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Speciation of selenium-containing small molecules in urine and cell lysate by CE-ICPMS with in-capillary enrichment. 利用毛细管内富集的 CE-ICPMS 对尿液和细胞裂解物中的含硒小分子进行定性。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-21 DOI: 10.1016/j.talanta.2024.126929
Yi Lu, Xue Men, Chengxin Wu, Xing Wei, Mingli Chen, Jianhua Wang

The quantitative speciation of selenium in biological systems is highly important for evaluating health status and elucidating transformations of Se species in physiological and pathological processes. Hyphenation of capillary electrophoresis with inductively coupled plasma mass spectrometry (CE-ICPMS) is promising for this purpose. However, the unfavorable or insufficient sensitivity for selenium analysis with CE-ICPMS seriously limits its practical applications in biological analysis, e.g., cell analysis. Therefore, it is crucial to improve the detection sensitivity for Se species. In this study, CE-ICPMS sensitivities for five selenium species (selenocystamine (SeA), methyl-2-acetamido-2-deoxy-1-seleno-β-d-galactopyranoside (SeSug 1), selenomethionine (SeMet), Se-Methylselenocysteine (MeSeCys) and selenocystine (SeCys)) were improved by in-capillary stacking via pH gradient between the zones of sample-leading buffer and the incorporation of isopropanol. The improvement on sensitivity of up to 9.9 folds was achieved in different biological samples, with LODs of 0.29-0.52 μg L-1. This approach was further applied for Se speciation in cell lysate, urine and culture medium. It showed that SeMet was more readily reduced in the medium and favorably accumulated by HepG2, HuH-7 and HCCLM3 cells with respect to SeSug 1 and MeSeCys. In cells, all the three Se species were largely transformed into other Se species. Furthermore, more than 70 % of SeMet reduced in medium was transformed into unknown Se species after 48-h interaction with cells.

生物系统中硒的定量分型对于评估健康状况以及阐明生理和病理过程中硒物种的转化非常重要。毛细管电泳与电感耦合等离子体质谱联用(CE-ICPMS)在这方面前景广阔。然而,用 CE-ICPMS 分析硒的灵敏度不高或不足,严重限制了其在生物分析(如细胞分析)中的实际应用。因此,提高硒的检测灵敏度至关重要。本研究采用毛细管内堆积法,在样品前缓冲液区之间进行 pH 梯度调节,并加入异丙醇,提高了对五种硒(硒囊胺(SeA)、甲基-2-乙酰氨基-2-脱氧-1-硒-β-d-吡喃半乳糖苷(SeSug 1)、硒蛋氨酸(SeMet)、硒甲基硒半胱氨酸(MeSeCys)和硒胱氨酸(SeCys))的检测灵敏度。不同生物样品的灵敏度提高了 9.9 倍,最低检测限为 0.29-0.52 μg L-1。这种方法还被进一步应用于细胞裂解物、尿液和培养基中的硒离子。结果表明,与 SeSug 1 和 MeSeCys 相比,SeMet 更容易在培养基中被还原,并有利于 HepG2、HuH-7 和 HCCLM3 细胞的积累。在细胞中,所有三种 Se 在很大程度上都转化成了其他 Se。此外,与细胞作用 48 小时后,培养基中减少的 SeMet 有超过 70% 转化为未知的 Se 物种。
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引用次数: 0
Specific isolation and quantification of PD-L1 positive tumor derived exosomes for accurate breast cancer discrimination via aptamer-functionalized magnetic composites and SERS immunoassay. 通过aptamer功能化磁性复合材料和SERS免疫测定,特异性分离和定量PD-L1阳性肿瘤外泌体,以准确鉴别乳腺癌。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-25 DOI: 10.1016/j.talanta.2024.126956
Ning Su, Jin Zhang, Wei Liu, Haoyang Zheng, Mengran Li, Jiandong Zhao, Mingxia Gao, Xiangmin Zhang

PD-L1 positive tumor derived exosomes (TEXsPD-L1) play a significant role in disease progression, tumor metastasis and cancer immunotherapy. However, the overlap of PD-L1 between TEXs and non-tumor derived exosomes (non-TEXs) restricts the specific isolation and quantification of TEXPD-L1 from clinical samples. Herein, a new aptamer-functionalized and hydrophilic immunomagnetic substrate was designed by decorating generation 5 polyamidoamine dendrimers (G5 PAMAM), zwitterionic trimethylamine N-oxide (TMAO) and EpCAM (Epithelial cell adhesion molecule) aptamers on magnetic cores sequentially (Fe3O4@PAMAM@TMAO@Aptamer, named as FPTA) for rapid target and efficient capture of TEXs. The FPTA substrate gathered excellent characters of strong magnetic responsiveness of Fe3O4, abundant affinity sites of PAMAM, strong hydrophilicity of TMAO and enhanced affinity properties of EpCAM aptamers. Because of these advantages, FPTA can isolate TEXs quickly within 30min with high capture efficiency of 90.5 % ± 3.0 % and low nonspecific absorption of 8.2 % ± 2.0 % for non-TEXs. Furthermore, PD-L1 (Programmed cell death-ligand 1) positive TEXs (TEXsPD-L1) from the captured TEXs were recognized and quantitatively analyzed by utilizing SERS (surface-enhanced Raman spectroscopy) reporter molecules 4-NTP (4-Nitrothiophenol) on PD-L1 aptamers-functionalized gold immunoaffinity probe. The signal of TEXsPD-L1 was converted to SERS signal of 4-NTP at 1344 cm-1 which exhibited a linear correlation to concentration of TEXsPD-L1(R2 = 0.9905). With these merits, this strategy was further applied to clinical plasma samples from breast cancer (BC) patients and healthy controls (HC), exhibited an excellent diagnosis accuracy with area under curve (AUC) of receiver operating characteristic (ROC) curve reaching 0.988. All these results demonstrate that the FPTA immunomagnetic substrate combined with SERS immunoaffinity probe may become a generic tool for specific isolation and quantitative analysis of PD-L1 positive tumor-derived exosomes in clinics.

PD-L1 阳性的肿瘤衍生外泌体(TEXsPD-L1)在疾病进展、肿瘤转移和癌症免疫疗法中发挥着重要作用。然而,PD-L1在TEXs和非肿瘤衍生外泌体(非TEXs)之间的重叠限制了从临床样本中特异性分离和定量TEXPD-L1。在此,我们设计了一种新的合子功能化亲水免疫磁性基底,将第5代聚氨基胺树枝状聚合物(G5 PAMAM)、齐聚三甲胺N-氧化物(TMAO)和EpCAM(上皮细胞粘附分子)合子依次装饰在磁芯上(Fe3O4@PAMAM@TMAO@合子,命名为FPTA),用于快速靶向和高效捕获TEXs。FPTA基底具有Fe3O4的强磁响应性、PAMAM的丰富亲和位点、TMAO的强亲水性和EpCAM适配体的增强亲和性等优良特性。由于这些优势,FPTA 可在 30 分钟内快速分离出 TEX,捕获效率高达 90.5% ± 3.0%,非特异性吸收率低至 8.2% ± 2.0%。此外,利用表面增强拉曼光谱(SERS)报告分子4-NTP(4-Nitrothiophenol)在PD-L1适配体功能化金免疫亲和探针上识别并定量分析了捕获的TEXs中的PD-L1(Programmed cell death-ligand 1,程序性细胞死亡配体1)阳性TEXs(TEXsPD-L1)。TEXsPD-L1 的信号被转换成 4-NTP 在 1344 cm-1 处的 SERS 信号,该信号与 TEXsPD-L1 的浓度呈线性相关(R2 = 0.9905)。鉴于上述优点,该方法被进一步应用于乳腺癌(BC)患者和健康对照组(HC)的临床血浆样本,显示出极佳的诊断准确性,接收者操作特征曲线(ROC)的曲线下面积(AUC)达到 0.988。所有这些结果表明,FPTA免疫磁性底物与SERS免疫亲和探针相结合可成为临床上特异性分离和定量分析PD-L1阳性肿瘤外泌体的通用工具。
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引用次数: 0
Dual-emission carbon dots-based biosensor for polarity/targeting bimodal recognition and mild photothermal therapy of tumor. 基于双发射碳点的生物传感器,用于极性/靶向双模识别和肿瘤的温和光热疗法。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-16 DOI: 10.1016/j.talanta.2024.127060
Xiaorui Dong, Wenjun Yan, Dongmei Zhang, Ruihan Wang, Liuyan Xue, Heping Shi, Yingqi Li

It is essential to develop a multifunctional nanoplatform for biosensing, tumor diagnosis and treatment simultaneously. Herein, dual-emission fluorescent carbon dots (HA-CDs) were fabricated via a one-pot solvothermal method using spinach powder as carbon source and hyaluronic acid (HA) as targeting agent. The obtained HA-CDs exhibited outstanding optical properties, good targeted tumor and excellent photothermal conversion performance. Interestingly, HA-CDs can sensitively perceive the changes in polar environments attributed to the inherent ratiometric fluorescence characteristics, and combined with the intrinsic targeting tumor ability achieved tumor cell recognition. More importantly, the HA-CDs possess good photothermal conversion efficiency of 21.2 % to be beneficial for photothermal therapy of tumors. The survival rate of HeLa cells incubated with HA-CDs dramatically decreased to 14 % after 660 nm laser irradiation, revealing the significant tumor inhibition of HA-CDs in vitro. Notably, through individual intraperitoneal and intratumoral injection, it was found that HA-CDs demonstrated a similar tumor suppressed effect on 4T1 tumor-bearing mice exposed to laser irradiation, fully uncovering that HA-CDs can efficiently accumulate at tumor site by intraperitoneal injection. Besides, the histopathological analysis of major organs ex vivo revealed a good biosafety profile. Collectively, this strategy of designed HA-CDs provides a new multifunctional nanoplatform for potential clinical application.

开发一种同时用于生物传感、肿瘤诊断和治疗的多功能纳米平台至关重要。本文以菠菜粉为碳源,透明质酸(HA)为靶向剂,通过一锅溶热法制备了双发射荧光碳点(HA-CDs)。所制备的 HA-CDs 具有优异的光学特性、良好的肿瘤靶向性和光热转换性能。有趣的是,HA-CDs能灵敏地感知极地环境的变化,这得益于其固有的比率荧光特性,并与内在的肿瘤靶向能力相结合,实现了对肿瘤细胞的识别。更重要的是,HA-CDs 具有良好的光热转换效率(21.2%),有利于肿瘤的光热治疗。经 660 纳米激光照射后,与 HA-CDs 一起培养的 HeLa 细胞存活率急剧下降至 14%,显示了 HA-CDs 在体外对肿瘤的显著抑制作用。值得注意的是,通过单独腹腔注射和瘤内注射发现,HA-CDs 对接受激光照射的 4T1 肿瘤小鼠也有类似的抑瘤作用,充分揭示了 HA-CDs 通过腹腔注射可在肿瘤部位有效蓄积。此外,体内主要器官的组织病理学分析表明,HA-CDs 具有良好的生物安全性。总之,这种设计HA-CDs的策略为潜在的临床应用提供了一种新的多功能纳米平台。
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引用次数: 0
Preparation of a V-COF@SWCNTs-COOH/SPCE supported molecularly imprinted electrochemical sensor for real-time detection of trace sulfadimidine. 制备用于实时检测痕量磺胺二甲嘧啶的 V-COF@SWCNTs-COOH/SPCE 分子印迹电化学传感器。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-15 DOI: 10.1016/j.talanta.2024.127046
Shuomeng Bai, Tingting Yang, Peiqiao Liu, Junhua Tan, Shuixie Chen, Hongtao Lei, Xiaoqun Wei

To overcome the limitations of insufficient sensitivity and poor specificity of portable screen-printed carbon electrode-electrochemical sensors (SPCE-EC) in practical applications, we prepared carrier composites of carboxylic single-walled carbon nanotubes vertically grafted by covalent organic frameworks (v-COF@SWCNTs-COOH) and coated with a molecularly imprinted polymer (MIP) of sulfadimidine (SM2). 55 °C hot steam elution is more eco-friendly than traditional organic solvent elution. The results showed that when the mass ratio of DBA to DBA-SWCNTs was 1:1, the v-COF@SWCNTs-COOH obtained by the two-step synthesis method could increase the electrical signal up to 2.33-fold of the bare electrode. The bifunctional monomer MIP prepared on the above structure enhanced the signal response by 2.91-fold, with a high imprint factor of 20. The assembled MIP/v-COF@SWCNTs-COOH/SPCE were analyzed by differential pulse voltammetry (DPV) with a high sensitivity of 0.21 nM for LOD and 0.70 nM for LOQ. In milk and fish samples, the recovery rate was 95.0 %-104.8 %. The validation of authentic pork samples with the statutory LC-MS/MS method showed no significant difference (P > 0.05). The sensor's performance indicators remained robust after five repeated uses. Therefore, the MIP/v-COF@SWCNTs-COOH/SPCE combines the cheapness and portability of SPCE, while the sensitivity and specificity of small molecule detection were significantly improved.

为了克服便携式丝网印刷碳电极电化学传感器(SPCE-EC)在实际应用中灵敏度不足和特异性差的局限性,我们制备了共价有机框架垂直接枝的羧基单壁碳纳米管(v-COF@SWCNTs-COOH)载体复合材料,并在其表面涂覆了磺胺二甲嘧啶(SM2)分子印迹聚合物(MIP)。55 °C 热蒸汽洗脱比传统的有机溶剂洗脱更环保。结果表明,当 DBA 与 DBA-SWCNTs 的质量比为 1:1 时,两步合成法得到的 v-COF@SWCNTs-COOH 可使电信号增加到裸电极的 2.33 倍。在上述结构上制备的双功能单体 MIP 将信号响应提高了 2.91 倍,印记因子高达 20。通过差分脉冲伏安法(DPV)对组装好的 MIP/v-COF@SWCNTs-COOH/SPCE 进行分析,灵敏度很高,LOD 为 0.21 nM,LOQ 为 0.70 nM。在牛奶和鱼肉样品中,回收率为 95.0 %-104.8 %。用法定的 LC-MS/MS 方法对真实的猪肉样品进行验证,结果显示两者无显著差异(P > 0.05)。该传感器的性能指标在重复使用五次后仍然保持稳定。因此,MIP/v-COF@SWCNTs-COOH/SPCE 集 SPCE 的廉价性和便携性于一身,同时显著提高了小分子检测的灵敏度和特异性。
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引用次数: 0
PyICLab: An integrated Python-based toolkit for in-silico simulations of ion chromatography. PyICLab:基于 Python 的集成工具包,用于离子色谱法的内部模拟。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-15 DOI: 10.1016/j.talanta.2024.127054
Kai Zhang, Yule Qian, Chaoyan Lou, Mingli Ye, Yan Zhu

PyICLab is an open-source Python-based package featuring an object-oriented programming (OOP) interface, providing tools for realistic and customized numerical simulations of ion chromatography (IC). In this paper, we showcase PyICLab's use in simulating diverse separation scenarios, including isocratic carbonate elution, gradient hydroxide elution, high-concentration and large-volume injections. The accuracy of the embedded models was validated by demonstrating strong correlations between predicted and experimental results. Additionally, PyICLab's capability to handle complex IC configurations was demonstrated through a simulation of a column-switching system for seawater analysis. PyICLab offers valuable resources for chromatographic optimization, method development, and educational purposes. It is available on PyPI at pypi.org/project/pyIClab. Interested readers can install PyICLab using the pip command in a Python 3.11 or higher environment.

PyICLab 是一个基于 Python 的开源软件包,具有面向对象编程(OOP)界面,为离子色谱(IC)的逼真和定制化数值模拟提供了工具。在本文中,我们展示了 PyICLab 在模拟各种分离场景中的应用,包括等度碳酸盐洗脱、梯度氢氧化物洗脱、高浓度和大体积进样。通过证明预测结果与实验结果之间的强相关性,验证了嵌入模型的准确性。此外,PyICLab 处理复杂集成电路配置的能力还通过模拟用于海水分析的色谱柱切换系统得到了验证。PyICLab 为色谱优化、方法开发和教育目的提供了宝贵的资源。它可从 PyPI 上获取,网址是 pypi.org/project/pyIClab。感兴趣的读者可以在 Python 3.11 或更高版本的环境中使用 pip 命令安装 PyICLab。
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引用次数: 0
Copper ions coordination-promoted self-assembly of DNA nanoflowers as cascade catalytic nanoreactor for colorimetric biosensor. 铜离子配位促进 DNA 纳米花的自组装,作为比色生物传感器的级联催化纳米反应器。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-10-15 DOI: 10.1016/j.talanta.2024.127049
Zhenjie Qiao, Shuzhen Yue, Xiaoyue Zhang, Pengfei Shi, Shuzhen Lv, Sai Bi

The controllable geometry and multifunctionality of DNA nano-bioreactors hold immense promise for disease diagnosis. Herein, a facile rolling circle amplification (RCA)-based crystallization method has been developed for highly efficient self-assembly of three-dimensional (3D) DNA nano-bioreactors, which show excellent cascade catalytic performance by confining bio-enzyme (glucose oxidase (GOx) used in this case) and copper ions (Cu2+) in DNA nanoflowers (DNFs) structure. The participation of Cu2+ during the self-assembly process not only endows the nano-bioreactors (designated as GOx/Cu@DNFs) with inspiring peroxidase-like activity but also greatly improves the assembly efficiency and yield via the effective coordination between Cu2+ and RCA-generated long concatemeric DNAs. The integration of GOx and Cu2+ in the constrained flower-like DNA nanomatrices makes for the efficient inter-catalyst communication, resulting in the striking enhancement of biocatalytic cascade activity. Based on the prepared nano-bioreactors, a colorimetric biosensor has been constructed for glucose detection, achieving a wide linear range (2-400 μM) and a low detection limit (0.45 μM). Furthermore, the proposed sensing strategy enables the accurate determination and discrimination of glucose levels in healthy and diabetic sera, delivering gratifying outcomes. Overall, the meticulously crafted cascade nano-bioreactors not only illuminate the design of multifunctional nanomaterials based on RCA, but also expand the conceptual framework of the universal analytical method for determining small molecules with catalytic reactions to generate H2O2.

DNA 纳米生物反应器的可控几何形状和多功能性为疾病诊断带来了巨大前景。在此,我们开发了一种基于滚圆放大(RCA)的简便结晶方法,用于高效自组装三维(3D)DNA 纳米生物反应器,这种反应器通过将生物酶(本例中使用的是葡萄糖氧化酶(GOx))和铜离子(Cu2+)限制在 DNA 纳米花(DNFs)结构中,显示出卓越的级联催化性能。Cu2+ 在自组装过程中的参与不仅赋予了纳米生物反应器(命名为 GOx/Cu@DNFs)鼓舞人心的过氧化物酶样活性,而且通过 Cu2+ 与 RCA 生成的长连接 DNA 之间的有效配位,大大提高了组装效率和产量。GOx 和 Cu2+ 在受约束的花朵状 DNA 纳米结构中的整合使得催化剂之间可以进行有效的交流,从而显著提高了生物催化级联活性。基于制备的纳米生物反应器,构建了一种用于葡萄糖检测的比色生物传感器,实现了宽线性范围(2-400 μM)和低检测限(0.45 μM)。此外,所提出的传感策略还能准确测定和区分健康血清和糖尿病血清中的葡萄糖水平,结果令人满意。总之,精心制作的级联纳米生物反应器不仅阐明了基于 RCA 的多功能纳米材料的设计,还拓展了利用催化反应生成 H2O2 来测定小分子的通用分析方法的概念框架。
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引用次数: 0
Achieving precise dual detection: One-tube reverse transcription-recombinase aided amplification (RT-RAA) combined with lateral flow strip (LFS) assay for RNA and DNA target genes from pepper mild mottle virus and Colletotrichum species in crude plant samples. 实现精确的双重检测:单管反转录-重组酶辅助扩增(RT-RAA)结合侧流条带(LFS)检测植物粗样品中辣椒轻度斑驳病病毒和壳斗孢菌的 RNA 和 DNA 目标基因。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-18 DOI: 10.1016/j.talanta.2024.126908
Yuhao Cao, Dankan Yan, Huijie Zhou, Kelei Han, Qionglian Wan, Jiejun Peng, Hongying Zheng, Lin Lin, Fei Yan, Xuemei Song

Ensuring the detection sensitivity of both RNA-derived and DNA-derived target genes in a single reaction has posed a significant challenge for on-site detection of plant pathogens. This challenge was addressed by developing a one-tube dual RT-RAA assay combined with LFS for the rapid on-site detection of pepper mild mottle virus (PMMoV) and four Colletotrichum species causing anthracnose in Solanaceous crops. By testing four different combinations of primer groups, two combinations were precisely adjusted within the dual RT-RAA system to balance amplification efficiency and maintain consistent levels of amplification in crude plant samples. Utilizing commercially accessible small-scale equipment and following a streamlined optimization strategy, the assay achieved a limit of detection of 0.32 copies/μL of target genes in the reaction. Importantly, it demonstrated no cross-reactivity with other plant pathogens, thereby affirming the high sensitivity and specificity of the developed dual RT-RAA-LFS detection assay. Moreover, the entire process took only 25 min from sample collection to the visible presentation of results. The assay was validated with 60 field samples and 10 seed samples, producing results consistent with reverse transcription quantitative polymerase chain reaction (RT-qPCR). Notably, it successfully detected PMMoV in systemic leaves without visible symptoms three days post-inoculation, underscoring its effectiveness in early disease detection. This streamlined strategy offers a valuable approach for rapid, low-cost, and highly sensitive on-site simultaneous detection of RNA genome-contained PMMoV and DNA genome-contained Colletotrichum species.

在单一反应中确保 RNA 衍生和 DNA 衍生目标基因的检测灵敏度是现场检测植物病原体的一大挑战。为解决这一难题,我们开发了一种结合 LFS 的单管双 RT-RAA 检测法,用于现场快速检测辣椒轻度斑驳病毒(PMMoV)和引起茄科作物炭疽病的四种 Colletotrichum 菌。通过测试四组不同的引物组合,在双 RT-RAA 系统中精确调整了两组引物组合,以平衡扩增效率,并在粗植物样本中保持稳定的扩增水平。利用市场上可买到的小型设备,并遵循简化的优化策略,该检测方法在反应中实现了 0.32 拷贝/μL 的目标基因检测限。重要的是,它与其他植物病原体没有交叉反应,从而证实了所开发的 RT-RAA-LFS 双检测方法的高灵敏度和特异性。此外,从样本采集到结果显现,整个过程只需 25 分钟。60 份田间样本和 10 份种子样本对该检测方法进行了验证,结果与反转录定量聚合酶链反应(RT-qPCR)一致。值得注意的是,它在接种后三天成功地检测到了无明显症状的系统叶片中的 PMMoV,这突出表明了它在早期病害检测中的有效性。这一简化策略为快速、低成本、高灵敏度地现场同时检测含 RNA 基因组的 PMMoV 和含 DNA 基因组的 Colletotrichum 菌种提供了宝贵的方法。
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引用次数: 0
Fluorescence of europium activated by molecular-like silver clusters for the detection of alkaline phosphatase activity. 用于检测碱性磷酸酶活性的分子样银簇激活的铕荧光。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-16 DOI: 10.1016/j.talanta.2024.126892
Chen-Xi Zhao, Xiao-Xia Li, Yang Shu

Alkaline phosphatase (ALP) is abnormally expressed in some cancers and promotes the growth, metastasis, and invasion of cancer cells. The detection of ALP is of great significance for both pathological study and clinical detection. In this work, a europium (Eu)-based fluorescence detection sensor was prepared in a mild reaction condition. LaF3:Eu nanoparticles was mixed with ethylene imine polymer (PEI) and Ag+ ions. PEI was used as stabilizer and reducing agent, and Ag+ ions were reduced as molecular-like silver clusters (ML-Ag NCs). The fluorescence of LaF3:Eu nanoparticles was enhanced by ML-Ag NCs through energy transfer. When ascorbic acid 2-phosphate (AAP) was hydrolyzed to ascorbic acid (AA) in the presence of ALP, AA reduced Ag+ ions to silver nanoparticles (Ag NPs) and quenched the fluorescence of LaF3:Eu/PEI/Ag. The activity of ALP was detected by measuring the fluorescence intensity of Eu3+ at 618 nm. In the concentration range from 2.0 to 16.0 U/L, the fluorescence intensity ratio ((F0-F)/F0) had a linear relationship with the logarithm of ALP concentration. The limit of detection (LOD) was 1.3 U/L. Moreover, the ALP activity was detected successfully in cancer cells by this method. The sensing platform has application potential in the detection of ALP activity in biological systems.

碱性磷酸酶(ALP)在某些癌症中表达异常,会促进癌细胞的生长、转移和侵袭。检测 ALP 对病理研究和临床检测都具有重要意义。本研究在温和的反应条件下制备了一种基于铕(Eu)的荧光检测传感器。LaF3:Eu 纳米粒子与乙烯亚胺聚合物(PEI)和 Ag+ 离子混合。PEI 用作稳定剂和还原剂,Ag+ 离子被还原成分子样银簇(ML-Ag NCs)。通过能量转移,ML-Ag NCs 增强了 LaF3:Eu 纳米粒子的荧光。当抗坏血酸 2-磷酸(AAP)在 ALP 存在下水解为抗坏血酸(AA)时,AA 将 Ag+ 离子还原为银纳米颗粒(Ag NPs),并淬灭了 LaF3:Eu/PEI/Ag 的荧光。通过测量 618 纳米波长处 Eu3+ 的荧光强度来检测 ALP 的活性。在 2.0 至 16.0 U/L 的浓度范围内,荧光强度比((F0-F)/F0)与 ALP 浓度的对数呈线性关系。检测限(LOD)为 1.3 U/L。此外,该方法还能成功检测出癌细胞中的 ALP 活性。该传感平台在检测生物系统中的 ALP 活性方面具有应用潜力。
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引用次数: 0
Multipath collaboration-based signal amplification on Z-scheme In2O3/g-C3N4 heterojunction photoelectrode for sensitive photoelectrochemical immunoassay. 在 Z 型 In2O3/g-C3N4 异质结光电电极上进行基于多径协作的信号放大,用于灵敏的光电化学免疫分析。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-23 DOI: 10.1016/j.talanta.2024.126935
Yuxiang Dong, Weisa Wang, Cheng Guo, Jialin Wang, Dan Li, Changqing Ye

The ideal photoelectrode and efficient signaling strategy are pivotal to achieve sensitive photoelectrochemical (PEC) analysis. Here, a multipath collaborative signal amplification-based PEC immunosensor was constructed for the ultrasensitive detection of cytokeratin 19 fragment 21-1. Specifically, the photoelectrode fabricated by Z-scheme In2O3/g-C3N4 heterojunction showed enhanced photocurrent intensity in response to visible light. Meanwhile, the signal probe, horseradish peroxidase functionalized dopamine-melanin nanosphere@Au nanoparticles (HRP-Dpa-melanin NS@AuNPs), were introduced into the system. When the target exists, the signal probe can induce multiple quenching of the photocurrent due to the competition of light absorption, steric hindrance and HRP-mediated biocatalytic precipitation, which effectively inhibit light, electron donor, and electron access to the photoelectrode. The fabricated immunosensor exhibits a wide linear range from 1.0 × 10-3 - 1.0 × 102 ng mL-1 with the detection limit of 0.35 pg mL-1 (S/N = 3) for cytokeratin 19 fragment 21-1 detection. The study enhances sensitivity for PEC detection by utilizing the superior Z-scheme heterojunction photoelectrode, providing a valuable method that combines multiple signal pathways for a synergistic effect in bioanalysis.

理想的光电电极和高效的信号策略是实现灵敏的光电化学(PEC)分析的关键。本文构建了一种基于多路径协同信号放大的 PEC 免疫传感器,用于超灵敏检测细胞角蛋白 19 片段 21-1。具体来说,由 Z 型 In2O3/g-C3N4 异质结制成的光电极在可见光下显示出更强的光电流强度。同时,将信号探针--辣根过氧化物酶功能化多巴胺-美兰宁纳米球@金纳米粒子(HRP-Dpa-美兰宁 NS@AuNPs)引入该系统。当目标物存在时,由于光吸收、立体阻碍和 HRP 介导的生物催化沉淀的竞争,信号探针可诱导光电流的多重淬灭,从而有效抑制光、电子供体和电子进入光电极。所制备的免疫传感器在 1.0 × 10-3 - 1.0 × 102 ng mL-1 范围内具有较宽的线性,细胞角蛋白 19 片段 21-1 的检测限为 0.35 pg mL-1 (S/N = 3)。该研究通过利用卓越的 Z 型异质结光电电极提高了 PEC 检测的灵敏度,提供了一种结合多种信号途径的有价值的方法,从而在生物分析中产生协同效应。
{"title":"Multipath collaboration-based signal amplification on Z-scheme In<sub>2</sub>O<sub>3</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction photoelectrode for sensitive photoelectrochemical immunoassay.","authors":"Yuxiang Dong, Weisa Wang, Cheng Guo, Jialin Wang, Dan Li, Changqing Ye","doi":"10.1016/j.talanta.2024.126935","DOIUrl":"10.1016/j.talanta.2024.126935","url":null,"abstract":"<p><p>The ideal photoelectrode and efficient signaling strategy are pivotal to achieve sensitive photoelectrochemical (PEC) analysis. Here, a multipath collaborative signal amplification-based PEC immunosensor was constructed for the ultrasensitive detection of cytokeratin 19 fragment 21-1. Specifically, the photoelectrode fabricated by Z-scheme In<sub>2</sub>O<sub>3</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction showed enhanced photocurrent intensity in response to visible light. Meanwhile, the signal probe, horseradish peroxidase functionalized dopamine-melanin nanosphere@Au nanoparticles (HRP-Dpa-melanin NS@AuNPs), were introduced into the system. When the target exists, the signal probe can induce multiple quenching of the photocurrent due to the competition of light absorption, steric hindrance and HRP-mediated biocatalytic precipitation, which effectively inhibit light, electron donor, and electron access to the photoelectrode. The fabricated immunosensor exhibits a wide linear range from 1.0 × 10<sup>-3</sup> - 1.0 × 10<sup>2</sup> ng mL<sup>-1</sup> with the detection limit of 0.35 pg mL<sup>-1</sup> (S/N = 3) for cytokeratin 19 fragment 21-1 detection. The study enhances sensitivity for PEC detection by utilizing the superior Z-scheme heterojunction photoelectrode, providing a valuable method that combines multiple signal pathways for a synergistic effect in bioanalysis.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126935"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338761","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Novel electrochemiluminescence platform utilizing AuNPs@Uio-66-NH2 bridged luminescent substrates and aptamers for the detection of pesticide residues in Chinese herbal medicines. 利用 AuNPs@Uio-66-NH2 桥接发光底物和适配体的新型电化学发光平台检测中药材中的农药残留。
IF 5.6 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-01-01 Epub Date: 2024-09-20 DOI: 10.1016/j.talanta.2024.126924
Chengqiang Li, Haifang Wang, Jiashuai Sun, Peisen Li, Jiwei Dong, Jingcheng Huang, Haowei Dong, Lingjun Geng, Zhiping Yu, Pengwei Zhang, Wei Chen, Yemin Guo, Xia Sun

A large number of Chinese herbal medicines (CHMs) are included in daily recipes, but their pesticide residues have aroused more and more concerns. In this paper, an electrochemiluminescence aptasensor was constructed for the trace detection of acetamiprid (ACE) in Angelica sinensis and Lycium barbarum. Possessing a large specific surface area, UiO-66 was modified with amino groups to improve biocompatibility, and the addition of AuNPs allowed UiO-66-NH2 to catalyze the formation of excited states of luminescent molecules (TPrA; Ru(bpy)32+), and AuNPs@UiO-66-NH2 was used to bridge the aptamer (Au-S) and luminescent substrate (peptide bond). The conventional luminescent reagent Ru(bpy)32+ was doped with multi-walled carbon nanotubes (MWCNTs) to obtain a more powerful and stable light signal. After optimizing the experimental parameters, the aptasensor could give results in 10 min with a detection range from 1×10-2-1×104 nM and a lower limit of detection (LOD) of 0.8 pM. The LOD of the study was at least one order of magnitude lower than that of the fluorescence detection method. Furthermore, the accuracy of the aptasensor was validated for spiked recovery experiments.

大量中药材被列入日常食谱,但其农药残留问题日益引起人们的关注。本文构建了一种电化学发光适配传感器,用于痕量检测当归和枸杞中的啶虫脒(ACE)。UiO-66 具有较大的比表面积,用氨基修饰可提高其生物相容性,加入 AuNPs 可使 UiO-66-NH2 催化发光分子(TPrA⁎;Ru(py)32+⁎)激发态的形成,AuNPs@UiO-66-NH2 则用于连接适配体(Au-S)和发光底物(肽键)。在传统的发光试剂 Ru(bpy)32+ 中掺杂了多壁碳纳米管(MWCNTs),以获得更强更稳定的光信号。优化实验参数后,该传感器可在 10 分钟内得到结果,检测范围为 1×10-2-1×104 nM,检测下限(LOD)为 0.8 pM。该研究的检测下限比荧光检测方法至少低一个数量级。此外,在加标回收实验中也验证了该传感器的准确性。
{"title":"Novel electrochemiluminescence platform utilizing AuNPs@Uio-66-NH<sub>2</sub> bridged luminescent substrates and aptamers for the detection of pesticide residues in Chinese herbal medicines.","authors":"Chengqiang Li, Haifang Wang, Jiashuai Sun, Peisen Li, Jiwei Dong, Jingcheng Huang, Haowei Dong, Lingjun Geng, Zhiping Yu, Pengwei Zhang, Wei Chen, Yemin Guo, Xia Sun","doi":"10.1016/j.talanta.2024.126924","DOIUrl":"10.1016/j.talanta.2024.126924","url":null,"abstract":"<p><p>A large number of Chinese herbal medicines (CHMs) are included in daily recipes, but their pesticide residues have aroused more and more concerns. In this paper, an electrochemiluminescence aptasensor was constructed for the trace detection of acetamiprid (ACE) in Angelica sinensis and Lycium barbarum. Possessing a large specific surface area, UiO-66 was modified with amino groups to improve biocompatibility, and the addition of AuNPs allowed UiO-66-NH<sub>2</sub> to catalyze the formation of excited states of luminescent molecules (TPrA<sup>⁎</sup>; Ru(bpy)<sub>3</sub><sup>2+</sup><sup>⁎</sup>), and AuNPs@UiO-66-NH<sub>2</sub> was used to bridge the aptamer (Au-S) and luminescent substrate (peptide bond). The conventional luminescent reagent Ru(bpy)<sub>3</sub><sup>2+</sup> was doped with multi-walled carbon nanotubes (MWCNTs) to obtain a more powerful and stable light signal. After optimizing the experimental parameters, the aptasensor could give results in 10 min with a detection range from 1×10<sup>-2</sup>-1×10<sup>4</sup> nM and a lower limit of detection (LOD) of 0.8 pM. The LOD of the study was at least one order of magnitude lower than that of the fluorescence detection method. Furthermore, the accuracy of the aptasensor was validated for spiked recovery experiments.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"281 ","pages":"126924"},"PeriodicalIF":5.6,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142338762","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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Talanta
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