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Integrated Electronic Tags based Vertical Flow Assay (e-VFA) with Micro-sieve and AlGaN/GaN HEMT sensors for Multi-target detection in Actual Saliva 基于电子标签的垂直流动分析仪 (e-VFA) 与微筛和 AlGaN/GaN HEMT 传感器的集成，用于实际唾液中的多目标检测

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-06 DOI: 10.1039/d4an00510d

Zhiqi Gu, Hui Chang, Guo Yang, Boxuan Xu, Bin Miao, Jiadong Li

Vertical flow assay (VFA) is an effective point-of-care (POC) diagnostic tool for widespread applications. Nevertheless, the lack of multi-target detection and multi-signal readout capability still remain challenges. Herein, a brand new VFA scheme for multi-target saliva detection based on electronic-tags was proposed, where AlGaN/GaN HEMT sensors modified with different bio-receptors as electronic tags endowed the VFA a multi-target detection capability. In addition, the use of electronic tags instead of optical tags made that the VFA could simultaneously carry out direct multi-target readout, which ensure the effective POC diagnostic of saliva analysis. Moreover, by integrating a hydrophilically optimized micro-sieve, impurities like sticky filaments, epidermal cells and other large-scale charged particles in saliva were effectively screened, which enabled the direct detection of saliva by AlGaN/GaN HEMT sensors. Glucose, urea, and cortisol were selected to verified the feasibility of the multi-target e-VFA scheme, results displayed that the limit-of-detection (LOD) was as low as 100 aM. The linear response was demonstrated in the dynamic range of 100 aM - 100 μM, the specificity and long-term stability and the validity of the actual saliva test were also verified. These results demonstrated that the as-proposed e-VFA had potential application in saliva detection for multi-target simultaneous detection, and it is expected to achieve the real-time detection of more biological targets in saliva.

垂直血流分析法（VFA）是一种有效的床旁诊断（POC）工具，应用广泛。然而，缺乏多目标检测和多信号读出能力仍然是一个挑战。本文提出了一种全新的基于电子标签的唾液多目标检测 VFA 方案，其中 AlGaN/GaN HEMT 传感器采用不同的生物受体作为电子标签，赋予了 VFA 多目标检测能力。此外，由于使用了电子标签而不是光学标签，因此 VFA 可以同时直接进行多目标读取，从而确保了唾液分析的有效 POC 诊断。此外，通过集成亲水性优化微筛，有效筛查了唾液中的粘丝、表皮细胞和其他大尺度带电粒子等杂质，实现了 AlGaN/GaN HEMT 传感器对唾液的直接检测。为了验证多目标 e-VFA 方案的可行性，选择了葡萄糖、尿素和皮质醇，结果显示检测限（LOD）低至 100 aM。在 100 aM - 100 μM 的动态范围内呈现线性响应，特异性和长期稳定性以及实际唾液检测的有效性也得到了验证。这些结果表明，拟议的电子唾液检测器具有在唾液检测中进行多目标同时检测的潜在应用价值，有望实现对唾液中更多生物目标的实时检测。

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引用次数: 0

Correction: Development of a novel X-ray fluorescence instrument equipped with a noble gas filter 更正：开发配备惰性气体过滤器的新型 X 射线荧光仪器。

IF 3.6 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-05 DOI: 10.1039/D4AN90046D

Tsugufumi Matsuyama, Tomoya Miyahara, Hiroshi Yoshii, Lee Wah Lim and Kouichi Tsuji

Correction for ‘Development of a novel X-ray fluorescence instrument equipped with a noble gas filter’ by Tsugufumi Matsuyama et al., Analyst, 2024, https://doi.org/10.1039/d4an00122b.

Tsugufumi Matsuyama 等人撰写的 "配备惰性气体过滤器的新型 X 射线荧光仪器的开发 "的更正，《分析家》，2024 年，https://doi.org/10.1039/d4an00122b。

引用次数: 0

Live chicken egg embryos as an alternative in vivo tumour model for deep surface enhanced Raman spectroscopy† 活鸡卵胚胎作为深层表面增强拉曼光谱的替代体内肿瘤模型

IF 3.6 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-04 DOI: 10.1039/D4AN00617H

Samantha M. McCabe, Hannah Gardiner, Calum Mullen, Gregory Q. Wallace, Neil C. Shand, Alexander B. Mullen, Linda Horan, Duncan Graham, Karen Faulds and Marie Boyd

Live chicken egg embryos offer new opportunities for evaluation and continuous monitoring of tumour growth for in vivo studies compared to traditional rodent models. Here, we report the first use of surface enhanced Raman scattering (SERS) mapping and surface enhanced spatially offset Raman scattering (SESORS) for the detection and localisation of targeted gold nanoparticles in live chicken egg embryos bearing a glioblastoma tumour.

与传统的啮齿类动物模型相比，活体鸡卵胚胎为体内研究提供了评估和持续监测肿瘤生长的新机会。在这里，我们报告了首次使用表面增强拉曼散射（SERS）绘图和表面增强空间偏移拉曼散射（SESORS）在携带人类胶质母细胞瘤肿瘤的活鸡蛋胚中检测和定位靶向金纳米粒子的情况。

引用次数: 0

Enabling the characterization of the nonlinear electrokinetic properties of particles using low voltage 利用低电压鉴定粒子的非线性电动特性

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-04 DOI: 10.1039/d4an00538d

J. Martin de los Santos-Ramirez, Carlos A Mendiola-Escobedo, Jose Manuel Cotera-Sarabia, Roberto Carlos Gallo-Villanueva, Rodrigo Martinez-Duarte, Victor H. Perez-Gonzalez

Insulator-based electrokinetically driven microfluidic devices stimulated with direct current (DC) voltages are an attractive solution for particle separation, concentration, or isolation. However, to design successful particle manipulation protocols, it is mandatory to know the mobilities of electroosmosis, and linear and nonlinear electrophoresis of the microchannel/liquid/particle system. Several techniques exist to characterize the mobilities of electroosmosis and linear electrophoresis. However, only one method to characterize the mobility of nonlinear electrophoresis has been thoroughly assessed, which generally requires DC voltages larger than 1000 V and measuring particle velocity in a straight microchannel. Under such conditions, Joule heating, electrolysis, and the DC power source cost become a concern. Also, measuring particle velocity at high voltages is noisy, limiting characterization quality. Here we present a protocol—tested on 2 µm polystyrene particles—for characterizing the mobility of nonlinear electrophoresis of the liquid/particle system using a DC voltage of only 30 V and visual inspection of particle dynamics in a microchannel featuring insulating obstacles. Multiphysics numerical modelling was used to guide microchannel design and to correlate particle location during an experiment with electric field intensity. The method was validated against the conventional characterization protocol, exhibiting excellent agreement while significantly reducing measurement noise and experimental complexity.

在直流电压的刺激下，基于绝缘体的电动微流控装置是一种极具吸引力的颗粒分离、浓缩或隔离解决方案。然而，要设计出成功的粒子操作方案，必须了解微通道/液体/粒子系统的电渗、线性和非线性电泳的流动性。有几种技术可以表征电渗和线性电泳的流动性。然而，只有一种表征非线性电泳流动性的方法经过了全面评估，这种方法通常需要大于 1000 V 的直流电压，并测量直微通道中粒子的速度。在这种条件下，焦耳热、电解和直流电源成本都会成为问题。此外，在高电压下测量粒子速度会产生噪声，从而限制了表征质量。在此，我们介绍了一种在 2 µm 聚苯乙烯颗粒上进行测试的方案，该方案利用仅 30 V 的直流电压和对微通道（具有绝缘障碍物）中颗粒动态的目测，来表征液体/颗粒系统非线性电泳的流动性。多物理场数值建模用于指导微通道设计，并将实验过程中粒子的位置与电场强度相关联。该方法与传统的表征规程进行了验证，显示出极佳的一致性，同时显著降低了测量噪声和实验复杂性。

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引用次数: 0

Recent Advances in Nanomaterial-Based Solid-Contact Ion-Selective Electrodes 基于纳米材料的固体接触离子选择电极的最新进展

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-04 DOI: 10.1039/d4an00334a

Seyed Oveis Mirabootalebi, Yang Liu

Solid-contact ion-selective electrodes (SC-ISEs) are advanced potentiometric sensors with high capability to detect a wide range of ions for monitoring of industrial processes and environmental pollutants, as well as determination of electrolytes for clinical analysis. Over the past decades, innovative design of ion-selective electrodes (ISEs), specifically SC-ISEs, to improve sensing performance including selectivity and sensitivity, has attracted considerable intersts. Recently, the utilisation of nanomaterials is particularly prominant in SC-ISEs due to their excellent physical and chemical properties. In this article, we review the recent applications of various types of nanostuctured materials that are composed of carbon, metal and polymer for the development of SC-ISEs. The challenges and opportunities in this field, along with the prospects of the future applications of nanomaterials in SC-ISE are also discussed.

固体接触式离子选择电极（SC-ISE）是一种先进的电位传感器，具有很强的检测各种离子的能力，可用于监测工业过程和环境污染物，以及测定临床分析中的电解质。在过去几十年中，离子选择性电极（ISE），特别是 SC-ISE 的创新设计引起了广泛关注，其目的是提高传感性能，包括选择性和灵敏度。最近，纳米材料因其优异的物理和化学特性在 SC-ISE 中的应用尤为突出。本文综述了由碳、金属和聚合物组成的各类纳米结构材料在开发 SC-ISE 中的最新应用。文章还讨论了这一领域的挑战和机遇，以及纳米材料在 SC-ISE 中的未来应用前景。

引用次数: 0

A Comparative Analysis of Stem Cell Differentiation on 2D and 3D Substrates using Raman Microspectroscopy 利用拉曼光谱对干细胞在二维和三维基底上的分化进行比较分析

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-04 DOI: 10.1039/d4an00315b

Francesca Ravera, Esen Efeoglu, Hugh J Byrne

Chondrogenesis is a complex cellular process that involves the transformation of mesenchymal stem cells (MSCs) into chondrocytes, the specialised cells that form cartilage. In recent years, three-dimensional (3D) culture systems have emerged as a promising approach to studying cell behaviour and development in a more physiologically relevant environment compared to traditional two-dimensional (2D) cell culture. The use of these systems provided insights into the molecular mechanisms that regulate chondrogenesis and has the potential to revolutionise the development of new therapies for cartilage repair and regeneration. This study demonstrates the successful application of Raman microspectroscopy (RMS) as a label-free, non-destructive, and sensitive method to monitor the chondrogenic differentiation of bone marrow-derived rat mesenchymal stem cells (rMSCs) in a collagen type I hydrogel, and explores the potential benefits of 3D hydrogels compared to conventional 2D cell culture environments. rMSCs were cultured on 3D substrates for 3 weeks and their differentiation was monitored by measuring the spectral signatures of their subcellular compartments. Additionally, the evolution of high-density micromass cultures was investigated to provide a comprehensive understanding of the process and complex interactions between cells and their surrounding extracellular matrix. For comparison, rMSCs were induced into chondrogenesis in identical medium conditions for 21 days in monolayer culture. Raman spectra showed that rMSCs cultured in a collagen type I hydrogel are able to undergo a distinct chondrogenic differentiation pathway at a significantly higher rate than the 2D culture cells. 3D cultures expressed stronger and more homogeneous chondrogenesis-associated peaks such as collagens, glycosaminoglycans (GAGs), and aggrecan while manifesting changes in proteins and lipidic content. These results suggest that 3D type I collagen hydrogel substrates are promising for in vitro chondrogenesis studies, and that RMS is a valuable tool for monitoring chondrogenesis in 3D environments.

软骨形成是一个复杂的细胞过程，涉及间充质干细胞（MSCs）向软骨细胞（形成软骨的特化细胞）的转化。近年来，与传统的二维（2D）细胞培养相比，三维（3D）培养系统已成为在更贴近生理的环境中研究细胞行为和发育的一种有前途的方法。利用这些系统可以深入了解调控软骨生成的分子机制，并有可能彻底改变软骨修复和再生新疗法的开发。本研究展示了拉曼光谱（RMS）作为一种无标记、非破坏性和灵敏的方法在监测骨髓来源的大鼠间充质干细胞（rMSCs）在 I 型胶原水凝胶中的软骨分化方面的成功应用，并探索了三维水凝胶与传统二维细胞培养环境相比的潜在优势。rMSCs 在三维基底上培养了 3 周，通过测量其亚细胞区的光谱特征监测其分化。此外，还对高密度微质量培养物的演变进行了研究，以全面了解细胞与其周围细胞外基质之间的过程和复杂的相互作用。为了进行比较，在相同的培养基条件下对 rMSCs 进行了为期 21 天的单层培养，诱导其形成软骨。拉曼光谱显示，在 I 型胶原水凝胶中培养的 rMSCs 能够以明显高于二维培养细胞的速度经历独特的软骨分化途径。三维培养物表达的胶原蛋白、糖胺聚糖（GAG）和凝集素等软骨形成相关峰值更强、更均匀，同时蛋白质和脂质含量也发生了变化。这些结果表明，三维 I 型胶原水凝胶基底有望用于体外软骨形成研究，而 RMS 是监测三维环境中软骨形成的重要工具。

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引用次数: 0

Identification of lipid-specific proteins with high-density lipid-immobilized beads. 利用高密度脂质固定珠鉴定脂质特异性蛋白质。

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-03 DOI: 10.1039/d4an00579a

Masayuki Morito, Hiroki Yasuda, Takaaki Matsufuji, Masanao Kinoshita, Nobuaki Matsumori

In biological membranes, lipids often interact with membrane proteins (MPs), regulating the localization and activity of MPs in cells. Although elucidating lipid-MP interactions is critical to comprehend the physiological roles of lipids, a systematic and comprehensive identification of lipid-binding proteins has not been adequately established. Therefore, we report the development of lipid-immobilized beads where lipid molecules were covalently immobilized. Owing to the detergent tolerance, these beads enable screening of water-soluble proteins and MPs, the latter of which typically necessitate surfactants for solubilization. Herein, two sphingolipid species-ceramide and sphingomyelin-which are major constituents of lipid rafts, were immobilized on the beads. We first showed that the density of immobilized lipid molecules on the beads was as high as that of biological lipid membranes. Subsequently, we confirmed that these beads enabled the selective pulldown of known sphingomyelin- or ceramide-binding proteins (lysenin, p24, and CERT) from protein mixtures, including cell lysates. In contrast, commercial sphingomyelin beads, on which lipid molecules are sparsely immobilized through biotin-streptavidin linkage, failed to capture lysenin, a well-known protein that recognizes clustered sphingomyelin molecules. This clearly demonstrates the applicability of our beads for obtaining proteins that recognize not only a single lipid molecule but also lipid clusters or lipid membranes. Finally, we demonstrated the screening of lipid-binding proteins from Neuro2a cell lysates using these beads. This method is expected to significantly contribute to the understanding of interactions between lipids and proteins and to unravel the complexities of lipid diversity.

在生物膜中，脂质经常与膜蛋白（MPs）相互作用，调节细胞中 MPs 的定位和活性。虽然阐明脂质与膜蛋白的相互作用对于理解脂质的生理作用至关重要，但系统而全面地鉴定脂质结合蛋白的工作尚未充分展开。因此，我们报告了脂质固定珠的开发情况，其中脂质分子被共价固定。由于具有去垢剂耐受性，这些珠子可以筛选水溶性蛋白质和 MPs，后者通常需要表面活性剂才能溶解。在这里，两种鞘脂类--神经酰胺和鞘磷脂--是脂筏的主要成分，被固定在珠子上。我们首先证明了固定在珠子上的脂质分子的密度与生物脂质膜的密度一样高。随后，我们证实这些珠子能从蛋白质混合物（包括细胞裂解液）中选择性地提取已知的鞘磷脂或神经酰胺结合蛋白（溶血素、p24 和 CERT）。相反，通过生物素-链霉亲和素连接将脂质分子稀疏固定在其上的商用鞘磷脂珠却未能捕获赖血宁，而赖血宁是一种众所周知的能识别簇状鞘磷脂分子的蛋白质。这清楚地表明，我们的珠子不仅适用于获得识别单个脂质分子的蛋白质，也适用于获得识别脂质簇或脂质膜的蛋白质。最后，我们展示了利用这些珠子从 Neuro2a 细胞裂解液中筛选脂质结合蛋白的方法。这种方法有望极大地促进人们对脂质和蛋白质之间相互作用的理解，并揭示脂质多样性的复杂性。

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引用次数: 0

Observation of anodic electrochemiluminescence from silicon quantum dots for the detection of hydrogen peroxide† 观测硅量子点的阳极电化学发光以检测过氧化氢

IF 3.6 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-03 DOI: 10.1039/D4AN00626G

Jing Wang, Yunfan Ying, Yuyao Zhang, Hao Ding, Yu Li, Jingjing Zhang and Dechen Jiang

Silicon quantum dots (QDs) with stable positively charged intermediates are prepared using chemical etching to generate strong anodic electrochemiluminescence (ECL) under a positive potential. Their surfaces could be passivated in the presence of strong oxidants, leading to enhanced ECL and offering the ability to carry out analysis for hydrogen peroxide.

具有稳定正电荷中间体的硅量子点（QDs）通过化学蚀刻预rared，在正电势下产生强烈的阳极电化学发光（ECL）。它们的表面可以在强氧化剂存在时被钝化，从而增强 ECL，提供分析过氧化氢的能力。

引用次数: 0

Ultrasensitive electrochemical immunosensor for the detection of C-reactive protein antigen 用于检测 C 反应蛋白抗原的超灵敏电化学免疫传感器

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-06-03 DOI: 10.1039/d4an00432a

Okoroike C. Ozoemena, Emmanuel Boateng, Aicheng Chen

Cardiovascular disease is one of the leading causes of premature death worldwide, and the determination of C-reactive protein (CRP) from human serum is of vital importance for the diagnosis of the disease. For this study, we have developed an electrochemical immunosensor based on onion-like carbon@polyacrylonitrile (OLC-PAN) for the detection of CRP antigens. This was accomplished by immobilizing CRP antibodies on a modified glassy carbon electrode (GCE). Several electrochemical techniques such as cyclic voltammetry (CV), square wave voltammetry (SWV), and electrochemical impedance spectroscopy (EIS) were employed to evaluate the electrochemical detection of the CRP antigen. This ultrasensitive method for CRP antigen detection exhibited a very good logarithmic plot from -4.52 to -12.05 g mL-1 and a limit of detection (LOD) of 0.9 fg mL-1. The high selectivity, sensitivity, and stability of the developed electrochemical immunosensor would facilitate miniaturization for point-of-care applications and the efficient diagnosis of cardiovascular diseases.

心血管疾病是导致全球过早死亡的主要原因之一，而测定人体血清中的 C 反应蛋白（CRP）对疾病的诊断至关重要。在这项研究中，我们开发了一种基于洋葱样碳@聚丙烯腈（OLC-PAN）的电化学免疫传感器，用于检测 CRP 抗原。这是通过将 CRP 抗体固定在改性玻璃碳电极（GCE）上实现的。为了评估 CRP 抗原的电化学检测效果，研究人员采用了多种电化学技术，如循环伏安法（CV）、方波伏安法（SWV）和电化学阻抗谱法（EIS）。这种超灵敏的 CRP 抗原检测方法在 -4.52 至 -12.05 g mL-1 范围内表现出非常好的对数曲线，检出限（LOD）为 0.9 fg mL-1。所开发的电化学免疫传感器具有高选择性、高灵敏度和高稳定性，有助于微型化的护理点应用和心血管疾病的高效诊断。

引用次数: 0

Molecularly imprinted polymer coated silica microbeads for high performance liquid chromatography 用于高效液相色谱的分子印迹聚合物包覆硅胶微珠

IF 4.2 3区化学 Q1 Chemistry

Analyst

Pub Date : 2024-05-31 DOI: 10.1039/d4an00239c

Wenpu Wu, Cuichi Yu, Lei Sui, Hui Xu, Jinhua Li, Na Zhou, Lingxin Chen, Zhihua Song

Molecularly imprinted polymers (MIPs) based chromatographic separation materials, owing to their advantages of unique selectivity, low cost, suitable reproducibility, and acceptable stability, have attracted a great deal of researchers in different fields. In this investigation, a new type of MIP coated silica (MIP/SiO2) separation material has been developed by using sulfamethoxazole as template; the specific recognition ability of MIP and appropriate physicochemical properties (abundant Si-OH, suitable pore structure, and good stability, etc.) of SiO2 microbeads were combined. The MIP/SiO2 separation materials were characterized carefully. Then, various compounds (such as sulfonamides, ginsenosides, nucleosides, and several pesticides) were used to comprehensively evaluate the chromatographic performance of MIP/SiO2 column. Furthermore, the chromatographic performances of MIP/SiO2 column were compared with those of other separation materials (like non-imprinted polymer coated silica, C18/SiO2, and bare silica) packed columns. The resolution value of all measured compounds was more than 1.51. And the column efficiency of 13,510 plates/m for sulfamethoxazole, 11,600 plates/m for ginsenoside Rd, and 10,510 plates/m for 2'-deoxyadenosine were obtained. The acceptable results verified that the MIP/SiO2 column can be applied for separation of highly polar drugs such as sulfonamides, ginsenosides, nucleosides, and pesticides.

基于分子印迹聚合物（MIPs）的色谱分离材料因其独特的选择性、低成本、合适的重现性和可接受的稳定性等优点吸引了不同领域的大量研究人员。本研究以磺胺甲噁唑为模板，结合 MIP 的特异性识别能力和 SiO2 微珠合适的理化性质（丰富的 Si-OH、合适的孔结构和良好的稳定性等），开发了一种新型 MIP 涂层二氧化硅（MIP/SiO2）分离材料。对 MIP/SiO2 分离材料进行了仔细的表征。然后，使用多种化合物（如磺胺类、人参皂苷、核苷类和多种农药）对 MIP/SiO2 色谱柱的色谱性能进行了综合评价。此外，还将 MIP/SiO2 色谱柱的色谱性能与其他分离材料（如无压印聚合物涂层硅胶、C18/SiO2 和裸硅胶）填料色谱柱的色谱性能进行了比较。所有测定化合物的分辨率均大于 1.51。磺胺甲噁唑的柱效为 13,510 板/米，人参皂苷 Rd 为 11,600 板/米，2'-脱氧腺苷为 10,510 板/米。结果表明，MIP/SiO2 柱可用于磺胺类、人参皂苷、核苷类和农药等高极性药物的分离。

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