〜120μm的特征尺寸。这里,我们展示了一个简单的,低成本模板掩模技术,以减少最小可分辨特征尺寸的LIG基于设备的120±20μm到45±3μm时,由CO2激光制造。器件性能的表征揭示了这种模版掩蔽的LIG(s-LIG)方法在电性能方面产生了伴随的改善,我们假设这是图案化LIG宏观结构变化的结果。我们通过生产包括温度和多电极电化学传感器的普通传感器来展示这种制造方法的性能。我们制造通常无法通过天然CO2激光加工实现的细线微阵列电极,展示了扩展设计能力的潜力。将具有和不具有模板的微阵列传感器与传统的宏LIG电极进行比较揭示了s-LIG传感器对于类似的电活性表面区域具有显著降低的电容。除了提高传感器性能,这种金属模板技术可以提高分辨率,从而扩展了在低资源环境下可扩展制造高性能可穿戴传感器的能力,而无需依赖传统的制造途径。
    The advent of wearable sensing platforms capable of continuously monitoring physiological parameters indicative of health status have resulted in a paradigm shift for clinical medicine. The accessibility and adaptability of such portable, unobtrusive devices enables proactive, personalized care based on real-time physiological insights. While wearable sensing platforms exhibit powerful capabilities for continuously monitoring physiological parameters, device fabrication often requires specialized facilities and technical expertise, restricting deployment opportunities and innovation potential. The recent emergence of rapid prototyping approaches to sensor fabrication, such as laser-induced graphene (LIG), provides a pathway for circumventing these barriers through low-cost, scalable fabrication. However, inherent limitations in laser processing restrict the spatial resolution of LIG-based flexible electronic devices to the minimum laser spot size. For a CO2 laser-a commonly reported laser for device production-this corresponds to a feature size of ∼120 μm. Here, we demonstrate a facile, low-cost stencil-masking technique to reduce the minimum resolvable feature size of a LIG-based device from 120 ± 20 μm to 45 ± 3 μm when fabricated by CO2 laser. Characterization of device performance reveals this stencil-masked LIG (s-LIG) method yields a concomitant improvement in electrical properties, which we hypothesize is the result of changes in macrostructure of the patterned LIG. We showcase the performance of this fabrication method via production of common sensors including temperature and multi-electrode electrochemical sensors. We fabricate fine-line microarray electrodes not typically achievable via native CO2 laser processing, demonstrating the potential of the expanded design capabilities. Comparing microarray sensors made with and without the stencil to traditional macro LIG electrodes reveals the s-LIG sensors have significantly reduced capacitance for similar electroactive surface areas. Beyond improving sensor performance, the increased resolution enabled by this metal stencil technique expands capabilities for scalable fabrication of high-performance wearable sensors in low-resource settings without reliance on traditional fabrication pathways.
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  • 文章类型: Journal Article
    植物雌激素是由植物产生的非甾体雌激素,可以与人体的雌激素受体位点结合,并用作维持激素平衡的替代品。它们主要被归类为类黄酮,酚酸,木脂素,二苯乙烯,和香豆素;有些是内酯的回环酸,是真菌毒素而不是天然的植物雌激素.植物雌激素具有许多有益的药用特性,使它们成为日常饮食的重要组成部分。电化学传感器是广泛用于分析各种药物的分析工具,化学品,污染物和食品。电化学传感器为高灵敏度和快速分析提供了广泛的平台。关于植物雌激素的生物学和药用特性的重要性,已经发表了一些评论。然而,这篇综述概述了自2019年以来,通过使用电化学传感器和生物传感器对所有类别的植物雌激素进行电化学测量所做的最新工作。
    Phytoestrogens are non-steroidal estrogens produced from plants that can bind with the human body\'s estrogenic receptor site and be used as a substitute for maintaining hormonal balance. They are mainly classified as flavonoids, phenolic acids, lignans, stilbenes, and coumestans; some are resocyclic acids of lactones, which are mycotoxins and not natural phytoestrogen. Phytoestrogens have many beneficial medicinal properties, making them an important part of the daily diet. Electrochemical sensors are widely used analytical tools for analysing various pharmaceuticals, chemicals, pollutants and food items. Electrochemical sensors provide an extensive platform for highly sensitive and rapid analysis. Several reviews have been published on the importance of the biological and medicinal properties of phytoestrogens. However, this review provides an overview of recent work performed through electrochemical measurements with electrochemical sensors and biosensors for all the classes of phytoestrogens done so far since 2019.
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  • 文章类型: Journal Article
    手性分子具有相似的物理化学性质,在生理活动和毒性方面是不同的,使他们的分化和识别变得非常重要。纳米酶,它们是具有固有酶样活性的纳米材料,由于其高成本效益,引起了人们的极大兴趣,增强稳定性,和简单的合成。然而,构建具有高活性和对映选择性的纳米酶仍然是一个重大挑战。本文简要介绍了手性纳米酶的合成方法,并系统总结了基于电化学方法和紫外-可见吸收光谱的手性分子对映选择性识别的最新研究进展。此外,讨论了开发对映选择性纳米酶的挑战和发展趋势。期望本综述为多功能手性纳米酶的设计提供新的思路,拓宽纳米酶的应用领域。
    Chiral molecules have similar physicochemical properties, which are different in terms of physiological activities and toxicities, rendering their differentiation and recognition highly significant. Nanozymes, which are nanomaterials with inherent enzyme-like activities, have garnered significant interest owing to their high cost-effectiveness, enhanced stability, and straightforward synthesis. However, constructing nanozymes with high activity and enantioselectivity remains a significant challenge. This review briefly introduces the synthesis methods of chiral nanozymes and systematically summarizes the latest research progress in enantioselective recognition of chiral molecules based on electrochemical methods and ultraviolet-visible absorption spectroscopy. Moreover, the challenges and development trends in developing enantioselective nanozymes are discussed. It is expected that this review will provide new ideas for the design of multifunctional chiral nanozymes and broaden the application field of nanozymes.
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  • 文章类型: Journal Article
    5-甲酰胞嘧啶(5fC)和5-羧基胞嘧啶(5caC)是DNA去甲基化过程中的关键中间体,对基因调控和疾病进展具有重要意义。在这项研究中,我们介绍了一种新型的电化学传感平台,专门设计用于DNA中5fC和5caC的灵敏和选择性检测。与特异性抗体偶联的蛋白A修饰的磁珠(ProtA-MBs)促进这些修饰的碱基的免疫识别和富集。信号放大是通过涉及N3-kethonaxl和鸟嘌呤之间的相互作用的几个化学反应来实现的,用于连接二苯并环辛炔(DBCO)-生物素的无铜点击化学,以及随后通过链霉亲和素缀合的辣根过氧化物酶(SA-HRP)的识别。测定的读出在一次性激光诱导石墨烯(LIG)电极上进行,在磁场中用珠子-抗体-DNA复合物修饰,并在使用氢醌(HQ)作为氧化还原介体和H2O2作为底物的系统中使用差分脉冲伏安法进行分析。这种免疫传感器显示出优异的灵敏度,在0.1-1000pM线性范围内,5fC的检测限为14.8fM,在0.5-5000pM线性范围内,5caC的检测限为87.4fM,并且即使在存在来自其他DNA修饰的干扰的情况下也保持高选择性。成功应用于从细胞提取物中定量基因组DNA中的5fC和5caC,回收率在97.7%至102.9%之间,强调了其临床诊断的潜力。N3-酮醛首次用于电化学传感器。这项工作不仅拓宽了检测DNA修饰的工具包,而且为即时检测(POCT)技术的发展提供了新的动力。
    5-formylcytosine (5 fC) and 5-carboxylcytosine (5caC) serve as key intermediates in DNA demethylation process with significant implications for gene regulation and disease progression. In this study, we introduce a novel electrochemical sensing platform specifically designed for the sensitive and selective detection of 5 fC and 5caC in DNA. Protein A-modified magnetic beads (ProtA-MBs) coupled with specific antibodies facilitate the immunorecognition and enrichment of these modified bases. Signal amplification is achieved through several chemical reactions involving the interaction between N3-kethonaxl and guanine, copper-free click chemistry for the attachment of dibenzocyclooctyne (DBCO)-Biotin, and the subsequent recognition by streptavidin-conjugated horseradish peroxidase (SA-HRP). The assay\'s readout is performed on a disposable laser-induced graphene (LIG) electrode, modified with the bead-antibody-DNA complex in a magnetic field, and analyzed using differential pulse voltammetry in a system employing hydroquinone (HQ) as the redox mediator and H2O2 as the substrate. This immunosensor displayed excellent sensitivity, with detection limits of 14.8 fM for 5 fC across a 0.1-1000 pM linear range and 87.4 fM for 5caC across a 0.5-5000 pM linear range, and maintained high selectivity even in the presence of interferences from other DNA modifications. Successful application in quantifying 5 fC and 5caC in genomic DNA from cell extracts, with recovery rates between 97.7% to 102.9%, underscores its potential for clinical diagnostics. N3-kethoxal was used for the first time in an electrochemical sensor. This work not only broadens the toolkit for detecting DNA modifications but also provides a fresh impetus for the development of point-of-care testing (POCT) technologies.
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  • 文章类型: Journal Article
    低碳钢在酸性环境中的劣化在各种行业中提出了重大挑战。有效腐蚀抑制剂的出现引起了人们对旨在减少腐蚀有害后果的研究的关注。在这项研究中,首次通过各种电化学和重量分析技术研究了Prinivil在1MHCl溶液中的腐蚀抑制效率。结果表明,Prinivil的抑制效率从50ppm时的61.37%扩展到298K时500ppm浓度时的97.35%。在500ppm的抑制剂浓度下,回归系数(R2)为0.987,Kads值为0.935,Ea值为43.024kJ/mol,已发现Prinivil对金属表面的吸附具有很强的亲和力。扫描电子显微镜(SEM)和接触角测量分析进一步支持Prinivil的抑制行为,证明了在低碳钢表面产生了防御层。此外,采用分子动力学(MD)和蒙特卡罗模拟研究了原子水平上Prinivil与金属表面(Fe(110))之间的稳定性和相互作用。计算结果表明,Prinivil在钢表面具有很强的吸附作用,确认其作为腐蚀抑制剂的可行性。
    The deterioration of mild steel in an acidic environment poses a significant challenge in various industries. The emergence of effective corrosion inhibitors has drawn attention to studies aimed at reducing the harmful consequences of corrosion. In this study, the corrosion inhibition efficiency of Prinivil in a 1M HCl solution through various electrochemical and gravimetric techniques has been investigated for the first time. The results demonstrated that the inhibition efficiency of Prinivil expanded from 61.37% at 50 ppm to 97.35% at 500 ppm concentration at 298 K. With a regression coefficient (R 2) of 0.987, Kads value of 0.935 and Ea value of 43.024 kJ/mol at 500 ppm concentration of inhibitor, a strong affinity of Prinivil for adsorption onto the metal surface has been significantly found. Scanning electron microscopy (SEM) and contact angle measurement analyses further support the inhibitory behavior of Prinivil, demonstrating the production of a defensive layer on the surface of mild steel. Additionally, molecular dynamics (MD) and Monte Carlo simulations were employed to investigate the stability and interactions between Prinivil and the metallic surface (Fe (1 1 0)) at the atomic level. The computed results reveal strong adsorption of Prinivil upon the steel surface, confirming its viability as a corrosion inhibitor.
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  • 文章类型: Journal Article
    5-乙酰巴比妥酸与4-二甲基硫代氨基脲或4-六亚甲基亚氨基硫代氨基脲之间的反应产生5-乙酰巴比妥-4-二甲基硫代氨基脲(H2AcbDM)和5-乙酰巴比妥-4N-六亚甲基亚氨基硫代氨基脲(H2Acbexim)。已制备了八种具有不同铜(II)盐的新配合物,并使用元素分析对其进行了表征。摩尔电导,UV-Vis,ESI-HRMS,FT-IR,磁矩,EPR,和循环伏安法。此外,[Cu(HAcbDM)(H2O)2](NO3)·H2O(3a)的三维分子结构,[Cu(HAcbDM)(H2O)2]ClO4(4),和[Cu(HAcbHexim)Cl](6)通过单晶X射线晶体学测定,并对它们的超分子结构进行了分析。使用DFT计算和MEP表面和QTAIM分析进一步研究了H键合组件。在这些复合物中,缩氨基硫脲以ONS三齿方式与金属离子配位,呈O-烯醇/S-硫酮形式。已使用DMFA中的循环伏安技术在室温下研究了氨基硫脲及其铜(II)配合物的电化学行为。发现Cu(II)/Cu(I)氧化还原系统与准可逆扩散控制过程一致。
    The reaction between 5-acetylbarbituric acid and 4-dimethylthiosemicarbazide or 4-hexamethyleneiminyl thiosemicarbazide produces 5-acetylbarbituric-4-dimethylthiosemicarbazone (H2AcbDM) and 5-acetylbarbituric-4N-hexamethyleneiminyl thiosemicarbazone (H2Acbhexim). Eight new complexes with different copper(II) salts have been prepared and characterized using elemental analysis, molar conductance, UV-Vis, ESI-HRMS, FT-IR, magnetic moment, EPR, and cyclic voltammetry. In addition, three-dimensional molecular structures of [Cu(HAcbDM)(H2O)2](NO3)·H2O (3a), [Cu(HAcbDM)(H2O)2]ClO4 (4), and [Cu(HAcbHexim)Cl] (6) were determined by single crystal X-ray crystallography, and an analysis of their supramolecular structure was carried out. The H-bonded assemblies were further studied energetically using DFT calculations and MEP surface and QTAIM analyses. In these complexes, the thiosemicarbazone coordinates to the metal ion in an ONS-tridentate manner, in the O-enolate/S-thione form. The electrochemical behavior of the thiosemicarbazones and their copper(II) complexes has been investigated at room temperature using the cyclic voltammetry technique in DMFA. The Cu(II)/Cu(I) redox system was found to be consistent with the quasi-reversible diffusion-controlled process.
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  • 文章类型: Journal Article
    神经电极最近已经开发出导电聚合物的表面改性,特别是聚(3,4-亚乙基二氧噻吩)(PEDOT),并广泛研究了它们在记录和刺激中的作用,旨在提高其生物相容性。在这项工作中,阐明了实际神经传感器设计的含义,并报告了准备的系统程序。特别是,这项研究介绍了使用体外双电极实验来模拟神经电极的反应,重点是用PEDOT修饰的信号记录电极。具体来说,阵列中一个未修饰电极上的电势阶跃用于识别掺杂有不同阴离子的PEDOT的响应,并与裸铂(Pt)电极进行比较。响应显示与电势阶跃引起的检测器电极附近溶液中离子的重排有关,在检测器电极处看到电流瞬变。掺杂有氯化物的PEDOT的快速反应(约观察到0.04s)离子,这归因于氯离子进出聚合物膜的快速运动。相比之下,掺杂有聚(苯乙烯磺酸盐)(PSS)的PEDOT响应慢得多(约2.2s),聚阴离子的本质固定性限制了电流的流动方向。
    Neural electrodes have recently been developed with surface modifications of conductive polymers, in particular poly(3,4-ethylenedioxythiophene) (PEDOT), and extensively studied for their roles in recording and stimulation, aiming to improve their biocompatibility. In this work, the implications for the design of practical neural sensors are clarified, and systematic procedures for their preparation are reported. In particular, this study introduces the use of in vitro double electrode experiments to mimic the responses of neural electrodes with a focus on signal-recording electrodes modified with PEDOT. Specifically, potential steps on one unmodified electrode in an array are used to identify the responses for PEDOT doped with different anions and compared with that of a bare platinum (Pt) electrode. The response is shown to be related to the rearrangement of ions in solution near the detector electrode resulting from the potential step, with a current transient seen at the detector electrode. A rapid response for PEDOT doped with chloride (ca. 0.04 s) ions was observed and attributed to the fast movement of chloride ions in and out of the polymer film. In contrast, PEDOT doped with poly(styrenesulfonate) (PSS) responds much slower (ca. 2.2 s), and the essential immobility of polyanion constrains the direction of current flow.
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  • 文章类型: Journal Article
    新烟碱,作为增长最快的一类杀虫剂,目前占全球农药市场的25%以上。它们在控制对农田构成威胁的各种害虫方面的有效性,家庭院子/花园,不能否认高尔夫球场果岭。然而,新烟碱的广泛使用导致传粉者等非靶标生物的显着下降,昆虫,和鸟。此外,潜在的慢性,这些化合物对人体健康的亚致死效应在很大程度上仍是未知的。为了解决这些紧迫的问题,探索和了解电化学传感器在检测新烟碱残留方面的能力至关重要。令人惊讶的是,尽管这个话题越来越重要,目前文献中没有全面的评论文章。因此,我们提出的综述旨在通过全面分析使用电化学方法测定新烟碱来弥补这一差距.在这篇评论文章中,我们将深入研究电化学分析的各个方面,包括电极材料的影响,采用的技术,和使用不同类型的电极机构。通过综合和分析该领域的现有研究,我们的审查将为研究人员提供有价值的见解和指导,科学家,和政策制定者一样。
    Neonicotinoids, as the fastest-growing class of insecticides, currently account for over 25% of the global pesticide market. Their effectiveness in controlling a wide range of pests that pose a threat to croplands, home yards/gardens, and golf course greens cannot be denied. However, the extensive use of neonicotinoids has resulted in significant declines in nontarget organisms such as pollinators, insects, and birds. Furthermore, the potential chronic, sublethal effects of these compounds on human health remain largely unknown. To address these pressing issues, it is crucial to explore and understand the capabilities of electrochemical sensors in detecting neonicotinoid residues. Surprisingly, despite the increasing importance of this topic, no comprehensive review article currently exists in the literature. Therefore, our proposed review aims to bridge this gap by providing a thorough analysis of the use of electrochemical methods for neonicotinoid determination. In this review article, we will delve into various aspects of electrochemical analysis, including the influence of electrode materials, employed techniques, and the different types of electrode mechanisms utilized. By synthesizing and analysing the existing research in this field, our review will offer valuable insights and guidance to researchers, scientists, and policymakers alike.
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  • 文章类型: Journal Article
    电原分解有机物,并通过胞外电子转移将储存的化学能转化为电能。它们是微生物燃料电池的重要生物催化剂,在绿色能源生产中具有实际应用,污水处理,和生物修复。从生物技术工厂的污泥中分离出兼性厌氧电菌株SQ-1。菌株SQ-1是花色克雷伯菌的近亲。在将分离的细菌接种到微生物燃料电池装置中之后,在碳电极的表面上形成多层生物膜。通过在三电极配置中使用乙酸盐作为碳源,该应变产生了625μAcm-2的高电流密度。还在双室微生物燃料电池中分析了发电性能。当相应的输出电压为0.59V时,它达到560mWm-2的最大功率密度。兼性菌株SQ-1利用水合氧化铁作为电子受体在厌氧条件下进行细胞外电生呼吸。由于兼性菌株比厌氧菌株具有更好的性能,克雷伯菌属。SQ-1可能是在微生物电化学中应用的有前途的外电菌株。
    Electricigens decompose organic matter and convert stored chemical energy into electrical energy through extracellular electron transfer. They are significant biocatalysts for microbial fuel cells with practical applications in green energy generation, effluent treatment, and bioremediation. A facultative anaerobic electrogenic strain SQ-1 is isolated from sludge in a biotechnology factory. The strain SQ-1 is a close relative of Klebsiella variicola. Multilayered biofilms form on the surface of a carbon electrode after the isolated bacteria are inoculated into a microbial fuel cell device. This strain produces high current densities of 625 μA cm-2 by using acetate as the carbon source in a three-electrode configuration. The electricity generation performance is also analyzed in a dual-chamber microbial fuel cell. It reaches a maximum power density of 560 mW m-2 when the corresponding output voltage is 0.59 V. The facultative strain SQ-1 utilizes hydrous ferric oxide as an electron acceptor to perform extracellular electricigenic respiration in anaerobic conditions. Since facultative strains possess better properties than anaerobic strains, Klebsiella sp. SQ-1 may be a promising exoelectrogenic strain for applications in microbial electrochemistry.
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  • 文章类型: Journal Article
    汞离子会对生态环境造成严重破坏,有必要开发可靠和优雅的汞离子传感器。在这个协议中,基于分层的Ti3C2MXene纳米片(DL-Ti3C2MXene),提出了Hg2的无标记光热/电化学双模式策略。Hg2+以HgCl2、Hg(OH)2和HgClOH的形式存在于水中,富电子元素O和Cl可以在边缘与带正电荷的DL-Ti3C2MXene特异性结合,并发生进一步的氧化-还原反应以获得TiO2/C和Hg2Cl2。鉴于DL-Ti3C2MXene本身的还原活性和光热转化性能,电化学和光热响应随Hg2+浓度对数的增加而降低。相应的线性范围为50pmolL-1-500nmolL-1和1nmolL-1-50μmolL-1,在3S/N下计算的检出限分别为17.2pmolL-1和0.43nmolL-1。DL-Ti3C2MXene具有原料范围广的特点,低成本,和容易准备。此外,该设计充分利用了材料本身的特性,避免了传统传感器复杂的装配和检测过程,并使高选择性和灵敏度的汞检测。特别是,双模式传感赋予了汞离子检测结果的自我确认,从而提高了传感器的可靠性。
    Mercury ions can cause serious damage to the ecological environment, and it is necessary to develop reliable and elegant mercury ion sensors. In this protocol, a label-free photothermal/electrochemical dual-mode strategy for Hg2+ is proposed based on delaminated Ti3C2 MXene nanosheets (DL-Ti3C2 MXene). Hg2+ exists in water in the form of HgCl2, Hg(OH)2, and HgClOH, and the electron-rich elements O and Cl can specifically bind to the positively charged DL-Ti3C2 MXene at the edge, and further oxidation-reduction reaction occurs to obtain TiO2/C and Hg2Cl2. In view of the reduction activity and the performance of photothermal conversion of DL-Ti3C2 MXene itself, the electrochemical and photothermal responses decrease with the increase of the logarithm of Hg2+ concentration. The corresponding linear ranges are 50 pmol L-1-500 nmol L-1 and 1 nmol L-1-50 μmol L-1, and their detection limits calculated at 3 S/N are 17.2 pmol L-1 and 0.43 nmol L-1, respectively. DL-Ti3C2 MXene has the characteristics of a wide range of raw materials, low cost, and easy preparation. In addition, the design takes full advantage of the properties of the material itself, avoids the complex assembly and detection process of conventional sensors, and enables high selectivity and sensitivity for mercury detection. In particular, the dual-mode sensing endows self-confirmation of mercury ion detection results, thereby improving the reliability of the sensor.
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