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Development of folate-conjugated polypyrrole nanoparticles incorporated with nitrogen-doped carbon quantum dots for targeted bioimaging and photothermal therapy 开发叶酸与掺氮碳量子点结合的聚吡咯纳米粒子,用于靶向生物成像和光热疗法
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1016/j.talanta.2024.126528
Aakriti Prakash , Sujit Yadav , Preeti S. Saxena , Anchal Srivastava

PPy nanoparticles are widely employed as PTT agents, because of their exceptional near-infrared absorption properties. Nonetheless, the efficacy of PTT with PPy nanoparticles is hindered by a challenge, specifically, a lack of precise targeting. In this study, a PTT imaging agent was developed by combining NCQDs having bright green fluorescent properties with PPy nanoparticles along with the masking of folic acid to overcome the challenge of targeting. The synthesized PPy:NCQDs:FA nanocomposite, characterized by extraordinary photothermal property, was utilized for imaging of folate receptor positive (FA+) MCF-7 cancer cells through the emission of green fluorescence by NCQDs incorporated within the nanocomposite. Additionally, these nanoparticles demonstrated a good level of cell viability, exceeding 82 %, even at a concentration of 600 μg mL−1. Even the in vivo toxicity inspection of the nanocomposite exemplified no observed acute toxicity at experimental dosages of 1 and 3 mg per kg body weight. By subjecting MCF-7 cells, inoculated with 100 μg mL−1 of nanocomposite, to NIR laser irradiation for 5 min, a significant decline in cell viability was witnessed, establishing the photothermal therapeutic potency of the nanocomposite. The death of cancer cells induced by nanocomposite was verified through MTT assay, imaging of cells by NCQDs alone, with nanocomposite, and by live/dead cell Calcein AM/PI staining assay. Quantification of induced apoptosis post-laser treatment is conducted through staining with Annexin V-FITC/PI. These findings establish potential use of PPy:NCQDs:FA nanocomposite as versatile theranostic agents, capable of targeted bioimaging and treatment for cancer cells exhibiting folate receptors.

PPy 纳米粒子具有特殊的近红外吸收特性,因此被广泛用作 PTT 剂。然而,PPy 纳米粒子的 PTT 疗效却受到一个难题的阻碍,特别是缺乏精确的靶向性。本研究通过将具有亮绿色荧光特性的 NCQDs 与 PPy 纳米粒子相结合,再加上叶酸的掩蔽,开发出了一种 PTT 成像剂,从而克服了靶向性难题。合成的 PPy:NCQDs:FA 纳米复合材料具有非凡的光热特性,通过纳米复合材料中的 NCQDs 发射绿色荧光,对叶酸受体阳性(FA+)的 MCF-7 癌细胞进行成像。此外,即使在 600 μg mL-1 的浓度下,这些纳米颗粒的细胞存活率也超过了 82%。即使对纳米复合材料进行体内毒性检测,在实验剂量为每公斤体重 1 毫克和 3 毫克时,也没有观察到急性毒性。将接种了 100 μg mL-1 纳米复合材料的 MCF-7 细胞置于近红外激光照射 5 分钟后,细胞存活率显著下降,这证明了纳米复合材料的光热治疗功效。通过 MTT 试验、单独使用 NCQDs 和使用纳米复合材料对细胞成像以及活/死细胞 Calcein AM/PI 染色试验,验证了纳米复合材料诱导的癌细胞死亡。通过 Annexin V-FITC/PI 染色法对激光治疗后诱导的细胞凋亡进行量化。这些发现证实了 PPy:NCQDs:FA 纳米复合材料作为多功能治疗剂的潜在用途,它能够对显示叶酸受体的癌细胞进行靶向生物成像和治疗。
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引用次数: 0
Size and isotope analysis of individual nanoparticles by multi-collector ICP-MS using "event-triggered signal capture" with a high-speed oscilloscope. 利用高速示波器的 "事件触发信号捕获",通过多收集器 ICP-MS 对单个纳米粒子的尺寸和同位素进行分析。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1016/j.talanta.2024.126540
Pengju Xing, Nicholas Stanley Belshaw, Junhang Dong, Lujie Li, Yuanhui Geng, Hongtao Zheng, Xing Liu, Zhenli Zhu

Accurate quantitative elemental and isotope analysis of nanoparticles at the single-particle level is crucial for better understanding their origin, properties and behaviors. Single particle inductively coupled plasma-mass spectrometry (spICP-MS) has emerged as a promising technique for nanoparticle analysis. However, challenges persist in obtaining accurate and consistent element profiles and ratios for small-sized nanoparticles by conventional quadrupole (QMS) or time-of-flight mass analyzers (TOF-MS) due to their low level and transient nature. In this paper, we present a novel analytical method for single nanoparticle analysis using multiple collector ICP-MS (MC-ICP-MS) combined with a modern high-speed digital oscilloscope. The single particle events are acquired using an "event-triggered signal capture" (ETSC) technique, which enables the simultaneously capture and visualization of multiple isotopes of transient individual particle profiles with nanosecond time resolution. This greatly facilitates precise and efficient analysis of nanoparticles. The minimum detectable particle size is calculated to be as small as 8 nm (∼1 ag 109Ag) for AgNPs. Based on the 109/107Ag ratios obtained from 2000 particles, the precisions of 109/107Ag ratio measurements on 20 nm, 40 nm, 60 nm, 80 nm and 100 nm were approximately 0.086 (SD), 0.063 (SD), 0.051 (SD), 0.040 (SD), and 0.029 (SD), which is limited by counting statistics of the isotopic signals. Furthermore, the achieved standard error of 109/107Ag can be reduced to sub-permil level (0.7 ‰) even for the measurement of 20 nm AgNPs (N = 17,000). These results demonstrate that the ETSC provides a unique method for isotope analysis of single particles, holding great potential for enhancing our understanding of nanoparticles.

在单颗粒水平上对纳米颗粒进行精确的定量元素和同位素分析,对于更好地了解纳米颗粒的起源、特性和行为至关重要。单颗粒电感耦合等离子体质谱法(spICP-MS)已成为一种前景广阔的纳米颗粒分析技术。然而,由于小尺寸纳米粒子的低水平和瞬态性质,传统的四极杆(QMS)或飞行时间质谱分析仪(TOF-MS)在获得准确一致的元素分布和比率方面仍面临挑战。在本文中,我们介绍了一种使用多收集器 ICP-MS (MC-ICP-MS) 结合现代高速数字示波器进行单个纳米粒子分析的新型分析方法。单颗粒事件是利用 "事件触发信号捕获"(ETSC)技术获取的,该技术能够以纳秒级的时间分辨率同时捕获和显示多个同位素的瞬态单颗粒轮廓。这极大地促进了对纳米粒子的精确、高效分析。根据计算,AgNPs 的最小可检测粒径可小至 8 nm(∼1 ag 109Ag)。根据从 2000 个颗粒中获得的 109/107Ag 比率,对 20 nm、40 nm、60 nm、80 nm 和 100 nm 的 109/107Ag 比率测量的精确度约为 0.086(标度)、0.063(标度)、0.051(标度)、0.040(标度)和 0.029(标度),这受到同位素信号计数统计的限制。此外,即使测量 20 nm 的 AgNPs(N = 17,000),109/107Ag 的标准误差也可降至亚微米级(0.7 ‰)。这些结果表明,ETSC 为单个颗粒的同位素分析提供了一种独特的方法,在提高我们对纳米颗粒的认识方面具有巨大潜力。
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引用次数: 0
Exosomal membrane proteins analysis using a silicon nanowire field effect transistor biosensor 利用硅纳米线场效应晶体管生物传感器分析外泌体膜蛋白。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1016/j.talanta.2024.126534
Meiyan Qin , Jiawei Hu , Xue Li , Jinlong Liu , Rui Jiang , Yimin Shi , Zizhen Wang , Lingqian Zhang , Yang Zhao , Hang Gao , Qingzhu Zhang , Haiping Zhao , Mingxiao Li , Chengjun Huang

Exosomes are of great significance in clinical diagnosis, due to their high homology with parental generation, which can reflect the pathophysiological status. However, the quantitative and classification detection of exosomes is still faced with the challenges of low sensitivity and complex operation. In this study, we develop an electrical and label-free method to directly detect exosomes with high sensitivity based on a Silicon nanowire field effect transistor biosensor (Si-NW Bio-FET). First, the impact of Debye length on Si-NW Bio-FET detection was investigated through simulation. The simulation results demonstrated that as the Debye length increased, the electrical response to Si-NW produced by charged particle at a certain distance from the surface of Si-NW was greater. A Si-NW Bio-FET modified with specific antibody CD81 on the nanowire was fabricated then used for detection of cell line-derived exosomes, which achieved a low limit of detection (LOD) of 1078 particles/mL in 0.01 × PBS. Furthermore, the Si-NW Bio-FETs modified with specific antibody CD9, CD81 and CD63 respectively, were employed to distinguish exosomes derived from human promyelocytic leukemia (HL-60) cell line in three different states (control group, lipopolysaccharide (LPS) inflammation group, and LPS + Romidepsin (FK228) drug treatment group), which was consistent with nano-flow cytometry. This study provides a highly sensitive method of directly quantifying exosomes without labeling, indicating its potential as a tool for disease surveillance and medication instruction.

外泌体与亲代具有高度同源性,可以反映病理生理状态,因此在临床诊断中具有重要意义。然而,外泌体的定量和分类检测仍面临灵敏度低、操作复杂等难题。在本研究中,我们基于硅纳米线场效应晶体管生物传感器(Si-NW Bio-FET),开发了一种直接检测外泌体的高灵敏度无标记电学方法。首先,通过仿真研究了德拜长度对 Si-NW Bio-FET 检测的影响。仿真结果表明,随着德拜长度的增加,在距离 Si-NW 表面一定距离处的带电粒子对 Si-NW 产生的电响应更大。制备出的 Si-NW 生物场效应晶体管在纳米线上修饰了特异性抗体 CD81,然后用于检测细胞系衍生的外泌体,在 0.01 × PBS 中达到了 1078 粒子/毫升的低检测限(LOD)。此外,用分别修饰了特异性抗体 CD9、CD81 和 CD63 的 Si-NW 生物场效应晶体管区分了三种不同状态(对照组、脂多糖(LPS)炎症组和 LPS + 罗米地辛(FK228)药物治疗组)的人类早幼粒细胞白血病(HL-60)细胞系衍生的外泌体,这与纳米流式细胞术一致。这项研究提供了一种无需标记即可直接量化外泌体的高灵敏度方法,显示了其作为疾病监测和用药指导工具的潜力。
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引用次数: 0
Mechanism of high sensitivity proton acids doped polypyrrole molecularly imprinted electrochemical sensor and its application in urea detection 高灵敏度质子酸掺杂聚吡咯分子印迹电化学传感器的机理及其在尿素检测中的应用。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-10 DOI: 10.1016/j.talanta.2024.126514
Guangxing Hu , Shuang Cui , Hongda Wang , Yan Shi , Zhuang Li

Molecularly imprinted electrochemical sensor is a kind of convenient, fast, and stable analyzer, but the conductivity of electrode materials and their affinity with the analyte affect its performance. A proton acid (PSS, SA, SSA) doping method was proposed to improve the electrochemical performance of the polypyrrole molecularly imprinted polymer (PPy-MIP), which promoted the electropolymerization of pyrrole, reduced the charge transfer resistance, and increased the electrochemical surface area. In terms of both improving conductivity and affinity, the response of the proton acids doped the polypyrrole molecularly imprinted electrochemical sensors (PPy-MIECS) to urea was improved by 25-fold (PSS), 5-fold (SA), and 3-fold (SSA) over that of PPy-MIECS. In addition, the PSS-PPy-MIECS was validated for the practical application with a linear detection range from 0.1 mM to 100 mM, high selectivity (α = 39.73), reusability (RSD% = 4.54 %), reproducibility (RSD% = 0.93 %), and stability (11 days). The advantage of proton acid doping method in PSS-PEDOT-MIECS to urea and PSS-PPy-MIECS to glucose extended its application in the performance enhancement of MIECS design.

分子印迹电化学传感器是一种方便、快速、稳定的分析仪器,但电极材料的电导率及其与被分析物的亲和性会影响其性能。为改善聚吡咯分子印迹聚合物(PPy-MIP)的电化学性能,提出了质子酸(PSS、SA、SSA)掺杂法,促进了吡咯的电聚合,降低了电荷转移电阻,增加了电化学比表面积。在提高电导率和亲和力方面,掺杂质子酸的聚吡咯分子印迹电化学传感器(PPy-MIECS)对尿素的响应分别比 PPy-MIECS 提高了 25 倍(PSS)、5 倍(SA)和 3 倍(SSA)。此外,PSS-PPy-MIECS 还通过了实际应用验证,其线性检测范围为 0.1 mM 至 100 mM,具有高选择性(α = 39.73)、可重复使用性(RSD% = 4.54 %)、可重复性(RSD% = 0.93 %)和稳定性(11 天)。质子酸掺杂法在 PSS-PEDOT-MIECS 至尿素和 PSS-PPy-MIECS 至葡萄糖中的优势扩大了其在 MIECS 性能增强设计中的应用。
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引用次数: 0
ZIF-8-wrapped AgNPs modified with β-cyclodextrin for sensitive detection of thiacloprid and imidacloprid by SERS technology 用 β-环糊精修饰的 ZIF-8 包裹的 AgNPs 利用 SERS 技术灵敏检测噻虫啉和吡虫啉。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-09 DOI: 10.1016/j.talanta.2024.126524
Bin Yang , Jia Liu , Xin Liu , Shiyue Niu , Fengming Zhang , Yuting Wang , Daqian Song , Shuyun Bi

The high efficient surface-enhanced Raman scatterring (SERS) methods to detect thiacloprid and imidacloprid were established using ZIF-8-wrapped Ag nanoparticles (AgNPs) modified with β-cyclodextrin (β-CD). The substrate of ZIF-8/β-CD@AgNPs was characterized by ultraviolet visible spectra (UV–vis), thermogravimetric analysis (TGA), X-ray diffraction (XRD), transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM). The interaction between the substrate and thiacloprid/imidacloprid was also explored. The optimum measurement conditions were obtained by response surface model based on single-factor experiments. Enhancement factors (EFs) of thiacloprid and imidacloprid were respectively 2.29 × 106 and 2.60 × 106. A good linearity between the scattering intensity and the concentration of thiacloprid/imidacloprid within 3–1000 nmol L−1/6–400 nmol L−1 was established. The interference experiments indicated that the methods had good selectivity. The SERS methods were successfully applied to detect thiacloprid and imidacloprid in several vegetables samples. The recoveries ranged from 95.5 % to 105 % (n = 5). The detection limits (LODs) (S/N = 3) for thiacloprid and imidacloprid were 1.50 and 0.83 nmol L−1, respectively.

利用β-环糊精(β-CD)修饰的ZIF-8包裹的银纳米颗粒(AgNPs)建立了高效检测噻虫啉和吡虫啉的表面增强拉曼散射(SERS)方法。通过紫外可见光谱(UV-vis)、热重分析(TGA)、X 射线衍射(XRD)、透射电子显微镜(TEM)和扫描透射电子显微镜(STEM)对 ZIF-8/β-CD@AgNPs 的基底进行了表征。此外,还探讨了基质与噻虫啉/吡虫啉之间的相互作用。在单因素实验的基础上,通过响应面模型获得了最佳测量条件。噻虫啉和吡虫啉的增强因子(EF)分别为 2.29 × 106 和 2.60 × 106。在 3-1000 nmol L-1/6-400 nmol L-1 范围内,散射强度与噻虫啉/吡虫啉浓度之间具有良好的线性关系。干扰实验表明该方法具有良好的选择性。SERS 方法被成功地应用于检测多种蔬菜样品中的噻虫啉和吡虫啉。回收率在 95.5 % 到 105 % 之间(n = 5)。噻虫啉和吡虫啉的检出限(LOD)(S/N = 3)分别为 1.50 nmol L-1 和 0.83 nmol L-1。
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引用次数: 0
A dual-mode, image-enhanced, miniaturized microscopy system for incubator-compatible monitoring of live cells 双模式、图像增强、微型显微镜系统,用于对活细胞进行与培养箱兼容的监测。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-09 DOI: 10.1016/j.talanta.2024.126537
Yuheng Liao , Chunlian Qin , Xiaoyu Zhang , Jing Ye , Zhongyuan Xu , Haotian Zong , Ning Hu , Diming Zhang

Imaging live cells under stable culture conditions is essential to investigate cell physiological activities and proliferation. To achieve this goal, typically, a specialized incubation chamber that creates desired culture conditions needs to be incorporated into a microscopy system to perform cell monitoring. However, such imaging systems are generally large and costly, hampering their wide applications. Recent advances in the field of miniaturized microscopy systems have enabled incubator cell monitoring, providing a hospitable environment for live cells. Although these systems are more cost-effective, they are usually limited in imaging modalities and spatial temporal resolution. Here, we present a dual-mode, image-enhanced, miniaturized microscopy system (termed MiniCube) for direct monitoring of live cells inside incubators. MiniCube enables both bright field imaging and fluorescence imaging with single-cell spatial resolution and sub-second temporal resolution. Moreover, this system can also perform cell monitoring inside the incubator with tunable time scales ranging from a few seconds to days. Meanwhile, automatic cell segmentation and image enhancement are realized by the proposed data analysis pipeline of this system, and the signal-to-noise ratio (SNR) of acquired data is significantly improved using a deep learning based image denoising algorithm. Image data can be acquired with 5 times lower light exposure while maintaining comparable SNR. The versatility of this miniaturized microscopy system lends itself to various applications in biology studies, providing a practical platform and method for studying live cell dynamics within the incubator.

对稳定培养条件下的活细胞进行成像对于研究细胞的生理活动和增殖至关重要。要实现这一目标,通常需要在显微镜系统中加入一个能创造所需培养条件的专用培养室,以进行细胞监测。然而,这种成像系统通常体积庞大、成本高昂,阻碍了其广泛应用。微型显微镜系统领域的最新进展实现了培养箱细胞监测,为活细胞提供了适宜的环境。虽然这些系统更具成本效益,但它们通常在成像模式和空间时间分辨率方面受到限制。在这里,我们介绍一种双模式、图像增强、微型显微系统(称为 MiniCube),用于直接监测培养箱内的活细胞。MiniCube 可进行明视野成像和荧光成像,具有单细胞空间分辨率和亚秒级时间分辨率。此外,该系统还能在培养箱内进行细胞监测,时间尺度可调,从几秒到几天不等。同时,该系统提出的数据分析流水线实现了自动细胞分割和图像增强,并利用基于深度学习的图像去噪算法显著提高了采集数据的信噪比(SNR)。在保持相当信噪比的情况下,可以用低 5 倍的光照获取图像数据。这种微型显微系统用途广泛,可用于生物学研究的各种应用,为在培养箱中研究活细胞动态提供了一个实用的平台和方法。
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引用次数: 0
Bright luminol electrochemiluminescence mediated by a simple TEMPO radical for visualized multiplex detection 由简单 TEMPO 自由基介导的明亮发光酚电化学发光,用于可视化多重检测。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-09 DOI: 10.1016/j.talanta.2024.126530
Haidong Li, Guangyue Zhao, Yuxin Yang, Danli Zhong, Zhenxing Yang, Chengyin Wang

In this work, a series of 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) radicals bearing different functional groups were exploited as a simple catalyst to promote electrochemiluminescence (ECL) generation in luminol/H2O2 system. These TEMPO radicals were found to facilitate the electrochemical oxidation of H2O2 and luminol through different catalytic mechanisms, as well as the subsequent ECL generation of luminol/H2O2 system. The electrochemical oxidation and luminol ECL generation could be tuned by the functional group on the para-position of TEMPO, for which the structure/activity relationship was revealed. Finally, with the combination of enzymatic system, luminol ECL enhancement up to 9.6-fold was obtained through the catalysis of 4-hydroxyl-TEMPO. The enhanced luminol ECL allows acquiring brighter ECL images in a single-electrochemical system (SEES) for multiplex detection of cholesterol, H2O2 and glucose.

本研究利用一系列具有不同官能团的 2,2,6,6-四甲基哌啶-N-氧自由基(TEMPO)作为简单催化剂,促进发光酚/H2O2 体系中电化学发光(ECL)的产生。研究发现,这些 TEMPO 自由基通过不同的催化机理促进了 H2O2 和鲁米诺的电化学氧化,以及随后鲁米诺/H2O2 体系的 ECL 生成。电化学氧化和发光酚 ECL 生成可通过 TEMPO 对位上的官能团进行调节,并揭示了其结构/活性关系。最后,结合酶系统,通过催化 4-hydroxyl-TEMPO 可使发光酚 ECL 增强 9.6 倍。增强的发光酚 ECL 可以在单电化学系统(SEES)中获得更亮的 ECL 图像,用于胆固醇、H2O2 和葡萄糖的多重检测。
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引用次数: 0
Iron protoporphyrin IX-hyaluronan hydrogel-supported luminol chemiluminescence for the detection of nitric oxide in physiological solutions 铁原卟啉 IX-透明质酸水凝胶支持的发光酚化学发光法检测生理溶液中的一氧化氮
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-08 DOI: 10.1016/j.talanta.2024.126522
Amir M. Alsharabasy , Magesh Sankar , Manus Biggs , Pau Farràs , Abhay Pandit

Due to its role as a free radical signal-transducing agent with a short lifespan, precise measurement of nitric oxide (NO) levels presents significant challenges. Various analytical techniques offer distinct advantages and disadvantages for NO detection. This research aims to simplify the detection process by developing a hydrogel system using iron(III)-protoporphyrin IX (hemin)-loaded hyaluronan for the detection of NO in solution. Various hydrogel formulations were created, and the effects of their components on hydrogel-supported luminol chemiluminescence (CL) kinetics, radical scavenging, and physicochemical properties were analysed through factorial analysis. The candidate formulations were then evaluated using two NO donors. An increase in the degree of crosslinking in unloaded formulations enhanced interactions with the CL reaction components, hydrogen peroxide (H2O2) and luminol, thereby affecting light generation. However, hemin loading negated these effects, resulting in more prominent luminescence kinetics in formulations with lower crosslinking degrees. Similarly, NO influenced the kinetics differently, interacting with both the CL reaction and hydrogel components. Hemin-loaded formulations exhibited enhanced signal propagation when exposed to NO, followed by H2O2 and luminol, whereas reversing the order of addition inhibited this propagation. The magnitude of these luminescence changes depended on the type and concentration of the NO donor, demonstrating greater sensitivity to NO levels compared to amperometric sensing. These findings suggest that the studied hydrogel platform has potential for the facile and accurate detection of NO in solution, requiring minimal sample sizes.

由于一氧化氮(●NO)是一种寿命较短的自由基信号转导剂,因此精确测量一氧化氮(●NO)的水平是一项重大挑战。各种分析技术在检测 ●NO 方面各有利弊。本研究旨在开发一种使用铁(III)-原卟啉 IX(hemin)负载透明质酸的水凝胶系统,用于检测溶液中的●NO,从而简化检测过程。我们制作了各种水凝胶配方,并通过因子分析分析了其成分对水凝胶支持的发光酚化学发光(CL)动力学、自由基清除和理化性质的影响。然后使用两种●NO 供体对候选配方进行了评估。未负载配方中交联度的增加增强了与 CL 反应成分过氧化氢(H2O2)和发光酚的相互作用,从而影响了光的产生。然而,在交联度较低的制剂中,加载 hemin 可抵消这些影响,使发光动力学更为突出。同样,●NO 与 CL 反应和水凝胶成分相互作用,对动力学产生了不同的影响。当暴露于●NO、H2O2 和发光酚时,血红素负载的制剂显示出更强的信号传播,而颠倒添加顺序则会抑制信号传播。这些发光变化的程度取决于●NO 供体的类型和浓度,这表明与安培传感相比,●NO 水平对发光的敏感性更高。这些研究结果表明,所研究的水凝胶平台具有方便、准确地检测溶液中●NO 的潜力,而且只需最小的样品量。
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引用次数: 0
Optimizing Ni–Cr patterned boron-doped diamond band electrodes: Doping effects on electrochemical efficiency and posaconazole sensing performance 优化掺硼的镍铬图形金刚石带状电极:掺杂对电化学效率和泊沙康唑传感性能的影响
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-08 DOI: 10.1016/j.talanta.2024.126519
Anna Dettlaff , Michał Rycewicz , Łukasz Macewicz , Paweł Rutecki , Mirosław Sawczak , Paul Wittendorp , Shruti Jain , Elizaveta Vereshchagina , Robert Bogdanowicz

There is growing interest in developing diamond electrodes with defined geometries such as, for example, micrometer-sized electrode arrays to acquire signals for electroanalysis. For electroanalytical sensing applications, it is essential to achieve precise conductive patterns on the insulating surface. This work provides a novel approach to boron-doped diamond patterning using nichrome masking for selective seeding on an oxidized silicon substrate. The optimized process involves nichrome deposition, sonication, chemical etching, seeding, and tailored chemical vapor deposition of boron-doped diamond with an intrinsic layer to suppress boron diffusion. Through a systematic investigation, it was determined that isolated boron-doped diamond band electrodes can be efficiently produced on non-conductive silica. Additionally, the influence of boron doping on electrochemical performance was studied, with higher doping enhancing the electrochemical response of band electrodes. To demonstrate sensing capabilities, boron-doped diamond bands were used to detect posaconazole, an antifungal drug, exploiting its electroactive behaviour. A linear correlation between posaconazole concentration and oxidation peak current was observed over 1.43 × 10−8 – 5.71 × 10−6 M with a 1.4 × 10−8 M detection limit. The developed boron-doped diamond microbands could significantly impact the field of electroanalysis, facilitating detection of diverse biologically relevant molecules. Overall, this diamond patterning approach overcomes major challenges towards all-diamond electrochemical sensor chips.

人们对开发具有特定几何形状的金刚石电极越来越感兴趣,例如用于获取电分析信号的微米级电极阵列。对于电分析传感应用而言,在绝缘表面实现精确的导电图案至关重要。这项研究提供了一种在氧化硅基底上使用镍铬掩膜选择性播种的掺硼金刚石图案化新方法。优化后的工艺包括镍铬沉积、超声处理、化学蚀刻、播种,以及掺硼金刚石的定制化学气相沉积和抑制硼扩散的固有层。通过系统研究,可以确定在不导电的二氧化硅上可以有效地生产出孤立的掺硼金刚石带状电极。此外,还研究了硼掺杂对电化学性能的影响,掺杂量越高,带状电极的电化学响应越强。为了展示传感能力,我们利用掺硼金刚石带电极的电活性特性来检测抗真菌药物泊沙康唑。在 1.43 × 10-8 - 5.71 × 10-6 M 的范围内,观察到了泊沙康唑浓度与氧化峰电流之间的线性关系,检测限为 1.4 × 10-8 M。所开发的掺硼金刚石微带可对电分析领域产生重大影响,促进对各种生物相关分子的检测。总之,这种金刚石图案化方法克服了全金刚石电化学传感器芯片所面临的主要挑战。
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引用次数: 0
Concurrent manipulation of competitive mechanisms to construct glutathione-stabilized gold nanocluster-based dual-channel molecular classifier for metal ions detection and information steganography 同时操纵竞争机制,构建基于谷胱甘肽稳定金纳米簇的双通道分子分类器,用于金属离子检测和信息隐写术
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-08 DOI: 10.1016/j.talanta.2024.126526
Na Li , Qing-Hong Long , Xin-Yuan Li , Can Dong , Tian-Sheng Zhao , Xi Mai , Yong-Sen Zhao , Zhong-Feng Gao , Qin Wei , Fan Xia

Understanding charge transport in metal ion-mediated glutathione-stabilized gold nanoclusters (GSH-Au NCs) has proved difficult due to the presence of various competitive mechanisms, such as electron transfer (ET) and aggregation induction effect (AIE). In this paper, we present a dual-channel fluorescence (FL) and second-order Rayleigh scattering (SRS) sensing method for high-throughput classification of metal ions, relying on the competition between ET and AIE using GSH-Au NCs. The SRS signals show significant enhancement when Pb2+, Ag+, Al3+, Cu2+, Fe3+, and Hg2+ are present, as a result of the aggregation of GSH-Au NCs. Notably, the fluorescence signal exhibits the opposite trend. The FL intensities of GSH-Au NCs are enhanced by Pb2+, Ag+, and Al3+ through the AIE mechanism, while they are quenched by Cu2+, Fe3+, and Hg2+, which is dominated by the ET mechanism. By employing principal component analysis and hierarchical cluster analysis, these signals are transformed into unique fingerprints and Euclidean distances, respectively, enabling successful distinction of six metal ions and their mixtures with a low detection limit of 30 nM. This new strategy has successfully addressed interference from impurities in the testing of real water samples, demonstrating its strong ability to detect multiple metal ions. Impressively, we have achieved molecular cryptosteganography, which involves encoding, storing, and concealing information by transforming the selective response of GSH-Au NCs to binary strings. This research is anticipated to advance utilization of nanomaterials in logic sensing and information safety, bridging the gap between molecular sensors and information systems.

由于存在各种竞争机制,如电子转移(ET)和聚集诱导效应(AIE),因此很难理解金属离子介导的谷胱甘肽稳定金纳米团簇(GSH-Au NCs)中的电荷传输。本文提出了一种双通道荧光(FL)和二阶瑞利散射(SRS)传感方法,利用 GSH-Au NCs 的 ET 和 AIE 竞争机制对金属离子进行高通量分类。由于 GSH-Au NCs 的聚集作用,当 Pb2+、Ag+、Al3+、Cu2+、Fe3+ 和 Hg2+ 存在时,SRS 信号明显增强。值得注意的是,荧光信号呈现出相反的趋势。Pb2+ 、Ag+ 和 Al3+ 通过 AIE 机制增强了 GSH-Au NCs 的荧光强度,而 Cu2+ 、Fe3+ 和 Hg2+ 则通过 ET 机制淬灭了 GSH-Au NCs 的荧光强度。通过采用主成分分析和分层聚类分析,这些信号分别被转化为独特的指纹和欧氏距离,从而成功区分了六种金属离子及其混合物,检测限低至 30 nM。这种新策略成功地解决了真实水样检测中杂质的干扰问题,证明了其检测多种金属离子的强大能力。令人印象深刻的是,我们还实现了分子密码学,即通过将 GSH-Au NCs 的选择性反应转化为二进制字符串来编码、存储和隐藏信息。这项研究有望推动纳米材料在逻辑传感和信息安全方面的应用,在分子传感器和信息系统之间架起一座桥梁。
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引用次数: 0
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