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Recent progress of DNAzyme-based biosensors for pathogen detection 基于 DNA 酶的病原体检测生物传感器的最新进展
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-24 DOI: 10.1039/d4ay00934g
Heng Xiao, Xingxing Liu, Wenxu Yuan
More pathogens endanger food safety, agricultural productivity, and human health. Many are spread through direct/indirect contact, airborne transmission and food/waterborne transmission, some with severe health consequences. As the population grows and global connections intensify, the transmission of infectious diseases expands. Existing detection methods of pathogen still have some shortcomings, such as time-consuming and operational costs. To fulfil the demands of simple and effective detection, numerous biosensors have been developed. DNAzyme, as a unique DNA structure with catalytic activity, is gradually being applied in the field of pathogen detection due to its ease of preparation and use. In this review, we concentrated on the two main kinds of DNAzyme, hemin/G-quadruplex DNAzyme (HGD) and RNA-cleaving DNAzyme (RCD), explaining its research progress in pathogen detection. Furthermore, we introduced two additional novel DNAzyme, CLICK 17 DNAzyme and Supernova DNAzyme, which showed promising potential in pathogen detection. In the end, we summarized the strengths and weaknesses of these four DNAzyme and offer feasible recommendations for the development of biosensors.
更多的病原体危及食品安全、农业生产力和人类健康。许多病原体通过直接/间接接触、空气传播和食物/水传播等途径传播,其中一些会造成严重的健康后果。随着人口的增长和全球联系的加强,传染病的传播范围也在扩大。现有的病原体检测方法仍存在一些缺点,如耗时长、操作成本高。为了满足简单有效的检测要求,人们开发了许多生物传感器。DNA 酶作为一种具有催化活性的独特 DNA 结构,因其易于制备和使用,逐渐被应用于病原体检测领域。在这篇综述中,我们主要介绍了两种主要的 DNA 酶,即 hemin/G-quadruplex DNA 酶(HGD)和 RNA-cleaving DNA 酶(RCD),并解释了其在病原体检测方面的研究进展。此外,我们还介绍了另外两种新型 DNA 酶:CLICK 17 DNA 酶和 Supernova DNA 酶,它们在病原体检测方面具有广阔的应用前景。最后,我们总结了这四种DNA酶的优缺点,并对生物传感器的开发提出了可行性建议。
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引用次数: 0
An electrochemical H2S sensor based on screen printing Fe@Pt/C/PTFE sensing electrode 基于丝网印刷 Fe@Pt/C/PTFE 传感电极的电化学 H2S 传感器
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-24 DOI: 10.1039/d4ay00657g
Dandan Liu, Xukun Deng, Chunhui Du, Lu Zheng, Yanting Guo, Yanmei Cheng, Guangming Nie
A novel electrochemical gas sensor for sensitive detection of H2S at room temperature is constructed based on Fe@Pt/C composite material. The core-shell structured Fe@Pt catalyst was synthesized by two-step reduction method and physically dispersed in Vulcan XC-72 carbon powders. The core-shell structure increases the effective catalytic surface area of Pt while significantly reducing the usage of the noble metal Pt, leading to improved catalytic performance and decreased production costs. Additionally, the mature screen-printing process is used to coat the catalyst film. Waterproof and breathable PTFE film was used as substrate and the parameters in the screen printing process were also optimized to achieve the best gas sensing performance of the electrode film. Through the detection of hydrogen sulfide (H2S) with different concentrations, it is found that the sensor strictly performs linear correlation in the range of 1-20 ppm, R2=0.99974. Notably, the sensor exhibits high sensitivity (658.45 nA/ppm) and the low detection limit of 0.33 ppm. Moreover, the consistency and stability of the sensor are satisfactory. The constructed gas sensor is expected to be well applied to industrial H2S detection.
基于 Fe@Pt/C 复合材料构建了一种新型电化学气体传感器,可在室温下灵敏检测 H2S。通过两步还原法合成了核壳结构的 Fe@Pt 催化剂,并将其物理分散在 Vulcan XC-72 碳粉中。核壳结构增加了铂的有效催化表面积,同时大大减少了贵金属铂的用量,从而提高了催化性能,降低了生产成本。此外,催化剂薄膜还采用了成熟的丝网印刷工艺。采用防水透气的聚四氟乙烯薄膜作为基底,并对丝网印刷工艺参数进行了优化,以实现电极薄膜的最佳气体传感性能。通过检测不同浓度的硫化氢(H2S),发现该传感器在 1-20 ppm 范围内严格执行线性相关,R2=0.99974。值得注意的是,该传感器具有较高的灵敏度(658.45 nA/ppm)和较低的检测限(0.33 ppm)。此外,传感器的一致性和稳定性也令人满意。所构建的气体传感器有望很好地应用于工业 H2S 检测。
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引用次数: 0
Detection of GSH with a dual-mode biosensor based on carbon quantum dots prepared from dragon fruit peel and T-Hg(Ⅱ)-T mismatch 基于火龙果皮制备的碳量子点和 T-Hg(Ⅱ)-T 错配的双模式生物传感器检测 GSH
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-24 DOI: 10.1039/d4ay00904e
Weiqin Zhao, Ruichen Zhai, Qianxiao Chen, Chun Huang, Haojia Li, Youyu Zhu, Yingfeng Duan, Jie Gao
Glutathione (GSH) was commonly used as a diagnostic biomarker for many diseases. In this study, based on carbon quantum dots prepared from dragon fruit peel (D-CQDs) and T-Hg(Ⅱ)-T mismatch, a dual-mode biosensor was developed for the detection of GSH. This system consists of two single-stranded DNA (ssDNA). DNA1 was the T-rich sequence; DNA2 was attached to streptavidin-coated magnetic beads, and consisted of T-rich and G-rich fragment. Due to the presence of Hg(Ⅱ), the T-Hg(Ⅱ)-T mismatch was formed between T-rich fragment of two ssDNA. In the presence of GSH, Hg(Ⅱ) detached from dsDNA and bound with GSH to form a new complex. The G-rich fragment assembled with the hemin shed from D-CQDs to form the G-quadruplex/hemin complex. At this time, in fluorescence mode, the fluorescence of D-CQDs quenched by hemin could be restored. In colorimetric mode, after the magnetic beads separate, a visual signal could be produced by catalyzing the oxidation of ABTS using the peroxide-like activity of G-quadruplex/hemin complex. This biosensor in fluorescence mode and colorimetric mode both had excellent selectivity and sensitivity, and the limit of detection was 0.089 μM and 0.26 μM for GSH, respectively. Moreover, this proposed dual-mode biosensor had good application prospects for detection of GSH.
谷胱甘肽(GSH)通常被用作多种疾病的诊断生物标志物。本研究以火龙果皮制备的碳量子点(D-CQDs)和 T-Hg(Ⅱ)-T 错配为基础,开发了一种检测 GSH 的双模式生物传感器。该系统由两条单链 DNA(ssDNA)组成。DNA1 是富含 T 的序列;DNA2 连接到链霉亲和素包被的磁珠上,由富含 T 和富含 G 的片段组成。由于 Hg(Ⅱ)的存在,两个 ssDNA 的富 T 片段之间形成了 T-Hg(Ⅱ)-T 错配。在有 GSH 存在的情况下,Hg(Ⅱ) 从 dsDNA 上脱离,并与 GSH 结合形成新的复合物。富含 G 的片段与 D-CQDs 上脱落的 hemin 结合,形成 G-四叠体/hemin 复合物。此时,在荧光模式下,被hemin淬灭的D-CQDs荧光可以恢复。在比色模式下,磁珠分离后,利用 G-quadruplex/hemin 复合物的过氧化物样活性催化 ABTS 氧化,可产生视觉信号。该生物传感器在荧光模式和比色模式下均具有良好的选择性和灵敏度,对 GSH 的检测限分别为 0.089 μM 和 0.26 μM。此外,该双模式生物传感器在检测 GSH 方面具有良好的应用前景。
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引用次数: 0
Human Biomonitoring of Serum Polycyclic Aromatic Hydrocarbons and Oxygenated Derivatives by Gas Chromatography Coupled with Tandem Mass Spectrometry 利用气相色谱-串联质谱法对血清中的多环芳烃和含氧衍生物进行人体生物监测
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-21 DOI: 10.1039/d4ay00758a
Rong Yang, Chenwen Shi, Xiaojing Li, Pingsheng Gan, Xinhong Pan, Rongfei Peng, Lei Tan
While polycyclic aromatic hydrocarbons (PAHs) are well-known for their potential carcinogenic and mutagenic effects, the health implications of exposure to oxygenated PAHs (OPAHs), which are significant substitutes with increased persistence and bioaccumulation, are less understood. In this work, we compared the background levels of liquid-liquid, solid-phase, and supported-liquid extraction for the determination of serum PAHs and OPAHs. Liquid-liquid extraction demonstrated minimal background interference and was validated and used for human biomonitoring of PAHs and OPAHs in 240 participants using gas chromatography tandem with mass spectrometry. We observed significant positive correlations between these compounds using Spearman correlation analysis. Furthermore, we investigated the concentration levels and compositions of PAHs and OPAHs among different demographic groups, including gender, age, and body mass index. Linear regression analysis demonstrated a weak but significant correlation between total concentrations PAHs and OPAHs with age and body mass index. A multivariate linear regression analysis was then conducted to examine the association of exposure to individual PAHs and OPAHs with body mass index. Naphthalene exposure and body mass index showed a statistically significant positive correlation, suggesting that higher levels of naphthalene exposure are associated with higher body mass index values. This study establishes a robust method for biomonitoring PAHs and OPAHs in serum, evaluating the exposure levels of these compounds in health adults and highlighting their associations with demographic characteristics.
众所周知,多环芳烃(PAHs)具有潜在的致癌和致突变作用,但人们对暴露于含氧多环芳烃(OPAHs)对健康的影响却知之甚少,因为含氧多环芳烃是持久性和生物累积性更强的重要替代品。在这项研究中,我们比较了液液萃取、固相萃取和支撑液萃取法测定血清多环芳烃和 OPAHs 的本底水平。液液萃取法的背景干扰最小,并通过了验证,可用于气相色谱-串联质谱法对 240 名参与者的多环芳烃和 OPAHs 进行人体生物监测。通过斯皮尔曼相关分析,我们发现这些化合物之间存在明显的正相关关系。此外,我们还调查了不同人群(包括性别、年龄和体重指数)中多环芳烃和 OPAHs 的浓度水平和组成。线性回归分析表明,PAHs 和 OPAHs 的总浓度与年龄和体重指数之间存在微弱但显著的相关性。然后进行了多变量线性回归分析,以研究暴露于单个 PAHs 和 OPAHs 与体重指数之间的关系。萘暴露量与体重指数在统计学上呈显著正相关,表明萘暴露量越高,体重指数值也越高。这项研究建立了一种对血清中多环芳烃和高芳烃进行生物监测的可靠方法,评估了健康成年人的这些化合物的暴露水平,并强调了它们与人口特征的关系。
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引用次数: 0
Detection of sulphur(ii) of carbon dots synthesized from Gardenia residue 用栀子渣合成的碳点的硫(II)检测。
IF 2.7 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-21 DOI: 10.1039/D4AY00909F
Zhaoxia Li, Yuchuan Dong, Xinyi Li, Dongchun Li, Jia Dong, Panchen Wang, Shuwei Chen and Huiling Geng

The detection of anions using carbon dots (CDs) has received less attention compared to cations. Therefore, the present study aimed to develop a fluorescence sensor based on carbon dots (CDs) capable of detecting S2− in real water samples. The CDs were successfully prepared from the residues of a traditional Chinese herb, Gardenia, which emitted green photoluminescence (PL) under ultraviolet light irradiation. The as-prepared CDs were quasi-spherical in shape and ranged in size from 10 to 30 nm. Different detailed analyses proved that the CDs had good morphology, various functional groups, high water solubility, great optical features, and excellent stability under diverse environmental conditions. The ion detection showed that only Ag+ had the strongest fluorescence quenching effect on the CDs, however, the addition of S2− could recover their fluorescence. Based on these results, an “off–on” fluorescence sensor was achieved to selectively detect the concentration of S2− in real water samples with a limit of detection (LOD) of 39 μM, which further expanded the application of residues from traditional Chinese herbal medicine.

与阳离子相比,使用碳点(CD)检测阴离子受到的关注较少。因此,本研究旨在开发一种基于碳点(CD)的荧光传感器,能够检测真实水样中的 S2-。本研究成功地从一种传统中草药栀子的残留物中制备了碳点,该残留物在紫外线照射下可发出绿色光致发光(PL)。制备的光盘呈类球形,大小在 10 至 30 纳米之间。各种详细的分析表明,这些光盘具有良好的形貌、多种官能团、高水溶性、优异的光学特性以及在不同环境条件下的优异稳定性。离子检测结果表明,只有 Ag+ 对光盘具有最强的荧光淬灭效应,但加入 S2- 则可恢复其荧光。基于这些结果,一种 "关-开 "荧光传感器实现了对真实水样中 S2- 浓度的选择性检测,检测限(LOD)为 39 μM,进一步拓展了中药残留的应用领域。
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引用次数: 0
Development in competitive immunoassay of a point-of-care testing for cotinine (COT) detection in urine† 用竞争性免疫测定法开发尿液中可替宁(COT)的护理点检测。
IF 2.7 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-20 DOI: 10.1039/D4AY00518J
Suthinee Konziw, Paweena Tunakhun, Sawinee Ngernpimai, Oranee Srichaiyapol, Patcharee Boonsiri, Patcharaporn Tippayawat, Anchalee Techasen, Pornsuda Maraming, Kiattawee Choowongkomon, Sakda Daduang, Limthong Promdee and Jureerut Daduang

We present a sensitive and selective lateral flow immunoassay (LFIA) for cotinine (COT), the primary metabolite of nicotine. COT is widely recognized as a superior biomarker to evaluate tobacco smoke exposure. The LFIA uses a competitive assay format where the COT–BSA capture competes with the target COT in urine samples for binding to the monoclonal antibody against COT (mAb–COT) conjugated with gold nanoparticles (mAb–COT–AuNPs). To improve the sensitivity and selectivity of the LFIA-COT, we focused on optimizing the diameter of AuNPs, the conjugation of mAb–COT, and the concentration of the COT–BSA capture. Our findings reveal that the utilization of 40 nm AuNPs in conjugation with a concentration of 4 mg mL−1 of mAb–COT demonstrated significantly greater efficacy compared to LFAs utilizing 20 nm AuNPs. Under the optimal conditions, the LFIA-COT demonstrated sensitive detection of COT at a level of 150 ng mL−1 within 15 min, as observed by the naked eye. It possesses a linear range of 25 to 200 ng mL−1 of COT, with the limit of detection (LOD) of 11.94 ng mL−1 in human urine samples when the color intensity is analyzed using ImageJ software. Our LFIA described here is simple and requires less time for COT detection. It can be used for the rapid and quantitative detection of COT in urine samples in clinical settings.

我们介绍了一种灵敏且具有选择性的侧流免疫分析法(LFIA),用于检测尼古丁的主要代谢物可替宁(COT)。可替宁(COT)被公认为是评估烟草烟雾暴露的一种优质生物标记物。LFIA 采用竞争性测定法,即 COT-BSA 捕获物与尿样中的目标 COT 竞争,以结合到与金纳米颗粒(mAb-COT-AuNPs)共轭的抗 COT 的单克隆抗体(mAb-COT)上。为了提高 LFIA-COT 的灵敏度和选择性,我们重点优化了 AuNPs 的直径、mAb-COT 的共轭以及 COT-BSA 的捕获浓度。我们的研究结果表明,与使用 20 nm AuNPs 的 LFAs 相比,使用 40 nm AuNPs 与浓度为 4 mg mL-1 的 mAb-COT 相结合的效果明显更好。在最佳条件下,LFIA-COT 能在 15 分钟内用肉眼灵敏地检测到 150 纳克 mL-1 水平的 COT。它的线性范围为 25 至 200 ng mL-1 COT,使用 ImageJ 软件分析颜色强度时,人尿液样本中 COT 的检测限(LOD)为 11.94 ng mL-1。本文所述的 LFIA 方法简单,检测 COT 所需的时间较短。它可用于临床尿样中 COT 的快速定量检测。
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引用次数: 0
One-step electrodeposition of MWCNTs-Cu MOF films for the ratiometric electrochemical analysis of glyphosate† 一步式电沉积 MWCNTs-Cu MOF 薄膜,用于草甘膦的比率电化学分析。
IF 2.7 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-20 DOI: 10.1039/D4AY00691G
Fan Zhao, Dongqing Guo, Jingyue Lan and Yunxi Liu

Sensitive and accurate determination of glyphosate (GLYP) is vital for food safety and environmental protection. Herein, a novel electrochemical ratiometric biosensor was designed for the accurate quantification of GLYP through one-step electrodeposition of MWCNTs-Cu MOF films. MWCNTs-Cu MOF nanostructures were directly electro-synthesized in situ on the electrode from the precursor solution. The combination of Cu MOFs with MWCNTs not merely improved the conductivity of MOFs, but also enhanced the sensitivity of the biosensor. Furthermore, Cu sites within Cu MOFs were turned into CuCl to further amplify the current signal and enable the specific recognition of GLYP through competing reactions with the transformation of CuCl into non-electroactive Cu-GLYP. Meanwhile, internal reference molecules of methylene blue (MB) were incorporated to improve the measurement accuracy of GLYP for reducing unpredictable measurement errors aroused by environmental deviations. The ratiometric electrochemical sensor exhibited a high linearity with the logarithmic value of GLYP concentration from 0.5 nM to 400 nM. The detection limit was estimated to be as low as 0.014 nM. Finally, the present sensor with ratiometric signal export was applied for GLYP analysis in real samples with high sensitivity and accuracy. The simplicity and reliability of the ratiometric sensor make it a worthy and powerful tool for food and environmental monitoring. This design strategy also provides an avenue for the development of simple and efficient biosensors for other substances.

灵敏而准确地测定草甘膦(GLYP)对食品安全和环境保护至关重要。本文设计了一种新型电化学比率生物传感器,通过一步电沉积 MWCNTs-Cu MOF 薄膜来准确定量 GLYP。MWCNTs-Cu MOF 纳米结构由前驱体溶液直接在电极上原位电合成。Cu MOFs 与 MWCNTs 的结合不仅提高了 MOFs 的导电性,还增强了生物传感器的灵敏度。此外,Cu MOFs 中的 Cu 位点变成了 CuCl,进一步放大了电流信号,并通过与 CuCl 转化为非电活性 Cu-GLYP 的竞争反应实现了对 GLYP 的特异性识别。同时,还加入了亚甲基蓝(MB)内参分子,以提高 GLYP 的测量精度,减少因环境偏差而产生的不可预测的测量误差。该比率电化学传感器在 0.5 nM 至 400 nM 的 GLYP 浓度对数值范围内表现出较高的线性度。检测限估计低至 0.014 nM。最后,这种具有比率信号输出的传感器被应用于实际样品中的 GLYP 分析,灵敏度和准确度都很高。比率测量传感器的简便性和可靠性使其成为食品和环境监测领域值得使用的强大工具。这种设计策略还为开发用于其他物质的简单高效的生物传感器提供了途径。
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引用次数: 0
Early Diagnosis of Autoimmune Diseases through Electrochemical Biosensing using Modified Plastic Chip Electrode 利用改性塑料芯片电极的电化学生物传感技术早期诊断自身免疫性疾病
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-20 DOI: 10.1039/d4ay00789a
Kinjal B. Patel, Sunil Luhar, Divesh Narayan Srivastava
Detecting chronic autoimmune disorders (AD) early reduces the risk of morbidity, disability, and mortality, and offers the possibility of significant therapeutic action in a timely manner. Developing low-cost, reliable, and sensitive sensors for AD can ensure the efficient utilization of healthcare resources at earlier stages. Here, we report on the development of an electrochemical biosensor for sensing CXCL10, a chemokine protein that serves as a biomarker for autoimmune diseases. A self-assembly strategy is used for the immobilization of biorecognition elements on a plastic chip electrode (PCE). A homemade PCE offers a versatile and cost-effective scaffold for sensing applications. Gold nanoparticles were electrochemically deposited on the electrode via the reduction of gold ions on the PCE galvanostatically. The CXCL10 antibody and recognition elements were immobilized on the gold-deposited PCE. The attachment of recognition molecules was confirmed by energy-dispersive scanning electron microscopy, atomic force microscopy, infrared spectroscopy, and electrochemical techniques. Electrochemical impedance spectroscopy (EIS) was used for the detection of CXCL10 within a concentration range spanning from pico- to micromolar levels. The sensor exhibited remarkable linearity in both buffer and plasma solutions, with a limit of detection (LOD) of up to 0.72 pg/mL
及早发现慢性自身免疫性疾病(AD)可降低发病、残疾和死亡风险,并为及时采取重大治疗行动提供可能性。开发低成本、可靠且灵敏的 AD 传感器可以确保在早期阶段有效利用医疗资源。在此,我们报告了一种用于检测 CXCL10 的电化学生物传感器的开发情况,CXCL10 是一种趋化因子蛋白,是自身免疫性疾病的生物标记物。我们采用自组装策略将生物识别元件固定在塑料芯片电极(PCE)上。自制的 PCE 为传感应用提供了一个多功能且经济高效的支架。金纳米粒子是通过电化学方法将金离子还原到 PCE 上沉积到电极上的。CXCL10 抗体和识别元件被固定在金沉积的 PCE 上。能量色散扫描电子显微镜、原子力显微镜、红外光谱和电化学技术证实了识别分子的附着。电化学阻抗光谱(EIS)用于检测浓度范围在皮摩尔到微摩尔水平的 CXCL10。该传感器在缓冲液和血浆溶液中均表现出卓越的线性度,检测限(LOD)高达 0.72 pg/mL
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引用次数: 0
Bioluminescent aptamer-based microassay for detection of melanoma inhibitory activity protein (MIA)† 基于生物发光适配体的微测定法,用于检测黑色素瘤抑制活性蛋白(MIA)。
IF 2.7 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-20 DOI: 10.1039/D4AY00706A
Eugenia E. Bashmakova, Alexander N. Kudryavtsev, Alexey E. Tupikin, Marsel R. Kabilov, Aleksey E. Sokolov and Ludmila A. Frank

Melanoma inhibitory activity protein (MIA) does obviously offer the potential to reveal clinical manifestations of melanoma. Despite a pressing need for effective diagnosis of this highly fatal disease, there are no clinically approved MIA detection ELISA kits available. A recommended MIA threshold has not yet been defined, mostly by reason of variability in immunoglobulins' affinity and stability, the difference in sample preparation and assay conditions. Here we present a pair of high-affinity DNA aptamers developed as an alternative recognition and binding element for MIA detection. Their stability and reproducible synthesis are expected to ensure this analysis under standard conditions. The devised aptamer-based solid-phase microassay of model standard and control human sera involves luciferase NLuc as a highly sensitive reporter. Bioluminescence dependence on MIA concentration ranges in a linear manner from 2.5 to 250 ng mL−1, providing a MIA detection limit of 1.67 ± 0.57 ng mL−1.

黑色素瘤抑制活性蛋白(MIA)显然具有揭示黑色素瘤临床表现的潜力。尽管迫切需要对这种高度致命的疾病进行有效诊断,但目前还没有临床认可的 MIA 检测 ELISA 试剂盒。主要由于免疫球蛋白亲和力和稳定性的变化、样品制备和检测条件的差异,目前尚未确定推荐的 MIA 临界值。在此,我们提出了一对高亲和力 DNA 对映体,作为 MIA 检测的另一种识别和结合元件。它们的稳定性和可重复合成有望确保在标准条件下进行分析。所设计的基于适配体的固相微量检测模型标准和对照人类血清,采用了荧光素酶 NLuc 作为高灵敏度的报告物。生物发光对 MIA 浓度的依赖性在 2.5 至 250 ng mL-1 之间呈线性关系,MIA 检测限为 1.67 ± 0.57 ng mL-1。
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引用次数: 0
Validation of microwave acid digestion, diffusive gradients in thin-films preconcentration and inductively coupled plasma optical emission spectrometry methodology for the determination of REEs in natural zeolites 验证用于测定天然沸石中稀土元素的微波酸消化、薄膜扩散梯度预富集和电感耦合等离子体光发射光谱法
IF 3.1 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-06-19 DOI: 10.1039/d4ay00745j
Marin Senila, Erika-Andrea Levei, Lacrimioara Senila, Oana Cadar
The determination of rare earth elements (REEs) content in different natural minerals is of high interest due to their extensive use in modern and sustainable technologies. The REEs occurring in natural zeolites are specific to each deposit. This study presents the validation and evaluation of measurement uncertainty for the determination of REEs (Ce, Dy, Er, Eu, Gd, La, Lu, Nd, Pr, Sm, Y, and Yb) in natural zeolites using microwave-assisted acid digestion and inductively coupled plasma optical emission spectrometry (ICP-OES) after diffusive gradients in thin-films preconcentration. The mixture of HNO3:HCl:HF of 3:9:2 (v/v/v) and microwave digestion provided suitable recoveries for the analysis of two certified reference materials, CRM BCS-CRM 375/1 and CRM OREAS 460. Good linearity over the calibration range of 0 – 2 µg mL-1, with correlation coefficients of 0.9995 – 1.0000 was obtained for each REEs by ICP-OES. The limits of quantification (LOQS), calculated considering the instrumental LOQs and the sample preparation by microwave digestion, were in the range of 0.20 – 0.60 mg kg-1. A supplementary step of preconcentration/matrix separation based on passive sampling by diffusive gradients in thin-films (DGT) technique improved the LOQs by about 20 times after three days of passive accumulation, allowing the measurement of the concentrations of all studied REEs in natural zeolite samples. The proposed methodology is a suitable approach for the measurement of REEs at low concentrations in natural zeolite samples by ICP-OES, and it can be extended to other geological samples. The measurement uncertainty was calculated based on the validation data. The proposed method provides reliable results for the measurement of REEs in natural zeolites and was used to measure the specific concentrations of REEs in natural zeolite samples from the three Romanian quarries. The REEs concentration can be used as a fingerprint for each deposit.
由于稀土元素在现代和可持续技术中的广泛应用,测定不同天然矿物中的稀土元素(REEs)含量备受关注。天然沸石中的稀土元素因矿床而异。本研究介绍了利用微波辅助酸消解和电感耦合等离子体光发射光谱(ICP-OES)测定天然沸石中的 REEs(Ce、Dy、Er、Eu、Gd、La、Lu、Nd、Pr、Sm、Y 和 Yb)的验证和测量不确定性评估。HNO3:HCl:HF 混合物的比例为 3:9:2(v/v/v),微波消解法可提供适当的回收率,用于分析两种经认证的参考材料:CRM BCS-CRM 375/1 和 CRM OREAS 460。在 0 - 2 µg mL-1 的校准范围内,ICP-OES 对每种稀土元素都具有良好的线性关系,相关系数在 0.9995 - 1.0000 之间。根据仪器定量限和微波消解样品制备方法计算出的定量限(LOQS)范围为 0.20 - 0.60 mg kg-1。在采用薄膜扩散梯度(DGT)技术进行被动采样的基础上,再辅以预浓缩/基质分离步骤,经过三天的被动累积,LOQs 提高了约 20 倍,从而可以测量天然沸石样品中所有研究的 REEs 的浓度。所提出的方法适用于利用 ICP-OES 测量天然沸石样品中低浓度的 REEs,并可扩展到其他地质样品。根据验证数据计算了测量的不确定性。所提出的方法为天然沸石中 REEs 的测量提供了可靠的结果,并被用于测量罗马尼亚三个采石场天然沸石样品中 REEs 的特定浓度。REEs 浓度可用作每个矿床的指纹。
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引用次数: 0
期刊
Analytical Methods
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