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Direct writing of graphene electrodes for point-of-care electrochemical sensing applications 直接写入石墨烯电极用于护理点电化学传感应用
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-31 DOI: 10.1039/D4SD00140K
Lei Zhao, Andrew Piper, Giulio Rosati and Arben Merkoçi

Electrochemical sensors are increasingly garnering attention as valuable tools for point-of-care (POC) testing due to their low costs, high sensitivities, and ease of miniaturization. Graphene-based materials, renowned for their tunable electrical conductivity, high specific surface areas, versatile functionality, and biocompatibility; are highly suited for the fabrication of electrochemical sensors with heightened sensitivities. Non-contact, maskless, direct writing methods allow the rapid, large-scale production of graphene electrodes with high design flexibility. Researchers globally are advancing graphene electrode production, aiming for smaller, faster, and more efficient sensors. This review provides a comprehensive overview of recent advances on the direct writing of graphene electrodes for electrochemical sensing applications. It covers the basics of direct writing techniques, the advancements in graphene ink/precursor preparation, structural design, and device integration, with a focus on POC platforms.

电化学传感器因其低成本、高灵敏度和易于微型化等特点,正日益受到人们的关注,成为进行床旁(POC)检测的重要工具。石墨烯基材料以其可调导电性、高比表面积、多功能性和生物兼容性而闻名,非常适合制造灵敏度更高的电化学传感器。通过非接触、无掩模、直接写入的方法,可以快速、大规模地生产具有高度设计灵活性的石墨烯电极。全球的研究人员正在推进石墨烯电极的生产,目标是制造出更小、更快、更高效的传感器。本综述全面概述了直接写入石墨烯电极用于电化学传感应用的最新进展。它涵盖了直接写入技术的基础知识、石墨烯墨水/前驱体制备的进展、结构设计和器件集成,重点关注 POC 平台。
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引用次数: 0
Synthesis and characterization of La QDs: sensors for anions and H2O2† La QDs 的合成与表征:阴离子和 H2O2 传感器
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-26 DOI: 10.1039/D4SD00142G
Amit Sahoo and Achyuta N. Acharya

The development of sensitive and accurate fluorescence sensors for the detection of anions and reactive oxygen species (ROS, H2O2) is essential as they play significant roles in biological and chemical processes. In this work, semiconductor La QDs were synthesized. The synthesized La QDs were determined to be pure with 100% La element using EDS technique. La QDs were observed in both cubic and hexagonal lattice configurations through powder XRD analysis. The morphology of the La QDs was characterized using HRTEM and FESEM data as tiny, spherical, homogenous QDs with a diameter ranging from 2 to 6 nm. The fluorescence characteristics of the synthesized La QDs were examined by studying their sensing properties that increased with an increase in anion concentration and decreased with an increase in [H2O2]. The variation in emission intensity at 315 nm and 440.5 nm satisfied the Stern–Volmer equation. The LOD and LOQ of H2O2 and anion sensing with La QDs were studied in the μM range. The Langmuir binding plots and FTIR spectra supported the concept that the surface functionalization of La QDs occurred in the presence of anions. With two band gap energies of about 3.26 eV and 4.66 eV, the synthesized La QDs are a mixture of two (binary) semiconductors.

由于阴离子和活性氧(ROS、H2O2)在生物和化学过程中发挥着重要作用,因此开发用于检测阴离子和活性氧的灵敏而准确的荧光传感器至关重要。本研究合成了半导体 La QDs。利用 EDS 技术确定合成的 La QDs 纯度为 100%。通过粉末 XRD 分析,观察到 La QDs 具有立方和六方两种晶格构型。利用 HRTEM 和 FESEM 数据对 La QDs 的形态进行了表征,发现它们是微小、球形、均匀的 QDs,直径在 2 到 6 nm 之间。通过研究合成的 La QDs 的传感特性,考察了它们的荧光特性,即随着阴离子浓度的增加而增加,随着[H2O2]的增加而减少。在 315 nm 和 440.5 nm 处的发射强度变化符合 Stern-Volmer 方程。研究了 La QDs 在 μM 范围内传感 H2O2 和阴离子的 LOD 和 LOQ。朗缪尔结合图和傅立叶变换红外光谱支持了 La QDs 在阴离子存在时发生表面官能化的概念。合成的 La QDs 具有约 3.26 eV 和 4.66 eV 的两个带隙能,是两种(二元)半导体的混合物。
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引用次数: 0
Optimized gadolinium-DO3A loading in RAFT-polymerized copolymers for superior MR imaging of aging blood–brain barrier† 优化 RAFT 聚合共聚物中的钆-DOTA 负载,为老化血脑屏障提供优质磁共振成像
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-25 DOI: 10.1039/D4SD00063C
Hunter A. Miller, Aaron Priester, Evan T. Curtis, Krista Hilmas, Ashleigh Abbott, Forrest M. Kievit and Anthony J. Convertine

The development of gadolinium-based contrast agents (GBCAs) has been pivotal in advancing magnetic resonance imaging (MRI), offering enhanced soft tissue contrast without ionizing radiation exposure. Despite their widespread clinical use, the need for improved GBCAs has led to innovations in ligand chemistry and polymer science. We report a novel approach using methacrylate-functionalized DO3A ligands to synthesize a series of copolymers through direct reversible addition-fragmentation chain transfer (RAFT) polymerization. This technique enables precise control over the gadolinium content within the polymers, circumventing the need for subsequent conjugation and purification steps, and facilitates the addition of other components such as targeting ligands. The resulting copolymers were analysed for their relaxivity properties, indicating that specific gadolinium-DO3A loading contents between 12–30 mole percent yield optimal MRI contrast enhancement. Inductively coupled plasma (ICP) measurements corroborated these findings, revealing a non-linear relationship between gadolinium content and relaxivity. Optimized copolymers were synthesized with the claudin-1 targeting peptide, C1C2, to image BBB targeting in aged mice to show imaging utility. This study presents a promising pathway for the development of more efficient GBCA addition to copolymers for targeted drug delivery and bioimaging application.

钆基造影剂(GBCAs)的开发在推动磁共振成像(MRI)方面发挥了关键作用,它能在不暴露于电离辐射的情况下增强软组织造影效果。尽管钆基造影剂已广泛应用于临床,但对改进型钆基造影剂的需求促使配体化学和聚合物科学不断创新。我们报告了一种使用甲基丙烯酸酯功能化 DOTA 配体,通过直接可逆加成-碎片链转移(RAFT)聚合合成一系列共聚物的新方法。这种技术可以精确控制聚合物中的钆含量,省去了后续的共轭和纯化步骤,并有利于添加靶向配体等其他成分。对所得共聚物的弛豫特性进行了分析,结果表明,钆-DOTA 的具体装载量在 12-30 摩尔% 之间,能产生最佳的磁共振成像对比度增强效果。电感耦合等离子体 (ICP) 测量证实了这些发现,揭示了钆含量与弛豫性之间的非线性关系。优化后的共聚物与 claudin-1 靶向肽 C1C2 合成,在老龄小鼠的 BBB 靶向成像中显示出成像效用。这项研究为开发更高效的 GBCA 添加到共聚物中,用于靶向给药和生物成像应用提供了一条前景广阔的途径。
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引用次数: 0
Detection of surfactants using a hydrophobic natural deep eutectic solvent and smartphone† 使用疏水性天然深共晶溶剂和智能手机检测表面活性剂
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-24 DOI: 10.1039/D4SD00196F
Vagner Bezerra dos Santos, Lucas B. Ayres, Helayne Santos de Sousa, Carlos D. Garcia and Willian Toito Suarez

We report on the advantages of a green method to detect surfactants in environmental water samples. The approach is based on the use of a hydrophobic natural deep eutectic solvent (NADES) to extract the complexes formed by the surfactants and methylene blue. The concentration of the surfactant is then determined by measuring the color intensity in the organic phase using a smartphone. Under optimized conditions, an aliquot of 3 mL of the NADES was mixed with 15 mL of water, and then allowed to settle (to enable the separation of the two phases) for 5 min. The procedure allowed quantification of sodium dodecyl sulfate (SDS), as a proxy for alkyl surfactants in the range from 0.010 mg L−1 to 0.600 mg L−1, with a detection limit of 2.0 μg L−1. Besides being a simple alternative to the traditional method (which requires chloroform and a spectrophotometer), the proposed approach offers low waste generation, low power-consumption, and fast analysis time, and is fully compatible with the plastic supplies (e.g. cuvettes, pipettes, tips, etc.) typically used for on-site analysis. The applicability of the approach was demonstrated by measuring various surface water samples and the overall green score of the method was calculated to be 96%.

我们报告了一种检测环境水样中表面活性剂的绿色方法的优点。该方法基于使用疏水性天然深共晶溶剂(NADES)来提取表面活性剂与亚甲基蓝形成的复合物。然后使用智能手机测量有机相中的颜色强度,从而确定表面活性剂的浓度。在优化条件下,将等分的 100 µL NADES 与 15 mL 水混合,然后静置 5 分钟(使两相分离)。该方法可定量检测十二烷基硫酸钠(SDS),作为烷基表面活性剂的替代物,检测范围为 0.010 mg L-1 至 0.600 mg L-1,检测限为 2.0 µg.L-1。除了可以简单地替代传统方法(需要氯仿和分光光度计)外,该方法还具有废物产生少、耗电量低、分析时间快等优点,并且与现场分析通常使用的塑料用品(如比色皿、移液管、吸头等)完全兼容。通过测量各种地表水样本,证明了该方法的适用性,并计算出该方法的总体绿色得分率为 96%。
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引用次数: 0
Highly efficient WS2 QD-based non-enzymatic fluorescent biosensor for ofloxacin and ciprofloxacin monitoring in aquatic media† 基于 WS2QDs 的高效非酶促荧光生物传感器用于监测水生介质中的氧氟沙星和环丙沙星
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-24 DOI: 10.1039/D4SD00148F
Sunayana Bora and Chandan Upadhyay

Quantum dot-based biosensors have gained prominence in recent times for the detection of biological and chemical hazards present in aquatic media which essentially contribute to the degradation of the environment and human health. Within this work, we demonstrate a WS2 QD-induced turn-on fluorescent probe for specific monitoring of ofloxacin (OFL) and ciprofloxacin (CIP) residues in water. An efficient one-pot hydrothermal approach is applied for fluorescent water-soluble WS2 QD preparation. The WS2 QDs possess excellent photostability and monodispersity along with a superior shelf life. The WS2 QDs interacting with FQns (OFL and CIP) showed a systematically enhanced fluorescence in varying FQn concentrations from 0 μM to 3 μM. Also, all the measurements showed excellent results for sensitivity along with superior specificity as well as anti-interference ability over other interfering substances like various metal ions and antibiotic derivatives. The proposed sensor allows the quantification of FQns in the range of 0–3 μM with the lowest detectable amount (LOD) of 0.08 μM and 0.06 μM and the minimal limit of quantification (LOQ) of 0.26 μM and 0.21 μM for both OFL and CIP, respectively, at natural pH. It achieved higher sensitivity than many established techniques and materials making up the gap of other existing systems in this range. We observed excellent results for the rapid in situ detection of FQns by implementing WS2 QDs. The findings show potential for future use in real-time applications for FQns.

近来,基于量子点的生物传感器在检测水生介质中存在的生物和化学危害方面日益突出,这些危害从根本上导致了环境和人类健康的恶化。在这项工作中,我们展示了一种 WS2QDs 诱导的开启荧光探针,用于特异性监测水中的氧氟沙星(oflx)和环丙沙星(cprx)残留。该研究采用高效的一锅水热法制备了荧光水溶性 WS2QDs。WS2QDs 具有出色的光稳定性和单分散性,而且保存期极长。与 FQns(oflx 和 cprx)相互作用的 WS2QDs 在不同浓度(0μM 至 3μM)的 FQns 中显示出系统增强的荧光。此外,所有测量结果都显示出卓越的灵敏度、特异性和抗干扰能力,不受其他干扰物质(如各种金属离子和抗生素衍生物)的影响。在自然 pH 条件下,该传感器可对 0 μM-3 μM 范围内的 FQns 进行定量,最低检测量(LOD)分别为 0.12μM 和 2.02μM,最低定量限(LOQ)分别为 0.36μM 和 6.11μM。与许多已有的技术和材料相比,它实现了更高的灵敏度,弥补了其他现有系统在这一范围内的空白。通过使用 WS2QDs,我们观察到了快速原位检测 FQns 的出色结果。这些研究结果表明,它在未来的 FQns 实时应用中具有很大的潜力。
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引用次数: 0
A handheld laser-cut device for the size-controlled assembly and electrical characterisation of lipid bilayers† 用于控制脂质双分子层的尺寸和电学特性的手持式激光切割装置
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-24 DOI: 10.1039/D4SD00076E
Ji Huang, Yuval Elani and Mark S. Friddin

We report the rapid fabrication of a handheld laser cut platform that can support the assembly, functionalisation, size-control and electrical characterisation of lipid bilayers. We achieve this by building a modular DIY platform that can support the lowering of a Ag/AgCl electrode through a phase transfer column consisting of an upper oil phase containing lipids, and a lower aqueous phase containing buffer.

我们报告了手持激光切割平台的快速制造过程,该平台可支持脂质双层膜的组装、功能化、尺寸控制和电学表征。我们通过构建模块化 DIY 平台来实现这一目标,该平台可支持通过由含有脂质的上层油相和含有缓冲液的下层水相组成的相转移柱来降低银/氯化银电极。
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引用次数: 0
DNA walker coupled with nicking endonuclease for sensitive electrochemical detection of saxitoxin† 与核酸内切酶联用的 DNA 步行器用于灵敏的沙西毒素电化学检测
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-24 DOI: 10.1039/D4SD00167B
Yiwei Liu, Shumin Feng, Ruoxi Zhong, Yuanchang Peng, Guoyuan Mu, Jiayi Bai, Wei Chen and Zhan Qu

Saxitoxin (STX) as one of the paralytic shellfish toxins has become a serious public health and environmental issue. In this regards, developing highly sensitive and selective biosensors may help find a solution. Herein, a ferrocene (Fc)-labeled DNA walker coupled with nicking endonuclease Nb.BbvCI was used to construct a sensitive electrochemical aptasensor for STX detection. First, an amplified DNA, aptamer and DNA walker formed a sandwich structure on a gold electrode. This structure was disintegrated when STX was added, resulting in the hybridization of the amplified DNA and DNA walker. Thereafter, the DNA walker was activated by Nb.BbvCI to achieve stepwise cleavage of the hybridized amplified DNA. The released Fc-amplified DNA generated an electrochemical signal that decreased linearly with the logarithm value of STX concentration in the range of 1 pM–100 nM with a detection limit of 0.58 pM. Meanwhile, the proposed aptasensor exhibited good selectivity and recovery rate. The DNA walker coupled with the nicking endonuclease provides effective signal amplification for the detection of toxins and fabrication of sensitive aptasensors.

沙西毒素(STX)作为麻痹性贝类毒素之一,已成为一个严重的公共卫生和环境问题。为此,开发高灵敏度和高选择性的生物传感器可能有助于找到解决方案。在此,研究人员利用二茂铁(Fc)标记的DNA步行器与核酸内切酶Nb.BbvCI联用,构建了一种用于检测STX的灵敏电化学传感器。首先,扩增 DNA、适配体和 DNA 走行子在金电极上形成了一个三明治结构。当加入 STX 时,该结构被瓦解,从而导致扩增 DNA 和 DNA walker 杂交。之后,DNA walker 被 Nb.BbvCI 激活,从而逐步裂解杂交扩增的 DNA。释放的 Fc 扩增 DNA 产生的电化学信号在 1 pM-100 nM 范围内随 STX 浓度的对数值线性下降,检测限为 0.58 pM。同时,该传感器还具有良好的选择性和回收率。DNA 步行器与核酸内切酶的结合为检测毒素和制造灵敏的适配传感器提供了有效的信号放大。
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引用次数: 0
Stretchable and body-conformable physical sensors for emerging wearable technology 用于新兴可穿戴技术的可拉伸和人体适形物理传感器
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-24 DOI: 10.1039/D4SD00189C
Yong Lin, Weijie Qiu and Desheng Kong

Wearable physical sensors represent attractive devices for health monitoring and human–machine interfaces. Unlike traditional devices that prioritize increased sensitivity and selectivity, stretchability is crucial for wearable sensors to effectively adhere to the dynamic and curved contours of the human body. In addition to being stretchable, the conformal integration allows for durable skin–device interfaces, enabling long-term wearable detection. To track the latest progress, this perspective focuses on the rapidly advancing field of skin-attached physical sensors, analyzing their design approaches, critical applications, and desirable characteristics. The discussion begins with two primary strategies for creating stretchable electronic devices through structural designs and material innovations. We further discuss the significance of a conformal, seamless skin–device interface for wearable detection. We further elaborate on several critical physical sensors and their system integration. Finally, this article addresses current challenges and outlines future directions to translate knowledge in this evolving field into cutting-edge wearable technologies.

可穿戴物理传感器是健康监测和人机界面的理想设备。与优先考虑提高灵敏度和选择性的传统设备不同,可伸缩性对于可穿戴传感器有效贴合人体的动态和弯曲轮廓至关重要。除了可拉伸外,保形集成还可实现耐用的皮肤-设备接口,从而实现长期的可穿戴检测。为了跟踪最新进展,本视角将重点关注快速发展的皮肤附着物理传感器领域,分析其设计方法、关键应用和理想特性。讨论从通过结构设计和材料创新制造可拉伸电子设备的两种主要策略开始。我们进一步讨论了可穿戴式检测中皮肤与设备的保形和无缝接口的重要性。我们进一步阐述了几个关键的物理传感器及其系统集成。最后,本文探讨了当前面临的挑战,并概述了将这一不断发展的领域的知识转化为尖端可穿戴技术的未来方向。
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引用次数: 0
A nitroreductase-sensitive near-IR fluorescent biosensor for detecting tumor hypoxia in vivo† 用于检测体内肿瘤缺氧的对硝基还原酶敏感的近红外荧光生物传感器
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-23 DOI: 10.1039/D4SD00146J
Safiya Nisar and Binglin Sui

Tumor cells have high metabolic demands, leading to increased oxygen consumption and further exacerbating hypoxia, which has been regarded as a characteristic feature of solid tumors and plays a significant role in tumor growth, resistance to therapy, and overall treatment outcomes. Hypoxia-specific sensing probes are currently in urgent need to provide valuable information for tumor detection and monitoring. In this work, we developed a new near-IR fluorescence-emitting biosensor with a high fluorescence quantum yield for hypoxia detection in tumor tissues. In the presence of nitroreductase enzyme under tumor hypoxia, the nitro group of the biosensor molecule is converted into an amino group, and the resulting compound turns itself into a nonfluorescent dye through a self-immolating process, thus turning off the fluorescence emission of the biosensor. The fluorescence change of the biosensor in response to nitroreductase is sensitive and selective and is not influenced by the presence of other physiologically important species. In the in vitro and in vivo bioimaging experiments, the biosensor demonstrated high efficiency in detecting hypoxia and the capability of distinguishing solid tumors of different sizes, indicating its potential applications in tumor diagnosis and progression monitoring.

肿瘤细胞具有高代谢需求,导致耗氧量增加,进一步加剧了缺氧。缺氧一直被认为是实体瘤的一个特征,在肿瘤生长、抗药性和总体治疗效果方面起着重要作用。缺氧特异性传感探针目前急需为肿瘤检测和监测提供有价值的信息。在这项工作中,我们开发了一种具有高荧光量子产率的新型近红外荧光发射生物传感器,用于肿瘤组织中的缺氧检测。在肿瘤缺氧条件下,当硝基还原酶存在时,生物传感器分子中的硝基转化为氨基,由此产生的化合物通过自褪色过程变成无荧光染料,从而关闭了生物传感器的荧光发射。生物传感器对硝基还原酶的荧光变化具有灵敏性和选择性,不会受到其他重要生理物质的影响。在体外和体内生物成像实验中,该生物传感器在检测缺氧方面表现出很高的效率,并能区分不同大小的实体肿瘤,这表明它在肿瘤诊断和进展监测方面具有潜在的应用价值。
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引用次数: 0
Paper-based sensing of pancreatic-cancer biomarker α-chymotrypsin through turn-on lanthanide-luminescence† 基于纸张的胰腺癌生物标记物 α-Chymotrypsin 触发镧系元素发光传感技术
IF 3.5 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-18 DOI: 10.1039/D4SD00124A
Ananya Biswas and Uday Maitra

We report the facile detection of a pancreatic cancer biomarker α-chymotrypsin (Chy) by turn-on, time-gated lanthanide luminescence for the first time. To the best of our knowledge, the non-peptide probe we designed is the simplest one currently available. The probe undergoes Chy-induced release of the sensitizing antenna (2,3-dihydroxynaphthalene), leading to enhanced lanthanide luminescence. The detection protocol was further modified to develop a paper-based sensor and was used to detect Chy in commercial tablets, and to rapidly screen Chy-inhibitors.

我们首次报道了利用开启的时间门控镧系元素发光法检测胰腺癌生物标志物α-糜蛋白酶(Chy)的简便方法。据我们所知,我们设计的非肽探针是目前最简单的探针。该探针会在 Chy 诱导下释放敏化天线(2,3-二羟基萘),从而导致镧系元素发光增强。该检测方案经进一步修改后被用于开发纸基传感器,并被用于检测商业药片中的糜蛋白酶和快速筛选糜蛋白酶抑制剂。
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引用次数: 0
期刊
Sensors & diagnostics
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