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Advanced design of target-driven self-powered sensor assisted by cascade catalytic strategy 级联催化策略辅助下的目标驱动型自供电传感器的先进设计
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-23 DOI: 10.1016/j.aca.2024.343359
Zongshan Zhang , Jing Xu , Lei Zhang , Gaoli Zhang , Hui Li
In this work, a self-powered microsensor platform based on enzyme biofuel cells (EBFCs) was developed for intelligent monitoring of disease markers miRNA-451. The cascade catalysis system constructed by using the strategy of enzyme-like ZIF-8 nanocapsule incorporation with biological enzymes, which could simultaneously take into account the specificity of biological enzymes and the high activity of nano-enzymes, significantly promoted the electron transfer between glucose and the bio-anode surface, and improved the sensitivity and stability of the sensing system. Meanwhile, the target-triggered hybridization chain reaction (HCR) amplification strategy to achieve exponential signal amplification based on accurate recognition, and jointly improve the detection sensitivity. As expected, the micro-sensor platform has a wide linear range of 0.5–1.0 fmol/L with a low limit of detection (LOD) of 0.13 fmol/L (S/N = 3) and exhibits excellent selectivity, reproducibility and stability in interference assays under optimal detection conditions. The designed self-powered system is simple to construct, easy to transport and the data transmission mode is intelligent and controllable, which is expected to be used in basic biochemical research, clinical diagnosis and environmental monitoring.
本研究开发了一种基于酶生物燃料电池(EBFCs)的自供电微传感器平台,用于智能监测疾病标志物miRNA-451。利用类酶 ZIF-8 纳米胶囊与生物酶结合的策略构建的级联催化系统,兼顾了生物酶的特异性和纳米酶的高活性,显著促进了葡萄糖与生物阳极表面的电子传递,提高了传感系统的灵敏度和稳定性。同时,采用目标触发杂交链反应(HCR)放大策略,在准确识别的基础上实现指数级信号放大,共同提高了检测灵敏度。正如预期的那样,微传感器平台的线性范围宽达 0.5-1.0 fmol/L,检出限(LOD)低至 0.13 fmol/L(S/N=3),并在最佳检测条件下的干扰检测中表现出优异的选择性、重现性和稳定性。所设计的自供电系统构造简单、运输方便,数据传输模式智能可控,有望用于基础生化研究、临床诊断和环境监测。
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引用次数: 0
Comprehensive targeted profiling of multiple steroid classes in rodent plasma using liquid chromatography-mass spectrometry 利用液相色谱-质谱法对啮齿动物血浆中的多种类固醇进行全面的靶向分析
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-23 DOI: 10.1016/j.aca.2024.343362
Taťána Gazárková , Hana Kočová Vlčková , Kateřina Plachká , Karla Vagnerová , Dominika Dubecová , Petra Klusoňová , Jiří Pácha , Frantisek Svec , Lucie Nováková

Background

Reliable quantification of multiple steroid classes in biological fluids within a single method remains an analytical challenge despite many previously published methods. Crosstalk of positional isomers, overlap of stereoisomer fragmentation patterns, differing proton affinities, in-source fragmentation, varying stability of protonated ions in the gas phase across steroid classes, and non-existence of steroid-free matrix are the main challenges limiting the number of simultaneously profiled steroids.

Results

In this study, we focused on the development of a derivatization-free, achiral, high-throughput, and cost-effective UHPLC-MS/MS approach that allows simultaneous profiling of a spectrum of 38 steroids covering progestogens, androgens, corticosteroids, and estrogens, while properly addressing the hurdles of steroid analysis. Within a 20-min method, 16 stereoisomers and 15 positional isomers were fully resolved within a single run while separated from 7 additional non-interfering steroids and matrix interferences in rodent plasma. Protein precipitation (PP) and supported liquid extraction (SLE) methods using only 40 μL of sample were developed to achieve the lowest possible limits of quantification. Nevertheless, 5α-dihydroprogesterone and 3α,5α-THDOC could be only qualitatively assessed when using PP. In contrast, DHEA-S could not be quantified or identified when using SLE. A novel surrogate matrix-background subtraction approach, using rat plasma after the animal's adrenalectomy, has been implemented into the optimized PP-UHPLC-MS/MS workflow, successfully validated according to the unified ICH/EMA M10 guidelines, and compared to the traditional quantification strategies. Moreover, the validity of the newly adopted approach has been verified by the targeted profiling of multiple biologically active endogenous steroids in more than 500 samples of mouse plasma in total.

Significance

Underestimation of hurdles associated with steroid analysis often compromises the accurate steroid quantification. Our comprehensive, fully validated UHPLC-MS/MS method targeting a wide spectrum of endogenous steroids, mitigating steroid crosstalk and using a minimal sample volume together with a novel surrogate matrix-background subtraction approach significantly advances steroid analysis for research and clinical applications covering multiple biological scopes.
背景尽管以前发表过许多方法,但用一种方法对生物液体中的多种类固醇进行可靠的定量仍然是一项分析挑战。位置异构体的串扰、立体异构体碎片模式的重叠、质子亲和力的不同、源内碎片、不同类固醇在气相中质子化离子的稳定性不同以及不存在不含类固醇的基质是限制同时分析类固醇数量的主要挑战。结果在这项研究中,我们重点开发了一种无衍生化、非手性、高通量、高性价比的超高效液相色谱-质谱/质谱分析方法,该方法可同时分析 38 种类固醇,涵盖孕激素、雄激素、皮质类固醇和雌激素,同时还能妥善解决类固醇分析中遇到的障碍。在 20 分钟的方法中,一次运行即可完全解析 16 种立体异构体和 15 种位置异构体,同时与啮齿类动物血浆中另外 7 种非干扰类固醇和基质干扰分离。为了达到尽可能低的定量限,我们开发了仅使用 40 μL 样品的蛋白质沉淀和辅助液体萃取方法。然而,使用蛋白沉淀法只能定性评估 5α-二氢孕酮和 3α,5α-THDOC。与此相反,使用 SLE 时无法定量或识别 DHEA-S。在优化的PP-UHPLC-MS/MS工作流程中采用了一种新颖的替代基质-背景减去方法,该方法使用的是动物肾上腺切除术后的大鼠血浆,根据统一的ICH/EMA M10指南成功地进行了验证,并与传统的定量策略进行了比较。此外,在总共 500 多份小鼠血浆样本中对多种具有生物活性的内源性类固醇进行了有针对性的分析,从而验证了新方法的有效性。我们的超高效液相色谱-质谱/质谱(UHPLC-MS/MS)方法针对多种内源性类固醇,减轻了类固醇的串扰,样品量极少,并采用了新颖的替代基质-背景减去方法,极大地推动了类固醇分析在多种生物学领域的研究和临床应用。
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引用次数: 0
Dual-mode sensing platform for Bisphenol A detection via bifunctional CsPbBr3@Cu-MOF assisted fluorescence and colorimetric analysis 通过双功能 Cu-MOF@CsPbBr3 辅助荧光和比色分析检测双酚 A 的双模式传感平台
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1016/j.aca.2024.343354
Junyi Ma , Ying-zhuo Shen , Jianxiao Gong , Seitkhan Azat , Zheng Ping Ji , Xiao-Ya Hu , Qin Xu

Background

Bisphenol A (BPA) has been identified as an endocrine disruptor with numerous detrimental effects on human health. There is an urgent need to develop fluorescence/colorimetric dual-mode sensing approaches with expanded detection linear range, increased accuracy, and enhanced application flexibility for BPA detection. The utilization of fluorescence and colorimetric signals in point-of-care applications and real-time sensitive sensing further highlights the significance of developing novel and efficient fluorescence/colorimetric dual-mode sensing platform with high-efficiency probes.

Results

Herein, a fluorescence and colorimetric dual-mode aptasensor was developed by using CsPbBr3@Cu-MOF as the aptamer immobilization matrix and signal generator. CsPbBr3 was functionalized with Cu-MOF using a simple two-step strategy. This strategy involved in-situ formation and modified ligand-assisted precipitation technique with 4,4′-bipyridine (4,4-Bpy) serving as the bifunctional linker. The resulting CsPbBr3@Cu-MOF exhibited improved stability in water and enhanced fluorescence. Additionally, it functioned as peroxidase mimetic to oxidize 3,3′,5,5′-tetramethyl benzidine (TMB), leading to a colorimetric change from colorless to blue. In the presence of BPA, aptamers were removed from CsPbBr3@Cu-MOF. Consequently, the fluorescence and peroxidase-activity of CsPbBr3@Cu-MOF were recovered, resulting in the enhanced fluorescence intensity and color change of TMB. Using this system, the proposed aptasensor demonstrated detection ranges of 1.0–80.0 nM with a LOD of 0.60 nM for the colorimetric method, and a linearity range of 0.1–100 nM with a LOD of 0.02 nM for the fluorescence method.

Significance

The obtained CsPbBr3@Cu-MOF composites showed excellent fluorescence properties, good peroxidase-like activity, and aqueous stability. Furthermore, the proposed dual-mode aptasensor demonstrated simplicity, cost-effectiveness and good anti-interference abilities. This can be extended to the construction of other dual-mode sensors by changing aptamers and provides novel insights on the potential applications of perovskites in bioanalysis.
背景双酚 A(BPA)已被确认为一种内分泌干扰物,对人体健康有诸多不利影响。目前急需开发荧光/比色双模式传感方法,以扩大双酚 A 检测的线性范围、提高准确性和应用灵活性。结果本文以 CsPbBr3@Cu-MOF 作为适配体固定基质和信号发生器,开发了一种荧光和比色双模式适配体传感器。CsPbBr3 通过简单的两步策略与 Cu-MOF 功能化。该策略包括原位形成和改进的配体辅助沉淀技术,以 4,4'-联吡啶(4,4-Bpy)作为双功能连接剂。由此产生的 CsPbBr3@Cu-MOF 在水中的稳定性更好,荧光也更强。此外,它还能作为过氧化物酶模拟物,氧化 3,3′,5,5′-四甲基联苯胺(TMB),从而使比色值从无色变为蓝色。在双酚 A 的存在下,CsPbBr3@Cu-MOF 中的适配体被去除。因此,CsPbBr3@Cu-MOF 的荧光和过氧化物酶活性得以恢复,从而增强了 TMB 的荧光强度和颜色变化。利用该系统,拟议的适配传感器在比色法中的检测范围为 1.0 至 80.0 nM,LOD 为 0.60 nM;在荧光法中的线性范围为 0.1 至 100 nM,LOD 为 0.02 nM。此外,所提出的双模灵敏度传感器具有简便、经济和良好的抗干扰能力。通过改变适配体,该研究还可扩展到其他双模传感器的构建,并为包晶石在生物分析中的潜在应用提供了新的见解。
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引用次数: 0
Enhanced data point importance: Layered significance of variables in multivariate calibration 增强数据点重要性:多变量校准中变量的分层重要性
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1016/j.aca.2024.343357
Somaye Vali Zade , Klaus Neymeyr , Mathias Sawall , Hamid Abdollahi

Background

The Enhanced Data Point Importance (EDPI) method, a systematic approach for evaluating the importance of data points in multivariate calibration, is introduced. Factor decomposition methods allow for the evaluation of the impact of variables on maintaining the structural pattern of data in the abstract space. Essential data points play a key role in these patterns and the method of Data Point Importance (DPI) aims to evaluate the essential data points in terms of their importance. All other points are rated by zero. In this contribution, DPI is extended to include inner points to evaluate the importance of these points in the absence of the essential points. The EDPI method employs convex peeling to sort data points systematically.

Results

EDPI method was applied to near-infrared and Raman spectroscopy data sets, including corn and alcohol mixtures and simulated data, to rank and select important variables. EDPI effectively identified variables that contributed to the preservation of the data structure and highlighted key spectral regions with different degrees of selectivity. In the alcohol dataset, EDPI revealed important physicochemical insights by focusing on specific regions where non-analytes spectra overlapped. It performed in a similar way to the Variable Importance in Projection (VIP) method, but with fewer variables selected.

Significance

The experimental results obtained from calibrating near-infrared and Raman spectroscopic datasets using partial least squares highlight the effectiveness of the proposed EDPI strategy when contrasted with the conventional variable importance in projection (VIP) method for variable selection.
背景介绍增强数据点重要性(EDPI)方法是一种评估多元校准中数据点重要性的系统方法。因子分解方法可以评估变量对维持抽象空间中数据结构模式的影响。基本数据点在这些模式中起着关键作用,数据点重要性(DPI)方法旨在评估基本数据点的重要性。所有其他点的评分均为零。在本文中,DPI 扩展到包括内部点,以便在没有基本点的情况下评估这些点的重要性。结果将 EDPI 方法应用于近红外和拉曼光谱数据集,包括玉米和酒精混合物以及模拟数据,对重要变量进行排序和选择。EDPI 有效地识别了有助于保持数据结构的变量,并突出了具有不同选择性的关键光谱区域。在酒精数据集中,EDPI 通过关注非分析物光谱重叠的特定区域,揭示了重要的物理化学观点。它的性能与投影变量重要性(VIP)方法类似,但选择的变量更少。重要意义使用偏最小二乘法校准近红外和拉曼光谱数据集所获得的实验结果,与传统的投影变量重要性(VIP)变量选择方法相比,凸显了所提出的 EDPI 策略的有效性。
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引用次数: 0
On-The-Flight trapping, LIBS analysis and discrimination of single meteorite particles generated by laser ablation 对激光烧蚀产生的单个陨石颗粒进行飞行捕获、Libs 分析和鉴别
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1016/j.aca.2024.343361
C. Burgos-Palop , F.J. Fortes , P. Purohit , T. Delgado , J. Laserna

Background

Thousands of micrometeorites fall to the Earth on a daily basis. Most of these meteorites have a rocky composition, but others are mainly composed of iron and nickel. Due to their small size, often ca. 100 μm in diameter, the process of searching for, collecting, and identifying these samples is remarkably tedious. In this work, we introduce a minimally invasive methodology for evaluating the full elemental composition of micrometeorites using optical emission spectroscopy of single particles produced by laser ablation of bulk targets.

Results

Bulk meteorite samples were directly ablated within an ablation cell. From few micrograms of ablated matrix, we originated dry aerosols consisting of multielemental particles which were representative of the sample chemistry. SEM images confirmed that the generated particles exhibited spherical geometry. Particles were first optically trapped in air and, then, analyzed by laser-induced breakdown spectroscopy (LIBS). LIBS spectra evidenced compositional differences among samples. For example, Campo de Cielo meteorite featured a high iron content due to its metallic nature whereas LIBS results for Jbilet Winselwan and NWA 869 suggested that pyroxene components dominated the composition of the samples. In contrast, NWA 13739 and Vaca Muerta contained high aluminum intensity, thus indicating that the feldspathic component was dominant, as then verified by XRD. The intra-sample compositional variability were quite satisfactory, as revealed by the RSD data, below 45 %. For quantitative analysis, the percentages of FeO, SiO2, Al2O3, Na2O, MgO, TiO2, CaO, K2O, MnO, SrO, Cr2O3, and Li2O were calculated using CF-LIBS.

Significance

This work demonstrates the applicability of laser excitation of individual particles in an optical trap for the multielemental analysis of meteorites. The methodology provides a complete overview of the samples, is capable of classificating them according to their main phases and yield preliminary quantitative information about those phases. Therefore, we present a minimally destructive pathway to be used as the first step in the inspection of these delicate samples. If the particles represent nanostructures inherent to the meteorites, it would constitute a major step in the analysis of extraterrestrial material that may provide fundamental insights into the structure and composition of the original materials at the microscale, a topic that remains an active area of research worldwide.
背景每天有数以千计的微陨石坠落到地球上。这些陨石大多数都是岩石成分,但也有一些主要由铁和镍组成。由于这些陨石体积小,直径通常只有约 100 微米,因此寻找、收集和鉴定这些样本的过程非常繁琐。在这项工作中,我们介绍了一种微创方法,利用激光烧蚀大块目标产生的单个颗粒的光学发射光谱来评估微陨石的全部元素组成。我们从几微克的烧蚀基质中产生了由多元素颗粒组成的干气溶胶,这些颗粒代表了样品的化学成分。扫描电子显微镜图像证实,生成的颗粒呈球形。首先在空气中对颗粒进行光学捕获,然后用激光诱导击穿光谱(LIBS)进行分析。激光诱导击穿光谱分析结果表明,不同样品之间存在成分差异。例如,Campo de Cielo 陨石因其金属特性而具有较高的铁含量,而 Jbilet Winselwan 和 NWA 869 的激光诱导击穿光谱分析结果表明,样品成分中主要是辉石成分。相比之下,NWA 13739 和 Vaca Muerta 含有较高的铝强度,从而表明长石成分占主导地位,XRD 也验证了这一点。正如 RSD 数据所显示的,样品内部的成分变化非常令人满意,低于 45%。为了进行定量分析,使用 CF-LIBS 计算了 FeO、SiO2、Al2O3、Na2O、MgO、TiO2、CaO、K2O、MnO、SrO、Cr2O3 和 Li2O 的百分比。该方法提供了样品的完整概览,能够根据主要物相对样品进行分类,并获得有关这些物相的初步定量信息。因此,我们提出了一种破坏性最小的方法,作为检测这些微妙样本的第一步。如果这些颗粒代表了陨石固有的纳米结构,那么这将是分析地外物质的重要一步,可以从根本上了解原始材料在微观尺度上的结构和组成,而这一主题仍然是全世界研究的一个活跃领域。
{"title":"On-The-Flight trapping, LIBS analysis and discrimination of single meteorite particles generated by laser ablation","authors":"C. Burgos-Palop ,&nbsp;F.J. Fortes ,&nbsp;P. Purohit ,&nbsp;T. Delgado ,&nbsp;J. Laserna","doi":"10.1016/j.aca.2024.343361","DOIUrl":"10.1016/j.aca.2024.343361","url":null,"abstract":"<div><h3>Background</h3><div>Thousands of micrometeorites fall to the Earth on a daily basis. Most of these meteorites have a rocky composition, but others are mainly composed of iron and nickel. Due to their small size, often ca. 100 μm in diameter, the process of searching for, collecting, and identifying these samples is remarkably tedious. In this work, we introduce a minimally invasive methodology for evaluating the full elemental composition of micrometeorites using optical emission spectroscopy of single particles produced by laser ablation of bulk targets.</div></div><div><h3>Results</h3><div>Bulk meteorite samples were directly ablated within an ablation cell. From few micrograms of ablated matrix, we originated dry aerosols consisting of multielemental particles which were representative of the sample chemistry. SEM images confirmed that the generated particles exhibited spherical geometry. Particles were first optically trapped in air and, then, analyzed by laser-induced breakdown spectroscopy (LIBS). LIBS spectra evidenced compositional differences among samples. For example, <em>Campo de Cielo</em> meteorite featured a high iron content due to its metallic nature whereas LIBS results for <em>Jbilet Winselwan</em> and <em>NWA 869</em> suggested that pyroxene components dominated the composition of the samples. In contrast, <em>NWA 13739</em> and <em>Vaca Muerta</em> contained high aluminum intensity, thus indicating that the feldspathic component was dominant, as then verified by XRD. The intra-sample compositional variability were quite satisfactory, as revealed by the RSD data, below 45 %. For quantitative analysis, the percentages of FeO, SiO<sub>2</sub>, Al<sub>2</sub>O<sub>3</sub>, Na<sub>2</sub>O, MgO, TiO<sub>2</sub>, CaO, K<sub>2</sub>O, MnO, SrO, Cr<sub>2</sub>O<sub>3</sub>, and Li<sub>2</sub>O were calculated using CF-LIBS.</div></div><div><h3>Significance</h3><div>This work demonstrates the applicability of laser excitation of individual particles in an optical trap for the multielemental analysis of meteorites. The methodology provides a complete overview of the samples, is capable of classificating them according to their main phases and yield preliminary quantitative information about those phases. Therefore, we present a minimally destructive pathway to be used as the first step in the inspection of these delicate samples. If the particles represent nanostructures inherent to the meteorites, it would constitute a major step in the analysis of extraterrestrial material that may provide fundamental insights into the structure and composition of the original materials at the microscale, a topic that remains an active area of research worldwide.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1332 ","pages":"Article 343361"},"PeriodicalIF":5.7,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mid-level data fusion strategy based on urinary nucleosides SERS spectra and blood CEA levels for enhanced preoperative detection of lymph node metastasis in colorectal cancer 基于尿核苷 SERS 光谱和血 CEA 水平的中层数据融合策略用于增强结直肠癌淋巴结转移的术前检测
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1016/j.aca.2024.343360
Jinyong Lin , Yuduo Wu , Zhizhong Lin , Xueliang Lin , Qiong Wu , JiaJia Lin , Yuanji Xu , Shangyuan Feng , Junxin Wu

Background

Preoperative prediction of lymph node metastasis (LNM) plays a crucial role in the treatment and prognosis of colorectal cancer (CRC). The traditional histopathological examination is invasive and time-consuming, providing pathological features only postoperatively. Preoperative serum carcinoembryonic antigen (CEA) is strongly correlated with postoperative LN status. However, the detection accuracy of LNM based on a single preoperative CEA level is low. Therefore, developing a more powerful and sensitive diagnostic tool would be of great clinical value for improving the accurate preoperative prediction of LNM in CRC patients.

Results

This study aimed to develop a mid-level fusion approach using urinary nucleosides Raman spectra and blood CEA data to enhance the preoperative discrimination of CRC patients with and without LNM. Surface-enhanced Raman scattering (SERS) spectra of urinary modified nucleosides, isolated by affinity chromatography, were first acquired from 48 patients with LNM and 49 patients without LNM. The principal component analysis (PCA) scores obtained from the SERS spectra were then combined with preoperative blood CEA values to create a fused data array. The discriminant accuracy based on either dataset alone or the fused data was evaluated using three machine learning algorithms: linear discriminant analysis, k-nearest neighbors, and support vector machine. Results showed that the fused data could discriminate between the two groups with an accuracy of up to 91 %, outperforming SERS alone (86 %) and CEA alone (69 %).

Significance

To our knowledge, this is the first report of mid-level data fusion of urinary nucleosides SERS spectra with blood CEA levels for the preoperative prediction of LNM in CRC. This work demonstrates that the mid-level data fusion strategy aided by SVM algorithm can greatly improve the preoperative prediction accuracy of LNM. This is crucial for therapeutic decision-making and prognostic assessment in CRC.
背景术前预测淋巴结转移(LNM)对结直肠癌(CRC)的治疗和预后起着至关重要的作用。传统的组织病理学检查具有创伤性且耗时,只能在术后提供病理特征。术前血清癌胚抗原(CEA)与术后 LN 状态密切相关。然而,基于单一术前 CEA 水平的 LNM 检测准确率很低。因此,开发一种更强大、更灵敏的诊断工具将对提高 CRC 患者术前 LNM 的准确预测具有重要的临床价值。结果 本研究旨在开发一种中层融合方法,利用尿液核苷拉曼光谱和血液 CEA 数据来提高有 LNM 和无 LNM 的 CRC 患者的术前分辨能力。首先从 48 名 LNM 患者和 49 名非 LNM 患者中获取了通过亲和层析法分离的尿液修饰核苷的表面增强拉曼散射(SERS)光谱。然后将从 SERS 光谱中获得的主成分分析 (PCA) 分数与术前血液 CEA 值相结合,创建一个融合数据阵列。使用三种机器学习算法(线性判别分析、k-近邻和支持向量机)评估了基于单独数据集或融合数据的判别准确性。结果表明,融合数据对两组患者的区分准确率高达 91%,优于单独使用 SERS(86%)和单独使用 CEA(69%)。这项工作表明,SVM 算法辅助下的中层数据融合策略可大大提高 LNM 的术前预测准确率。这对 CRC 的治疗决策和预后评估至关重要。
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引用次数: 0
Fluorescence imaging of dopamine in living cells triggered by unique coupling reactions 独特耦合反应引发的活细胞多巴胺荧光成像
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1016/j.aca.2024.343358
Shaofei Fu , Jianwen Qiu , Biaofeng Gu , Yong Gao

Background

Dopamine (DA) is a significant neurotransmitter and catecholamine molecule in the mammalian brain. It plays a crucial role in perception, cognition, central nervous system regulation, and hormone secretion. The detection of DA levels in living systems is a vital aspect of the research and early diagnosis of neurological disorders.

Results

In this study, we achieved an effective fluorescence generation specific to DA under physiological pH conditions by coupling the DA detection reaction to the HClO oxidation reaction. This method has been used for the detection of DA in cells, as well as for the visualization of DA levels in cellular models of inflammation and depression.

Significance

This is the first time that utilizes an organic fluorescent molecular probe to detect DA in living cells.
背景多巴胺(DA)是哺乳动物大脑中一种重要的神经递质和儿茶酚胺分子。它在感知、认知、中枢神经系统调节和激素分泌中起着至关重要的作用。结果在这项研究中,我们通过将 DA 检测反应与 HClO 氧化反应耦合,在生理 pH 条件下实现了有效的 DA 特异荧光生成。该方法已被用于细胞中 DA 的检测,以及炎症和抑郁细胞模型中 DA 水平的可视化。
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引用次数: 0
Development of a multiplexing method for the quantification of “high-risk” host cell lipases in biotherapeutics by Luminex 利用 Luminex 开发用于定量生物治疗药物中 "高风险 "宿主细胞脂肪酶的多重方法
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-21 DOI: 10.1016/j.aca.2024.343349
Jeremy D. Osko, Shannon Rivera, Fengqiang Wang, Thomas Niedringhaus
Clearance of residual Host Cell Proteins (HCPs) is critical for the manufacturing processes of biotherapeutics. HCPs have the potential to impact product efficacy and quality, posing a risk to patient safety. It is therefore essential to be able to both identify and quantitate HCPs throughout drug development, even if the proteins are present in low concentrations. Traditional Enzyme-Linked Immunosorbent Assays (ELISAs) have historically served as the gold standard for monitoring HCPs; however, ELISA methods are labor-intensive and costly. With an increase of HCPs being identified below detectable quantification levels, there is a need for simultaneous detection of selectively targeted HCPs. Here, we develop a Luminex multiplexing method that is able to accurately quantify two “high-risk” lipases Lipoprotein Lipase (LPL) and Phospholipase B-Like 2 (PLBL2) within the same assay. This study outlines the method development for optimizing parameters such as antibody constructs, conjugation ratios, signal enhancement, and more in order to create the most efficient multiplexing method. As a result, a Luminex multiplexing method can provide a similar result to a monoplexing ELISA method but in a faster and more cost-effective manner. This method can be expanded to include other “high-risk” HCPs and used for future HCP applications.
清除残留的宿主细胞蛋白 (HCP) 对生物治疗药物的生产过程至关重要。HCP 有可能影响产品的疗效和质量,给患者安全带来风险。因此,在整个药物开发过程中,即使蛋白质的浓度很低,也必须能够识别和定量 HCP。传统的酶联免疫吸附试验(ELISA)历来是监测 HCPs 的黄金标准,但 ELISA 方法耗费大量人力且成本高昂。随着越来越多的 HCP 被鉴定出低于可检测的定量水平,因此需要同时检测有选择性的目标 HCP。在此,我们开发了一种 Luminex 多路复用方法,它能在同一种检测方法中准确定量两种 "高风险 "脂肪酶--脂蛋白脂肪酶 (LPL) 和类磷脂酶 B 2 (PLBL2)。本研究概述了优化抗体构建、共轭比率、信号增强等参数的方法开发过程,以创建最高效的多重检测方法。因此,Luminex 多路复用法可提供与单路酶联免疫吸附法类似的结果,但速度更快,成本效益更高。这种方法可扩展到其他 "高风险 "HCP,并可用于未来的 HCP 监测应用。
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引用次数: 0
A visual electrochemiluminescence sensor based on the combination of distance-readout strategy and nanozymes catalyzing precipitation 基于读距策略和纳米催化沉淀相结合的可视电化学发光传感器
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-20 DOI: 10.1016/j.aca.2024.343355
Jiadong Zhang , Yanming Yang , Kexing Zhu , Yujiang Wang , Lijing Zhang , Xiangyu Ma , Nan Hao , Liangdong Feng , Yi Chen

Background

Nanozyme is a kind of biomimetic enzyme with unique properties and catalytic function of nanomaterials. Various nanozymes have been applied in the development of visual biosensors because of its excellent stability and availability. Nevertheless, the current applications of nanozymes primarily focus on colorimetric sensing based on color changes, which is susceptible to external factors interference including sample solution color and ambient light. Incorporating a distance-readout strategy with nanozymes presents a promising avenue for the advancement of innovative visual biosensing technologies in the future.

Results

A visual electrochemiluminescence (ECL) sensor was developed by combining the distance-readout strategy with nanozymes catalyzing precipitation for the first time. The detection is based on the ECL length change induced by nanozymes. This sensor chip comprises a square detection area and a visual ECL channel area. A peroxidase-mimic, core-shell hollow Fe3O4@PDA@ZIF-67, was modified in the detection region. The substrate 4-chloro-1-naphthol was rapidly catalyzed by nanozymes to form purple precipitate benzo-4-chlorohexanedione, leading to an increase in impedance within the detection region. Consequently, the detection area's partial voltage rose while the visual channel's dropped, resulting in a shorter ECL length. As a proof-of-concept experiment, the visual distance-readout ECL sensor was utilized for the quantitative detection of H2O2. The alteration in ECL length exhibited a good linear relationship with H2O2 concentration (logarithm) within the range of 300 nM to 300 μM, with the limit of detection (LOD) of 87 nM.

Significance

This work developed a novel approach for the application of nanozymes in analytical chemistry. Compared with common colorimetric sensing, this method is more convenient and intuitive, which can effectively eliminate potential interference from humans and the environment during signal acquisition. Because biocatalytic precipitation can be formed through multiple sensing processes, this strategy holds great promise as a portable and cost-effective tool with diverse applications.
背景纳米酶是一种具有独特性质和催化功能的纳米材料仿生酶。由于纳米酶具有极佳的稳定性和可用性,各种纳米酶已被应用于视觉生物传感器的开发。然而,目前纳米酶的应用主要集中在基于颜色变化的比色传感上,这很容易受到样品溶液颜色和环境光线等外部因素的干扰。将读取距离策略与纳米酶结合起来,为未来创新视觉生物传感技术的发展提供了一条大有可为的途径。结果 首次将读取距离策略与纳米酶催化沉淀相结合,开发出了一种视觉电化学发光(ECL)传感器。检测是基于纳米酶诱导的 ECL 长度变化。这种传感器芯片由一个正方形检测区和一个可视 ECL 通道区组成。在检测区内改性了过氧化物酶模拟物--核壳空心 Fe3O4@PDA@ZIF-67。底物 4-氯-1-萘酚在纳米酶的催化下迅速形成紫色沉淀苯并-4-氯己二酮,导致检测区域内阻抗增加。因此,检测区域的部分电压上升,而视觉通道的电压下降,导致 ECL 长度缩短。作为概念验证实验,视觉距离读出 ECL 传感器被用于定量检测 H2O2。在 300 nM 至 300 μM 范围内,ECL 长度的变化与 H2O2 浓度(对数)呈良好的线性关系,检测限(LOD)为 87 nM。与普通比色法相比,该方法更加方便直观,可有效排除信号采集过程中可能存在的人为和环境干扰。由于生物催化沉淀可通过多种传感过程形成,因此该策略有望成为一种便携式、经济高效的工具,具有广泛的应用前景。
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引用次数: 0
Dual-channel fluorescent probe for detecting SO2 and Hg2+, and dynamic imaging SO2 under Cd2+ in alfalfa (Medicago sativa) 用于检测紫花苜蓿(Medicago sativa)中 SO2 和 Hg2+,以及 Cd2+ 条件下 SO2 动态成像的双通道荧光探针
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-19 DOI: 10.1016/j.aca.2024.343353
Ya-Qian Wu , Xiang-Yu Wang , Tian-Wen Bai , Ying-Long Fu

Background

As an antioxidant, SO2 plays a critical role in maintaining the plant's redox balance. At the same time, Hg2+ as heavy metals, will accumulate in plants through soil, often disrupting physiological processes in plants. However, few studies have been reported to examine changes in Hg2+ and SO2 in plants. Here, we developed a dual-channel fluorescent probe NYD, which can differentiate between the detection of Hg2+ and SO2.

Results

The probe exhibits high sensitivity (LOD, 44 nM for Hg2+ and 26 nM for SO2). When Hg2+ and HSO3 deprotect and attack the double bond by nucleophilic addition, significant emission of fluorescence at 475 nm and 574 nm with blue and red fluorescence respectively. In addition, NYD has the capability to detect the levels of Hg2+ and SO2 in cells and alfalfa seedlings. Meanwhile, the findings indicated that alfalfa seedlings were exposed to Cd2+, which led to redox imbalance and increased endogenous SO2 production.

Significance

We anticipate that this research will contribute to a better understanding of the functions of SO2 under oxidative stress induced by Cd2+.
背景作为一种抗氧化剂,二氧化硫在维持植物的氧化还原平衡方面发挥着至关重要的作用。同时,作为重金属的 Hg2+ 会通过土壤在植物体内积累,往往会破坏植物的生理过程。然而,有关植物体内 Hg2+ 和 SO2 变化的研究报道很少。在此,我们开发了一种双通道荧光探针 NYD,它可以区分检测 Hg2+ 和 SO2。当 Hg2+ 和 HSO3- 通过亲核加成作用脱保护并攻击双键时,在 475 nm 和 574 nm 处分别会发出蓝色和红色荧光。此外,NYD 还能检测细胞和苜蓿幼苗中 Hg2+ 和 SO2 的含量。同时,研究结果表明,苜蓿幼苗暴露于 Cd2+ 后,氧化还原失衡,内源 SO2 生成增加。
{"title":"Dual-channel fluorescent probe for detecting SO2 and Hg2+, and dynamic imaging SO2 under Cd2+ in alfalfa (Medicago sativa)","authors":"Ya-Qian Wu ,&nbsp;Xiang-Yu Wang ,&nbsp;Tian-Wen Bai ,&nbsp;Ying-Long Fu","doi":"10.1016/j.aca.2024.343353","DOIUrl":"10.1016/j.aca.2024.343353","url":null,"abstract":"<div><h3>Background</h3><div>As an antioxidant, SO<sub>2</sub> plays a critical role in maintaining the plant's redox balance. At the same time, Hg<sup>2+</sup> as heavy metals, will accumulate in plants through soil, often disrupting physiological processes in plants. However, few studies have been reported to examine changes in Hg<sup>2+</sup> and SO<sub>2</sub> in plants. Here, we developed a dual-channel fluorescent probe NYD, which can differentiate between the detection of Hg<sup>2+</sup> and SO<sub>2</sub>.</div></div><div><h3>Results</h3><div>The probe exhibits high sensitivity (LOD, 44 nM for Hg<sup>2+</sup> and 26 nM for SO<sub>2</sub>). When Hg<sup>2+</sup> and HSO<sub>3</sub><sup>−</sup> deprotect and attack the double bond by nucleophilic addition, significant emission of fluorescence at 475 nm and 574 nm with blue and red fluorescence respectively. In addition, NYD has the capability to detect the levels of Hg<sup>2+</sup> and SO<sub>2</sub> in cells and alfalfa seedlings. Meanwhile, the findings indicated that alfalfa seedlings were exposed to Cd<sup>2+</sup>, which led to redox imbalance and increased endogenous SO<sub>2</sub> production.</div></div><div><h3>Significance</h3><div>We anticipate that this research will contribute to a better understanding of the functions of SO<sub>2</sub> under oxidative stress induced by Cd<sup>2+</sup>.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1332 ","pages":"Article 343353"},"PeriodicalIF":5.7,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Analytica Chimica Acta
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