首页 > 最新文献

Analytica Chimica Acta最新文献

英文 中文
Mass Spectrometry Imaging Tutorial: From Cancer Biomarker Discovery To Clinical Applications 质谱成像教程:从癌症生物标志物的发现到临床应用
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-24 DOI: 10.1016/j.aca.2025.344925
Amirsalar Mansouri, Nipun Babu Varukattu, Brennan J. Curole, Omeed Moaven, Jiri Adamec
{"title":"Mass Spectrometry Imaging Tutorial: From Cancer Biomarker Discovery To Clinical Applications","authors":"Amirsalar Mansouri, Nipun Babu Varukattu, Brennan J. Curole, Omeed Moaven, Jiri Adamec","doi":"10.1016/j.aca.2025.344925","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344925","url":null,"abstract":"","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"3 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145593336","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
Flow injection bioassay platform with electrochemical detection for pyruvate determination: Development of highly efficient immobilized enzyme reactors 流动注射电化学检测丙酮酸的生物测定平台:高效固定化酶反应器的研制
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-22 DOI: 10.1016/j.aca.2025.344923
Sofiia Tvorynska, Bohdan Josypcuk
<div><h3>Background</h3><div>Pyruvate determination is of great importance in the biomedical field, as its altered level, often assessed together with lactate level as the lactate/pyruvate ratio, is a potential biomarker of various diseases. Additionally, the monitoring of pyruvate is used in the food industry to control processes of fermented food/beverage production. Due to the high selectivity and sensitivity, enzyme-based bioassays can be successfully applied for pyruvate detection; however, the short lifetime and high costs limit their full integration as analytical devices. Therefore, the design of bioassay techniques that have good analytical performance, high storage and operational stability, interference-free from the complex biological matrices, along with simplicity and affordability, is a great demand.</div></div><div><h3>Results</h3><div>We developed a new electrochemical flow injection bioassay system based on an immobilized enzyme reactor (IMER) with pyruvate oxidase (POx) for pyruvate determination. An electrochemical detection involves amperometric monitoring of enzymatically consumed oxygen via its reduction at the silver amalgam screen-printed electrode. For IMER preparation, two POx enzymes and two immobilization protocols (covalent attachment onto mesoporous silica powder SBA-15 and physical adsorption onto mesoporous carbon powder Starbon@300) were compared. Both IMERs, regardless of the protocol used, with POx from <em>microorganisms</em> (<em>m</em>POx) as the preferred enzyme, are characterized by high enzymatic capacity (<em>ca.</em> 620 μg of <em>m</em>POx per IMER) with a negligible degree of enzyme leaching (1.7 %). Importantly, the <em>m</em>POx-based IMERs demonstrate high storage stability (6 months) and reusability (400 measurements), while no passivation of the working electrode is observed. The developed bioassay is capable of detecting 11 μM of pyruvate. Finally, the advantages and limitations of pyruvate determination using the enzymatic substrate recycling approach were discussed by testing the IMER consisting of lactate dehydrogenase and lactate oxidase.</div></div><div><h3>Significance</h3><div>This work represents a high-performance pyruvate bioassay with amperometric detection in flow injection analysis, which can be easily automated to increase the expressiveness and productivity of measurements. The long-term operation of the IMERs combined with their affordability (≤€19) and no passivation of the working electrode provides a reliable, rapid, and cost-effective approach for pyruvate determination. The practical applicability of the proposed bioassay platform has been successfully verified by the analysis of various pyruvate-containing beverages/food products as well as samples of human urine and plasma. The relative recovery values in the spiked-found tests ranged from 95.5 to 104.0 %, suggesting the high accuracy and precision of quantitative determination of pyruvate utilizing the developed bioassay.
背景丙酮酸测定在生物医学领域具有重要意义,其变化水平通常与乳酸水平(乳酸/丙酮酸比值)一起评估,是多种疾病的潜在生物标志物。此外,丙酮酸监测在食品工业中用于控制发酵食品/饮料生产过程。酶法具有高选择性和高灵敏度,可成功应用于丙酮酸的检测;然而,短寿命和高成本限制了它们作为分析设备的全面集成。因此,设计具有良好的分析性能,高存储和操作稳定性,不受复杂生物基质干扰,以及简单和负担得起的生物测定技术是一个很大的需求。结果基于固定化酶反应器(IMER)和丙酮酸氧化酶(POx)建立了丙酮酸测定的电化学流动注射生物测定系统。电化学检测包括通过在银汞合金丝网印刷电极上的还原对酶耗氧的安培监测。对于IMER的制备,比较了两种POx酶和两种固定方案(共价附着在介孔硅粉SBA-15上和物理吸附在介孔碳粉Starbon@300上)。无论使用何种方案,这两种IMERs都具有高酶容量(每个IMER约620 μg mPOx)和可忽略不计的酶浸出程度(1.7%)。重要的是,基于mpox的iers具有高存储稳定性(6个月)和可重复使用性(400次测量),同时没有观察到工作电极的钝化。该方法可检测11 μM的丙酮酸。最后,通过对由乳酸脱氢酶和乳酸氧化酶组成的内聚酶(IMER)的检测,讨论了酶底物回收法测定丙酮酸盐的优点和局限性。意义本工作代表了流动注射分析中具有安培检测的高效丙酮酸生物测定方法,该方法可以很容易地自动化以提高测量的表达性和生产率。IMERs的长期运行,加上其可负担性(≤19欧元)和工作电极无钝化,为丙酮酸测定提供了一种可靠、快速和经济有效的方法。通过分析各种含丙酮酸的饮料/食品以及人类尿液和血浆样本,成功验证了所提出的生物测定平台的实际适用性。该方法的相对回收率为95.5% ~ 104.0%,具有较高的准确度和精密度。
{"title":"Flow injection bioassay platform with electrochemical detection for pyruvate determination: Development of highly efficient immobilized enzyme reactors","authors":"Sofiia Tvorynska,&nbsp;Bohdan Josypcuk","doi":"10.1016/j.aca.2025.344923","DOIUrl":"10.1016/j.aca.2025.344923","url":null,"abstract":"&lt;div&gt;&lt;h3&gt;Background&lt;/h3&gt;&lt;div&gt;Pyruvate determination is of great importance in the biomedical field, as its altered level, often assessed together with lactate level as the lactate/pyruvate ratio, is a potential biomarker of various diseases. Additionally, the monitoring of pyruvate is used in the food industry to control processes of fermented food/beverage production. Due to the high selectivity and sensitivity, enzyme-based bioassays can be successfully applied for pyruvate detection; however, the short lifetime and high costs limit their full integration as analytical devices. Therefore, the design of bioassay techniques that have good analytical performance, high storage and operational stability, interference-free from the complex biological matrices, along with simplicity and affordability, is a great demand.&lt;/div&gt;&lt;/div&gt;&lt;div&gt;&lt;h3&gt;Results&lt;/h3&gt;&lt;div&gt;We developed a new electrochemical flow injection bioassay system based on an immobilized enzyme reactor (IMER) with pyruvate oxidase (POx) for pyruvate determination. An electrochemical detection involves amperometric monitoring of enzymatically consumed oxygen via its reduction at the silver amalgam screen-printed electrode. For IMER preparation, two POx enzymes and two immobilization protocols (covalent attachment onto mesoporous silica powder SBA-15 and physical adsorption onto mesoporous carbon powder Starbon@300) were compared. Both IMERs, regardless of the protocol used, with POx from &lt;em&gt;microorganisms&lt;/em&gt; (&lt;em&gt;m&lt;/em&gt;POx) as the preferred enzyme, are characterized by high enzymatic capacity (&lt;em&gt;ca.&lt;/em&gt; 620 μg of &lt;em&gt;m&lt;/em&gt;POx per IMER) with a negligible degree of enzyme leaching (1.7 %). Importantly, the &lt;em&gt;m&lt;/em&gt;POx-based IMERs demonstrate high storage stability (6 months) and reusability (400 measurements), while no passivation of the working electrode is observed. The developed bioassay is capable of detecting 11 μM of pyruvate. Finally, the advantages and limitations of pyruvate determination using the enzymatic substrate recycling approach were discussed by testing the IMER consisting of lactate dehydrogenase and lactate oxidase.&lt;/div&gt;&lt;/div&gt;&lt;div&gt;&lt;h3&gt;Significance&lt;/h3&gt;&lt;div&gt;This work represents a high-performance pyruvate bioassay with amperometric detection in flow injection analysis, which can be easily automated to increase the expressiveness and productivity of measurements. The long-term operation of the IMERs combined with their affordability (≤€19) and no passivation of the working electrode provides a reliable, rapid, and cost-effective approach for pyruvate determination. The practical applicability of the proposed bioassay platform has been successfully verified by the analysis of various pyruvate-containing beverages/food products as well as samples of human urine and plasma. The relative recovery values in the spiked-found tests ranged from 95.5 to 104.0 %, suggesting the high accuracy and precision of quantitative determination of pyruvate utilizing the developed bioassay.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1384 ","pages":"Article 344923"},"PeriodicalIF":6.0,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145567834","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
One-pot fabrication of highly stable and luminescent InP quantum dots nanobeads through multifunctional polymer encapsulation for lateral flow immunoassay 用多功能聚合物包封一锅法制备高稳定发光的InP量子点纳米球,用于横向流动免疫分析
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-22 DOI: 10.1016/j.aca.2025.344924
Xinxin Chen , Qingbiao Zheng , Xiaoquan Li , Li Wang , Lifang Zhang , Yuxin Zhang , Lei Wang , Yanbing Lv , Lin Song Li , Ruili Wu

Background

Lateral flow immunoassay (LFIA) with the advantages of simplicity, rapidness, and low cost have been a prominent point-of-care test (POCT) technology in in vitro diagnostics (IVD). Quantum dots (QDs) based-LFIA have attracted strong attention due to higher sensitivity and quantitative capabilities. Developing the less toxic InP QDs, the most promising candidate for Cd-based QDs, can advance their practical applications in industrial products. However, the use of InP QDs as fluorescence label in LFIA is limited by their unstable and poor luminescent properties due to their highly susceptibility towards O2 and H2O.

Results

We developed a one-pot approach to fabricate InP nanobeads (InP QBs) by emulsion evaporation and multifunctional polymer encapsulation. After the InP@DTAB nanobeads formed by emulsion-solvent evaporation with dodecyl trimethylammonium bromide (DTAB), the InP@DTAB nanobeads were encapsulated with PVP and carboxyl PEG. This method not only minimizes fluorescence loss caused by defects in multi-step reactions but also directly introduces carboxyl groups, facilitating subsequent conjugation with biomolecules. The prepared InP QBs showed high brightness, good alkaline resistance, photostability and thermal stability. Subsequently, the InP QBs was used as labels in LFIA for detection of C-reactive protein (CRP) and N-terminal pro-B-type natriuretic peptide (NT-proBNP), achieving lower detection limits of 0.67 ng/mL for CRP and 0.003 ng/mL for NT-proBNP. The InP QBs based-LFIA also had excellent specificity, stability, and accuracy verified by clinical samples.

Significance

This study illustrates the first introduction of PVP and carboxyl PEG to prepare InP nanobeads after the nanobeads formed with emulsion evaporation, which avoided the method of silica encapsulation leading to the fluorescence quench. The InP nanobeads retains the fluorescence and their stability was greatly improved. Compared to other point-of-care test (POCT) assay, the developed InP QBs based-LFIA achieves lower detection limits with excellent specificity, stability, especially accuracy, which shows great application prospects for POCT kits.
横向流动免疫测定(LFIA)具有简单、快速和低成本的优点,已成为体外诊断(IVD)中重要的即时检测(POCT)技术。基于量子点(QDs)的lfia由于具有较高的灵敏度和定量能力而受到广泛关注。开发毒性较低的InP量子点可以促进其在工业产品中的实际应用,这是最有前途的cd基量子点候选材料。然而,由于InP量子点对O2和H2O的高度敏感性,其不稳定且发光性能差,限制了其在LFIA中作为荧光标记的使用。结果通过乳液蒸发和多功能聚合物包封,建立了一锅法制备InP纳米球的方法。用十二烷基三甲基溴化铵(DTAB)乳化-溶剂蒸发法制备InP@DTAB纳米球后,再用PVP和羧基PEG包封InP@DTAB纳米球。该方法不仅最大限度地减少了多步反应中缺陷引起的荧光损失,而且还直接引入了羧基,便于后续与生物分子的偶联。制备的InP QBs具有高亮度、良好的耐碱性、光稳定性和热稳定性。随后,将InP qb作为LFIA中c反应蛋白(CRP)和n端前b型利钠肽(NT-proBNP)的标记物进行检测,CRP和NT-proBNP的检出限分别为0.67 ng/mL和0.003 ng/mL。基于InP QBs的lfia也具有良好的特异性,稳定性和准确性,经临床样品验证。意义本研究首次将PVP和羧基PEG引入到InP纳米球的制备中,通过乳液蒸发形成纳米球,避免了二氧化硅包封导致荧光猝灭的方法。InP纳米球保留了荧光,其稳定性大大提高。与其他POCT检测方法相比,所建立的基于InP QBs的lfia检测限低,具有良好的特异性、稳定性,特别是准确性,在POCT试剂盒中具有广阔的应用前景。
{"title":"One-pot fabrication of highly stable and luminescent InP quantum dots nanobeads through multifunctional polymer encapsulation for lateral flow immunoassay","authors":"Xinxin Chen ,&nbsp;Qingbiao Zheng ,&nbsp;Xiaoquan Li ,&nbsp;Li Wang ,&nbsp;Lifang Zhang ,&nbsp;Yuxin Zhang ,&nbsp;Lei Wang ,&nbsp;Yanbing Lv ,&nbsp;Lin Song Li ,&nbsp;Ruili Wu","doi":"10.1016/j.aca.2025.344924","DOIUrl":"10.1016/j.aca.2025.344924","url":null,"abstract":"<div><h3>Background</h3><div>Lateral flow immunoassay (LFIA) with the advantages of simplicity, rapidness, and low cost have been a prominent point-of-care test (POCT) technology in <em>in</em> <em>vitro</em> diagnostics (IVD). Quantum dots (QDs) based-LFIA have attracted strong attention due to higher sensitivity and quantitative capabilities. Developing the less toxic InP QDs, the most promising candidate for Cd-based QDs, can advance their practical applications in industrial products. However, the use of InP QDs as fluorescence label in LFIA is limited by their unstable and poor luminescent properties due to their highly susceptibility towards O<sub>2</sub> and H<sub>2</sub>O.</div></div><div><h3>Results</h3><div>We developed a one-pot approach to fabricate InP nanobeads (InP QBs) by emulsion evaporation and multifunctional polymer encapsulation. After the InP@DTAB nanobeads formed by emulsion-solvent evaporation with dodecyl trimethylammonium bromide (DTAB), the InP@DTAB nanobeads were encapsulated with PVP and carboxyl PEG. This method not only minimizes fluorescence loss caused by defects in multi-step reactions but also directly introduces carboxyl groups, facilitating subsequent conjugation with biomolecules. The prepared InP QBs showed high brightness, good alkaline resistance, photostability and thermal stability. Subsequently, the InP QBs was used as labels in LFIA for detection of C-reactive protein (CRP) and N-terminal pro-B-type natriuretic peptide (NT-proBNP), achieving lower detection limits of 0.67 ng/mL for CRP and 0.003 ng/mL for NT-proBNP. The InP QBs based-LFIA also had excellent specificity, stability, and accuracy verified by clinical samples.</div></div><div><h3>Significance</h3><div>This study illustrates the first introduction of PVP and carboxyl PEG to prepare InP nanobeads after the nanobeads formed with emulsion evaporation, which avoided the method of silica encapsulation leading to the fluorescence quench. The InP nanobeads retains the fluorescence and their stability was greatly improved. Compared to other point-of-care test (POCT) assay, the developed InP QBs based-LFIA achieves lower detection limits with excellent specificity, stability, especially accuracy, which shows great application prospects for POCT kits.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344924"},"PeriodicalIF":6.0,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145568016","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
Efficient TiO2-catalyzed photochemical vapor generation method for the determination of Se 高效tio2催化光化学气相生成法测定硒
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-22 DOI: 10.1016/j.aca.2025.344928
Eliška Nováková , Natália Remper , Daniel N. Rainer , Daniel Nentvich

Background

TiO2-assisted photochemical vapor generation (PVG) elegantly solves the inertness of selenate to PVG allowing on-line prereduction of this species and sensitive determination of the element. Overall efficiency of TiO2-assisted photochemical generation depends on the efficiency of electron transfer from the photocatalyst to the dissolved analyte, which is affected by the characteristics of the photocatalyst as well as by the chemical conditions. Up to date, the overall PVG efficiency of the Se TiO2 assisted-PVG system has not been known and the effect of particle size and crystal phase on the efficiency has not been studied.

Results

Two types of TiO2 photocatalyst were characterized and tested showing that smaller particle plays more important role than crystal phase. Optimization of the chemical conditions including addition of transition metal mediators led to the development of photochemical vapor generation method having overall vapor generation efficiency of 63 % (selenite) or 67 % (selenate). The limits of detection were 1.2 μg dm−3 (selenite) and 1.1 μg dm−3 (selenate) with quartz furnace atomic absorption spectrometry detection or 0.15 μg dm−3 (selenite) and 0.14 μg dm−3 (selenate) with inductively coupled plasma mass spectrometry detection on mass 78 Da (not using polyatomic interference suppression). The method shows unusually good tolerance toward dissolved salts and inorganic acids including HNO3. The method's accuracy was successfully verified on spiked freshwater and seawater samples and water reference materials.

Significance

The overall PVG efficiency of a benchmark photocatalysis approach to the on-line prereduction of selenate has been determined. The importance of particle size and corresponding larger surface area over crystal phase was demonstrated. The developed method for determination of Se is suitable for seawater matrix and can be used without modification with various detection techniques.
二氧化钛辅助光化学蒸汽生成(PVG)优雅地解决了硒酸盐对PVG的惰性,允许该物种的在线预还原和元素的敏感测定。tio2辅助光化学生成的总体效率取决于从光催化剂到溶解分析物的电子转移效率,这受到光催化剂特性以及化学条件的影响。迄今为止,Se - TiO2辅助PVG体系的整体PVG效率尚不清楚,粒径和晶相对效率的影响也未得到研究。结果对两种类型的TiO2光催化剂进行了表征和测试,结果表明,粒径较小的TiO2光催化剂比晶相的TiO2光催化剂起更重要的作用。优化化学条件,包括添加过渡金属介质,开发了总蒸汽生成效率为63%(亚硒酸盐)或67%(硒酸盐)的光化学蒸汽生成方法。石英炉原子吸收光谱法检测的检出限分别为1.2 μg dm−3(亚硒酸盐)和1.1 μg dm−3(硒酸盐);电感耦合等离子体质谱法检测的检出限分别为0.15 μg dm−3(亚硒酸盐)和0.14 μg dm−3(硒酸盐),质量为78 Da(不使用多原子干扰抑制)。该方法对溶解盐和包括HNO3在内的无机酸表现出异常良好的耐受性。该方法在加标淡水、海水样品和水标准物质上的准确性得到了验证。已经确定了一种基准光催化方法在线预还原硒酸盐的总体PVG效率。证明了晶粒尺寸和相应的较大表面积对晶相的重要性。该方法适用于海水基质中硒的测定,可与各种检测技术相结合,无需修改。
{"title":"Efficient TiO2-catalyzed photochemical vapor generation method for the determination of Se","authors":"Eliška Nováková ,&nbsp;Natália Remper ,&nbsp;Daniel N. Rainer ,&nbsp;Daniel Nentvich","doi":"10.1016/j.aca.2025.344928","DOIUrl":"10.1016/j.aca.2025.344928","url":null,"abstract":"<div><h3>Background</h3><div>TiO<sub>2</sub>-assisted photochemical vapor generation (PVG) elegantly solves the inertness of selenate to PVG allowing on-line prereduction of this species and sensitive determination of the element. Overall efficiency of TiO<sub>2</sub>-assisted photochemical generation depends on the efficiency of electron transfer from the photocatalyst to the dissolved analyte, which is affected by the characteristics of the photocatalyst as well as by the chemical conditions. Up to date, the overall PVG efficiency of the Se TiO<sub>2</sub> assisted-PVG system has not been known and the effect of particle size and crystal phase on the efficiency has not been studied.</div></div><div><h3>Results</h3><div>Two types of TiO<sub>2</sub> photocatalyst were characterized and tested showing that smaller particle plays more important role than crystal phase. Optimization of the chemical conditions including addition of transition metal mediators led to the development of photochemical vapor generation method having overall vapor generation efficiency of 63 % (selenite) or 67 % (selenate). The limits of detection were 1.2 μg dm<sup>−3</sup> (selenite) and 1.1 μg dm<sup>−3</sup> (selenate) with quartz furnace atomic absorption spectrometry detection or 0.15 μg dm<sup>−3</sup> (selenite) and 0.14 μg dm<sup>−3</sup> (selenate) with inductively coupled plasma mass spectrometry detection on mass 78 Da (not using polyatomic interference suppression). The method shows unusually good tolerance toward dissolved salts and inorganic acids including HNO<sub>3</sub>. The method's accuracy was successfully verified on spiked freshwater and seawater samples and water reference materials.</div></div><div><h3>Significance</h3><div>The overall PVG efficiency of a benchmark photocatalysis approach to the on-line prereduction of selenate has been determined. The importance of particle size and corresponding larger surface area over crystal phase was demonstrated. The developed method for determination of Se is suitable for seawater matrix and can be used without modification with various detection techniques.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1384 ","pages":"Article 344928"},"PeriodicalIF":6.0,"publicationDate":"2025-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145575400","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
Ag+ dual-driven self-calibration for high-performance dual-photoelectrode self-powered ratiometric sensing Ag+双驱动自校准用于高性能双光电极自供电比率传感
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-21 DOI: 10.1016/j.aca.2025.344908
Yanru Zhang, Xuechen Zhang, Xue Fan, Hongye Liu, Jingyao Peng, Wenbo Song, Daqian Song
Despite significant advances in the dual-photoelectrode self-powered sensor, the single-signal output mode usually brings false positives/negatives from environmental interference and instrumental fluctuations, which fails to meet the requirement of accurate and sensitive detection of low-level markers in food safety and environmental monitoring. To address this critical issue, we herein report an Ag+ dual-driven self-calibrating strategy for self-powered ratiometric assay. In the ZnIn2S4//Bi2S3/CuTCPP dual-photoelectrode system, the synergy effect of Ag+-triggered DNAzyme cleavage and cation exchange on ZnIn2S4 photoanode produces a stable and weak reference signal. Specifically, Ag+-triggered DNAzyme cleavages the 3D DNA walker-amplified signal label, and the ion exchange between Ag+ and ZnIn2S4 quenches the reference signal simultaneously via electron migration pathway change. A proof-of-concept detection of mycotoxin ochratoxin A in the crop samples is demonstrated. The ratiometric self-powered sensor demonstrates a wide linear range of 10−6 -102 ng/mL with an ultralow detection limit of 0.20 fg/mL. This work breaks the limits of single-signal self-powered detection, providing a brand-new idea for developing portable devices with great potential of on-site testing in the field environment.
尽管双光电极自供电传感器取得了重大进展,但单信号输出模式往往会受到环境干扰和仪器波动的假阳性/阴性,无法满足食品安全和环境监测中对低水平标志物准确、灵敏检测的要求。为了解决这一关键问题,我们在此报告了一种用于自供电比率测定的Ag+双驱动自校准策略。在ZnIn2S4//Bi2S3/CuTCPP双光电极体系中,Ag+触发的DNAzyme裂解和阳离子交换在ZnIn2S4光阳极上的协同效应产生了稳定而微弱的参考信号。具体来说,Ag+触发的DNAzyme切割了3D DNA walk - amplification信号标签,Ag+和ZnIn2S4之间的离子交换通过电子迁移途径的改变同时淬灭了参考信号。演示了作物样品中真菌毒素赭曲霉毒素A的概念验证检测。比例自供电传感器具有10-6 -102 ng /mL的宽线性范围,超低检出限为0.20 fg/mL。该工作突破了单信号自供电检测的局限,为开发具有巨大现场环境测试潜力的便携式设备提供了全新思路。
{"title":"Ag+ dual-driven self-calibration for high-performance dual-photoelectrode self-powered ratiometric sensing","authors":"Yanru Zhang,&nbsp;Xuechen Zhang,&nbsp;Xue Fan,&nbsp;Hongye Liu,&nbsp;Jingyao Peng,&nbsp;Wenbo Song,&nbsp;Daqian Song","doi":"10.1016/j.aca.2025.344908","DOIUrl":"10.1016/j.aca.2025.344908","url":null,"abstract":"<div><div>Despite significant advances in the dual-photoelectrode self-powered sensor, the single-signal output mode usually brings false positives/negatives from environmental interference and instrumental fluctuations, which fails to meet the requirement of accurate and sensitive detection of low-level markers in food safety and environmental monitoring. To address this critical issue, we herein report an Ag<sup>+</sup> dual-driven self-calibrating strategy for self-powered ratiometric assay. In the ZnIn<sub>2</sub>S<sub>4</sub>//Bi<sub>2</sub>S<sub>3</sub>/CuTCPP dual-photoelectrode system, the synergy effect of Ag<sup>+</sup>-triggered DNAzyme cleavage and cation exchange on ZnIn<sub>2</sub>S<sub>4</sub> photoanode produces a stable and weak reference signal. Specifically, Ag<sup>+</sup>-triggered DNAzyme cleavages the 3D DNA walker-amplified signal label, and the ion exchange between Ag<sup>+</sup> and ZnIn<sub>2</sub>S<sub>4</sub> quenches the reference signal simultaneously via electron migration pathway change. A proof-of-concept detection of mycotoxin ochratoxin A in the crop samples is demonstrated. The ratiometric self-powered sensor demonstrates a wide linear range of 10<sup>−6</sup> -10<sup>2</sup> ng/mL with an ultralow detection limit of 0.20 fg/mL. This work breaks the limits of single-signal self-powered detection, providing a brand-new idea for developing portable devices with great potential of on-site testing in the field environment.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344908"},"PeriodicalIF":6.0,"publicationDate":"2025-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145560621","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
Review on electrochemical sensors for anticancer drug susceptibility testing 电化学传感器在抗癌药物敏感性检测中的研究进展
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-20 DOI: 10.1016/j.aca.2025.344905
Paula C.R. Corsato, Christian O. Silva, Iris R.S. Ribeiro, Renato S. Lima
Anticancer drug susceptibility tests play an essential role in areas such as drug development, pharmacokinetic research, and precision oncology. Across these tests, the methods that are traditionally used for gauging the drug effect—by determining the cell viability of in vitro cell models after drug exposure—are commonly time-consuming and limited to end-point detection. In this regard, electrochemical sensors have emerged as a promising alternative to increase throughput and yield real-time pharmacokinetic monitoring. In this critical review, considerations on the operating principles, advantages, and disadvantages of the state-of-the-art electrochemical drug screening devices are critically discussed. Promising sensing devices have addressed drug susceptibility tests by monitoring (i) cellular, e.g., cell proliferation, adhesion, and detachment for 2D cells and the formation of ionic inter-cell gap junctions for 3D cells), or (ii) extracellular markers, e.g., O2, pH, and metabolic intermediates such as glucose, lactate, and hydrogen peroxide. The advances in these devices are covered here in two parts relying on the aforesaid viability indicators, i.e., cellular and extracellular markers of both 2D and 3D cell models (i.e., spheroids and organ-on-a-chip systems). These advances have aimed at boosting the performance of sensors by utilizing nanomaterials and machine learning. Finally, an outlook on the field's bottlenecks to overcome is provided, seeking to draw new sensing paradigms in electrochemical drug susceptibility tests. Briefly, multisensor, microfluidic, and machine learning-aided sensing devices coupled with 3D cell models stand out as an attractive alternative to offer high-throughput, reproducible, real-time, accurate, and free-calibration predictions of in vivo drug effects. This type of platform can play a key role in steering electrochemical sensors to bridge the translational gap between research and end users in daily anticancer drug susceptibility testing applications.
抗癌药敏试验在药物开发、药代动力学研究和精准肿瘤学等领域发挥着重要作用。在这些测试中,传统上用于测量药物效应的方法——通过确定药物暴露后体外细胞模型的细胞活力——通常是耗时的,并且仅限于终点检测。在这方面,电化学传感器已经成为一种有希望的替代方案,以提高吞吐量和产生实时药代动力学监测。在这篇批判性的综述中,对最先进的电化学药物筛选装置的工作原理、优点和缺点的考虑进行了批判性的讨论。有前途的传感装置通过监测(i)细胞,如2D细胞的细胞增殖、粘附和脱离,以及3D细胞的离子细胞间间隙连接的形成,或(ii)细胞外标记,如O2、pH和代谢中间体,如葡萄糖、乳酸盐和过氧化氢,来解决药物敏感性测试。这些设备的进展在这里分为两部分,依赖于上述活力指标,即2D和3D细胞模型(即球体和器官芯片系统)的细胞和细胞外标记。这些进步旨在通过利用纳米材料和机器学习来提高传感器的性能。最后,展望了该领域有待克服的瓶颈,寻求在电化学药物敏感性测试中绘制新的传感范式。简而言之,多传感器、微流体和机器学习辅助传感设备与3D细胞模型相结合,作为一种有吸引力的替代方案,可以提供高通量、可重复、实时、准确和自由校准的体内药物效应预测。这种类型的平台可以在指导电化学传感器方面发挥关键作用,以弥合研究和最终用户在日常抗癌药物敏感性测试应用中的转化差距。
{"title":"Review on electrochemical sensors for anticancer drug susceptibility testing","authors":"Paula C.R. Corsato, Christian O. Silva, Iris R.S. Ribeiro, Renato S. Lima","doi":"10.1016/j.aca.2025.344905","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344905","url":null,"abstract":"Anticancer drug susceptibility tests play an essential role in areas such as drug development, pharmacokinetic research, and precision oncology. Across these tests, the methods that are traditionally used for gauging the drug effect—by determining the cell viability of <em>in vitro</em> cell models after drug exposure—are commonly time-consuming and limited to end-point detection. In this regard, electrochemical sensors have emerged as a promising alternative to increase throughput and yield real-time pharmacokinetic monitoring. In this critical review, considerations on the operating principles, advantages, and disadvantages of the state-of-the-art electrochemical drug screening devices are critically discussed. Promising sensing devices have addressed drug susceptibility tests by monitoring (i) cellular, e.g., cell proliferation, adhesion, and detachment for 2D cells and the formation of ionic inter-cell gap junctions for 3D cells), or (ii) extracellular markers, e.g., O<sub>2</sub>, pH, and metabolic intermediates such as glucose, lactate, and hydrogen peroxide. The advances in these devices are covered here in two parts relying on the aforesaid viability indicators, i.e., cellular and extracellular markers of both 2D and 3D cell models (i.e., spheroids and organ-on-a-chip systems). These advances have aimed at boosting the performance of sensors by utilizing nanomaterials and machine learning. Finally, an outlook on the field's bottlenecks to overcome is provided, seeking to draw new sensing paradigms in electrochemical drug susceptibility tests. Briefly, multisensor, microfluidic, and machine learning-aided sensing devices coupled with 3D cell models stand out as an attractive alternative to offer high-throughput, reproducible, real-time, accurate, and free-calibration predictions of <em>in vivo</em> drug effects. This type of platform can play a key role in steering electrochemical sensors to bridge the translational gap between research and end users in daily anticancer drug susceptibility testing applications.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"103 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554393","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
Electrospun core (PVA-ninhydrin)-sheath (PVP) fibrous film for multi-level feature visualization and quantitative analysis of latent fingerprints 用于潜在指纹多层次特征可视化和定量分析的静电纺丝芯(PVA-ninhydrin)鞘(PVP)纤维膜
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-20 DOI: 10.1016/j.aca.2025.344911
Shiyue Ma , Hongyu Chen , Xin Du , Lu Liu , Yanfeng Zhang , Rongliang Ma , Yongqiang Wen , Meiqin Zhang

Background

The development of level 3 features in various latent fingerprints (LFPs) is pivotal to improving the matching accuracy of damaged fingerprints. Among the various LFP development methods, the traditional ninhydrin method is widely employed in forensic science. However, it exhibits two key limitations: first, it is only effective for developing eccrine LFPs; second, it can only reveal level 2 features. These constraints compromise the extraction efficiency and utility of the developed fingerprints, thereby restricting the method's applicable scenarios.

Results

We report the fabrication of core (polyvinyl alcohol ninhydrin (PVA-ninhydrin))-sheath (polyvinyl pyrrolidone (PVP)) fibrous films by using coaxial electrospinning technology for high-level development of various LFPs. The film achieves safe, fast and chemical visualization of eccrine, sebaceous and natural LFPs with levels 1–3 features, showing a better visualization effect than ninhydrin solution and PVA-Nin fibrous film. It may be attributed to high specific surface area of thin film with uniform distribution of ninhydrin in the PVA core for high proportion of active sites of amino acids, which enables the film to have strong sweat adsorption and spreading properties. It further allows a more thorough and complete reaction between ninhydrin and the amino acids in the fingerprint residues that enhances the contrast of the developed photos. The statistical analyses of sweat pore count, ridge width, and pore spacing show high consistency and accuracy.

Significant

This study developed the core (PVA-ninhydrin)-sheath (PVP) fibrous films to achieve safe, fast and chemical visualization of eccrine, sebaceous and natural LFPs with levels 1–3 features and accurate quantitative analysis of the developed eccrine one. Moreover, even the interspacing and angles between sweat pores can be derived from level 3 features of the developed fingerprints. These results lay a robust foundation for subsequent fingerprint identification and personal recognition.
各种潜在指纹中3级特征的发展对于提高受损指纹的匹配精度至关重要。在各种LFP显影方法中,传统的茚三酮法在法医学中应用广泛。然而,它表现出两个关键的局限性:首先,它只对发展内分泌lfp有效;其次,它只能显示二级功能。这些制约因素影响了已开发指纹的提取效率和实用性,从而限制了该方法的应用场景。结果采用同轴静电纺丝技术制备了芯部(聚乙烯醇茚三酮(PVA-ninhydrin))-鞘部(聚乙烯醇吡啶酮(PVP))纤维膜,用于各种lfp的高水平发展。该膜实现了内分泌、皮脂腺和天然lfp的安全、快速、化学可视化,具有1-3级特征,比茚三酮溶液和PVA-Nin纤维膜具有更好的可视化效果。这可能是由于薄膜的比表面积高,氨基酸活性位点比例高,茚三酮均匀分布在PVA芯中,使薄膜具有较强的吸汗和扩散性能。它进一步使茚三酮和指纹残留物中的氨基酸之间的反应更加彻底和完全,从而增强了冲洗照片的对比度。汗孔数、脊宽和孔间距的统计分析结果具有较高的一致性和准确性。本研究开发了核心(PVA-ninhydrin)-鞘(PVP)纤维膜,实现了具有1-3级特征的内分泌、皮脂腺和天然lfp的安全、快速和化学可视化,并对所开发的内分泌膜进行了准确的定量分析。此外,汗孔之间的间距和角度也可以从指纹的三级特征中得到。这些结果为后续的指纹识别和个人识别奠定了坚实的基础。
{"title":"Electrospun core (PVA-ninhydrin)-sheath (PVP) fibrous film for multi-level feature visualization and quantitative analysis of latent fingerprints","authors":"Shiyue Ma ,&nbsp;Hongyu Chen ,&nbsp;Xin Du ,&nbsp;Lu Liu ,&nbsp;Yanfeng Zhang ,&nbsp;Rongliang Ma ,&nbsp;Yongqiang Wen ,&nbsp;Meiqin Zhang","doi":"10.1016/j.aca.2025.344911","DOIUrl":"10.1016/j.aca.2025.344911","url":null,"abstract":"<div><h3>Background</h3><div>The development of level 3 features in various latent fingerprints (LFPs) is pivotal to improving the matching accuracy of damaged fingerprints. Among the various LFP development methods, the traditional ninhydrin method is widely employed in forensic science. However, it exhibits two key limitations: first, it is only effective for developing eccrine LFPs; second, it can only reveal level 2 features. These constraints compromise the extraction efficiency and utility of the developed fingerprints, thereby restricting the method's applicable scenarios.</div></div><div><h3>Results</h3><div>We report the fabrication of core (polyvinyl alcohol ninhydrin (PVA-ninhydrin))-sheath (polyvinyl pyrrolidone (PVP)) fibrous films by using coaxial electrospinning technology for high-level development of various LFPs. The film achieves safe, fast and chemical visualization of eccrine, sebaceous and natural LFPs with levels 1–3 features, showing a better visualization effect than ninhydrin solution and PVA-Nin fibrous film. It may be attributed to high specific surface area of thin film with uniform distribution of ninhydrin in the PVA core for high proportion of active sites of amino acids, which enables the film to have strong sweat adsorption and spreading properties. It further allows a more thorough and complete reaction between ninhydrin and the amino acids in the fingerprint residues that enhances the contrast of the developed photos. The statistical analyses of sweat pore count, ridge width, and pore spacing show high consistency and accuracy.</div></div><div><h3>Significant</h3><div>This study developed the core (PVA-ninhydrin)-sheath (PVP) fibrous films to achieve safe, fast and chemical visualization of eccrine, sebaceous and natural LFPs with levels 1–3 features and accurate quantitative analysis of the developed eccrine one. Moreover, even the interspacing and angles between sweat pores can be derived from level 3 features of the developed fingerprints. These results lay a robust foundation for subsequent fingerprint identification and personal recognition.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344911"},"PeriodicalIF":6.0,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554392","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
Smartphone-based molecular imprinting electrochemiluminescence microscope for non-invasive alpha-fetoprotein visual quantitation 基于智能手机的分子印迹电化学发光显微镜用于无创甲胎蛋白视觉定量
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-20 DOI: 10.1016/j.aca.2025.344922
Yusheng Wu , Shenglan Hu , Lixin Xu , Juan Yang , Na Wang , Biyang Deng

Background

Alpha-fetoprotein (AFP) is a marker of liver cancer. Patients are harmed by the blood sample collection. Saliva samples are painless, safe, and easy to collect. The development of detecting AFP in saliva is important. Electrochemiluminescence (ECL) has low background signal, a wide dynamic range, and high sensitivity, but traditional ECL methods use a photomultiplier tube as a detector, which is bulky and delicate, and limits the spatial and temporal resolution of ECL. ECL microscopy (ECLM) is a new imaging technique that combines ECL with optical microscopy and makes up for the shortcomings of traditional ECL.

Results

In this study, we developed a smartphone-based electrochemiluminescence microscope (SECLM), utilizing a gold nanorods@polyethyleneimine@ferrocene composite as a quencher and Ru-bpy as the emitter. The SECLM was integrated with molecular imprinting and an immunological technique for the quantitative visual detection of AFP in saliva samples. The method's detection sensitivity was significantly enhanced by the presence of multiple quenching mechanisms, including a blocking effect, inner filter effect, and electron transfer. This study presents a novel strategy to improve the sensing performance of molecular-imprinted ECL sensors. The method demonstrated a linear detection range of 0.01–100 pg/mL, with a limit of detection of 4.5 fg/mL. Comparative analyses with existing techniques indicated that this method achieves a low limit of detection, high sensitivity, and excellent stability, comparable to traditional ECL sensors.

Significance

This novel quantitative visual technique may enhance biomarker detection, and offer a reliable means for disease diagnosis and screening, and open new avenues for the development of sensing methodologies. This expands the application scope of ECLM and is expected to realize the rapid and sensitive biomarker detection for point-of-care and on-site detection. MI-ECLM provides a new tool for disease diagnosis, physiological activity exploration, pathogenesis and molecular biology researches.
甲胎蛋白(AFP)是肝癌的标志物。病人会因为采集血样而受到伤害。唾液样本无痛、安全、易于收集。唾液中AFP检测技术的发展具有重要意义。电化学发光(ECL)具有背景信号低、动态范围宽、灵敏度高的特点,但传统的ECL方法采用光电倍增管作为探测器,体积大、精细,限制了ECL的时空分辨率。ECLM是一种将ECL与光学显微镜相结合的新型成像技术,弥补了传统ECL的不足。在本研究中,我们开发了一种基于智能手机的电化学发光显微镜(隐居),利用金nanorods@polyethyleneimine@二茂铁复合材料作为猝灭剂,Ru-bpy作为发射器。该方法结合了分子印迹和免疫技术,用于唾液样本中AFP的定量视觉检测。由于存在多种猝灭机制,包括阻断效应、内过滤效应和电子转移,该方法的检测灵敏度显著提高。本研究提出了一种提高分子印迹ECL传感器传感性能的新策略。该方法线性检测范围为0.01 ~ 100 pg/mL,检出限为4.5 fg/mL。与现有技术的对比分析表明,该方法具有检测限低、灵敏度高、稳定性好等优点,可与传统ECL传感器相媲美。这种新的定量视觉技术可以增强生物标志物的检测,为疾病诊断和筛查提供可靠的手段,并为传感方法的发展开辟新的途径。这扩大了ECLM的应用范围,有望实现在护理点和现场检测的快速、灵敏的生物标志物检测。MI-ECLM为疾病诊断、生理活性探索、发病机制和分子生物学研究提供了新的工具。
{"title":"Smartphone-based molecular imprinting electrochemiluminescence microscope for non-invasive alpha-fetoprotein visual quantitation","authors":"Yusheng Wu ,&nbsp;Shenglan Hu ,&nbsp;Lixin Xu ,&nbsp;Juan Yang ,&nbsp;Na Wang ,&nbsp;Biyang Deng","doi":"10.1016/j.aca.2025.344922","DOIUrl":"10.1016/j.aca.2025.344922","url":null,"abstract":"<div><h3>Background</h3><div>Alpha-fetoprotein (AFP) is a marker of liver cancer. Patients are harmed by the blood sample collection. Saliva samples are painless, safe, and easy to collect. The development of detecting AFP in saliva is important. Electrochemiluminescence (ECL) has low background signal, a wide dynamic range, and high sensitivity, but traditional ECL methods use a photomultiplier tube as a detector, which is bulky and delicate, and limits the spatial and temporal resolution of ECL. ECL microscopy (ECLM) is a new imaging technique that combines ECL with optical microscopy and makes up for the shortcomings of traditional ECL.</div></div><div><h3>Results</h3><div>In this study, we developed a smartphone-based electrochemiluminescence microscope (SECLM), utilizing a gold nanorods@polyethyleneimine@ferrocene composite as a quencher and Ru-bpy as the emitter. The SECLM was integrated with molecular imprinting and an immunological technique for the quantitative visual detection of AFP in saliva samples. The method's detection sensitivity was significantly enhanced by the presence of multiple quenching mechanisms, including a blocking effect, inner filter effect, and electron transfer. This study presents a novel strategy to improve the sensing performance of molecular-imprinted ECL sensors. The method demonstrated a linear detection range of 0.01–100 pg/mL, with a limit of detection of 4.5 fg/mL. Comparative analyses with existing techniques indicated that this method achieves a low limit of detection, high sensitivity, and excellent stability, comparable to traditional ECL sensors.</div></div><div><h3>Significance</h3><div>This novel quantitative visual technique may enhance biomarker detection, and offer a reliable means for disease diagnosis and screening, and open new avenues for the development of sensing methodologies. This expands the application scope of ECLM and is expected to realize the rapid and sensitive biomarker detection for point-of-care and on-site detection. MI-ECLM provides a new tool for disease diagnosis, physiological activity exploration, pathogenesis and molecular biology researches.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344922"},"PeriodicalIF":6.0,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554394","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
Ligation-mediated circuit-driven cascade amplification with high utilization rate of template for lncRNA MALAT1 detection in cancer mice tissues 结扎介导电路驱动级联扩增,模板利用率高,用于肿瘤小鼠组织中lncRNA MALAT1检测
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-19 DOI: 10.1016/j.aca.2025.344912
Yuyan Huang , Fan Huang , Qianqian Du , Rui Yu , Jingfeng Lan , Junwei Luo , Hongli Chen , Huige Zhang

Background

Long non-coding RNAs (lncRNAs) are essential in the regulation of gene expression and the abnormal expression of them are considered as one of the driving forces for the development and progression of cancers including apoptosis regulation, migration and invasion of cancer cells. Especially, it has been confirmed the diagnostic and prognostic significance of long non-coding RNA metastasis-associated lung adenocarcinoma transcript 1 (MALAT1) in breast, cervical, lung and other cancers. Thus, lncRNA MALAT1 has emerged as significant biomarker and therapeutic target.

Results

Here, we devised a highly sensitive method for detecting lncRNA MALAT1 by utilizing the ligation-mediated circuit-driven cascade amplification with high utilization rate of template. A special template was designed to initiate the ligation reaction occurring within and between templates in the presence of MALAT1, generating circle template for rolling circle amplification (RCA) and linear template for dual exponential amplification (EXPAR). Subsequently, the primer hybridized with the ligated templates to initiate the RCA and dual EXPAR simultaneously, generating three different products for producing enhanced fluorescent signal. Moreover, the method could be operated by a simple “mixing” procedure for highly selective and sensitive detection of lncRNA MALAT1 with a detection limit of 0.81 aM, and it has been successfully validated for detecting MALAT1 in the extract of cancer mice tissues, demonstrating its potential for practical implementation in MALAT1-related diagnosis and prognosis response.

Significance

Furthermore, the method provides a new way for transforming lncRNA MALAT1 into multiple short DNAs by isothermal amplification with only three DNA reactants, holding the promise for ultrasensitive, selective and cost-effective detection of other long non-coding RNAs.
长链非编码rna (long non-coding RNAs, lncRNAs)在基因表达调控中起着至关重要的作用,其异常表达被认为是肿瘤发生发展的驱动力之一,包括调控癌细胞凋亡、迁移和侵袭等。特别是长链非编码RNA转移相关肺腺癌转录本1 (MALAT1)在乳腺癌、宫颈癌、肺癌等癌症中的诊断和预后意义已被证实。因此,lncRNA MALAT1已成为重要的生物标志物和治疗靶点。结果我们设计了一种高灵敏度的检测lncRNA MALAT1的方法,利用连接介导的电路驱动级联扩增,模板利用率高。设计了一种特殊模板,在MALAT1存在的情况下启动模板内部和模板之间的连接反应,生成用于滚动圈扩增(RCA)的圆形模板和用于双指数扩增(EXPAR)的线性模板。随后,引物与连接的模板杂交,同时启动RCA和双EXPAR,产生三种不同的产物,以产生增强的荧光信号。此外,该方法可以通过简单的“混合”操作,对lncRNA MALAT1进行高选择性和高灵敏度的检测,检测限为0.81 aM,并已成功用于检测癌小鼠组织提取物中的MALAT1,显示了其在MALAT1相关诊断和预后反应中的实际应用潜力。此外,该方法提供了一种仅用三种DNA反应物等温扩增将lncRNA MALAT1转化为多个短DNA的新方法,有望对其他长链非编码rna进行超灵敏、选择性和低成本的检测。
{"title":"Ligation-mediated circuit-driven cascade amplification with high utilization rate of template for lncRNA MALAT1 detection in cancer mice tissues","authors":"Yuyan Huang ,&nbsp;Fan Huang ,&nbsp;Qianqian Du ,&nbsp;Rui Yu ,&nbsp;Jingfeng Lan ,&nbsp;Junwei Luo ,&nbsp;Hongli Chen ,&nbsp;Huige Zhang","doi":"10.1016/j.aca.2025.344912","DOIUrl":"10.1016/j.aca.2025.344912","url":null,"abstract":"<div><h3>Background</h3><div>Long non-coding RNAs (lncRNAs) are essential in the regulation of gene expression and the abnormal expression of them are considered as one of the driving forces for the development and progression of cancers including apoptosis regulation, migration and invasion of cancer cells. Especially, it has been confirmed the diagnostic and prognostic significance of long non-coding RNA metastasis-associated lung adenocarcinoma transcript 1 (MALAT1) in breast, cervical, lung and other cancers. Thus, lncRNA MALAT1 has emerged as significant biomarker and therapeutic target.</div></div><div><h3>Results</h3><div>Here, we devised a highly sensitive method for detecting lncRNA MALAT1 by utilizing the ligation-mediated circuit-driven cascade amplification with high utilization rate of template. A special template was designed to initiate the ligation reaction occurring within and between templates in the presence of MALAT1, generating circle template for rolling circle amplification (RCA) and linear template for dual exponential amplification (EXPAR). Subsequently, the primer hybridized with the ligated templates to initiate the RCA and dual EXPAR simultaneously, generating three different products for producing enhanced fluorescent signal. Moreover, the method could be operated by a simple “mixing” procedure for highly selective and sensitive detection of lncRNA MALAT1 with a detection limit of 0.81 aM, and it has been successfully validated for detecting MALAT1 in the extract of cancer mice tissues, demonstrating its potential for practical implementation in MALAT1-related diagnosis and prognosis response.</div></div><div><h3>Significance</h3><div>Furthermore, the method provides a new way for transforming lncRNA MALAT1 into multiple short DNAs by isothermal amplification with only three DNA reactants, holding the promise for ultrasensitive, selective and cost-effective detection of other long non-coding RNAs.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344912"},"PeriodicalIF":6.0,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145546136","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
Fluorescent aptasensor based on magnetic bead–assisted displacement reaction for monitoring vancomycin in plasma 基于磁珠辅助位移反应的荧光体传感器监测血浆中万古霉素
IF 6 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-11-19 DOI: 10.1016/j.aca.2025.344895
Cheng-Shiuan Hsieh , Hsu-Yun Tsai , Ting-Chien Tsai , Yang-Chun Wang , Yi-Tung Cheng , Jing-Ru Liou , Meng-Yu Liu , Yen-Ling Chen , Chien-Chin Chen

Background

Vancomycin is a glycopeptide antibiotic commonly prescribed for infection by methicillin-resistant Staphylococcus aureus. Due to its narrow therapeutic window and time-dependent bactericidal activity, therapeutic drug monitoring is essential to optimize dosing and minimize toxicity. Immunoassay-based approaches have traditionally been widely used; however, they often require long assay times and are susceptible to matrix interferences, which limit their applicability for rapid clinical use. To enhance the development of point-of-care testing for therapeutic drug monitoring, we developed a fluorescent aptasensor based on a magnetic bead-assisted displacement reaction for the quantification of vancomycin in human plasma.

Results

The sensing mechanism is based on the competition between vancomycin and a complementary single-stranded DNA (cDNA) for binding to a fluorescent aptamer. The cDNA-aptamer complex was immobilized on magnetic beads, and upon addition of vancomycin, the stronger binding affinity between vancomycin and the aptamer displaced the cDNA, releasing the aptamer-vancomycin complex into the supernatant. After magnetic separation, the fluorescence intensity of the supernatant was measured to quantify vancomycin concentration. The optimized experimental conditions were using a 16-mer cDNA and 1 × PBS buffer containing 10 mM MgCl2 at pH 7.0, with a total reaction time of only 15 min. The aptasensor exhibited a linear response for vancomycin in plasma over the range of 1–25 μM, with a low detection limit of 0.5 μM.

Significance

The developed assay was successfully applied to clinical plasma samples, and the results showed good agreement with those obtained by enzyme-linked immunosorbent assay, confirming the accuracy and potential of this aptasensor for clinical application. This aptasensor provides a simple, rapid, and cost-effective strategy for therapeutic drug monitoring of vancomycin in clinical settings.
万古霉素是一种糖肽类抗生素,通常用于治疗耐甲氧西林金黄色葡萄球菌感染。由于其狭窄的治疗窗口和时间依赖的杀菌活性,治疗药物监测是必要的,以优化剂量和尽量减少毒性。传统上广泛使用基于免疫测定的方法;然而,它们通常需要很长的测定时间,并且容易受到基质干扰,这限制了它们在快速临床应用中的适用性。为了促进治疗药物监测的即时检测技术的发展,我们开发了一种基于磁珠辅助位移反应的荧光配体传感器,用于定量人血浆中万古霉素的含量。结果万古霉素的感应机制是基于互补单链DNA (cDNA)与荧光适体结合的竞争机制。将cDNA-适配体复合物固定在磁珠上,加入万古霉素后,万古霉素与适配体之间更强的结合亲和力取代了cDNA,将适配体-万古霉素复合物释放到上清液中。磁分离后测定上清液荧光强度,定量万古霉素浓度。优化后的实验条件为:16链cDNA, 1× PBS缓冲液,含10 mM MgCl2, pH 7.0,总反应时间仅为15 min。该传感器对血浆中万古霉素的检测在1 ~ 25 μM范围内呈线性响应,检测限低至0.5 μM。该方法已成功应用于临床血浆样品中,结果与酶联免疫吸附法吻合较好,证实了该方法的准确性和临床应用潜力。该适配体传感器为临床环境中万古霉素的治疗性药物监测提供了一种简单、快速和具有成本效益的策略。
{"title":"Fluorescent aptasensor based on magnetic bead–assisted displacement reaction for monitoring vancomycin in plasma","authors":"Cheng-Shiuan Hsieh ,&nbsp;Hsu-Yun Tsai ,&nbsp;Ting-Chien Tsai ,&nbsp;Yang-Chun Wang ,&nbsp;Yi-Tung Cheng ,&nbsp;Jing-Ru Liou ,&nbsp;Meng-Yu Liu ,&nbsp;Yen-Ling Chen ,&nbsp;Chien-Chin Chen","doi":"10.1016/j.aca.2025.344895","DOIUrl":"10.1016/j.aca.2025.344895","url":null,"abstract":"<div><h3>Background</h3><div>Vancomycin is a glycopeptide antibiotic commonly prescribed for infection by <em>methicillin-resistant Staphylococcus aureus</em>. Due to its narrow therapeutic window and time-dependent bactericidal activity, therapeutic drug monitoring is essential to optimize dosing and minimize toxicity. Immunoassay-based approaches have traditionally been widely used; however, they often require long assay times and are susceptible to matrix interferences, which limit their applicability for rapid clinical use. To enhance the development of point-of-care testing for therapeutic drug monitoring, we developed a fluorescent aptasensor based on a magnetic bead-assisted displacement reaction for the quantification of vancomycin in human plasma.</div></div><div><h3>Results</h3><div>The sensing mechanism is based on the competition between vancomycin and a complementary single-stranded DNA (cDNA) for binding to a fluorescent aptamer. The cDNA-aptamer complex was immobilized on magnetic beads, and upon addition of vancomycin, the stronger binding affinity between vancomycin and the aptamer displaced the cDNA, releasing the aptamer-vancomycin complex into the supernatant. After magnetic separation, the fluorescence intensity of the supernatant was measured to quantify vancomycin concentration. The optimized experimental conditions were using a 16-mer cDNA and 1 × PBS buffer containing 10 mM MgCl<sub>2</sub> at pH 7.0, with a total reaction time of only 15 min. The aptasensor exhibited a linear response for vancomycin in plasma over the range of 1–25 μM, with a low detection limit of 0.5 μM.</div></div><div><h3>Significance</h3><div>The developed assay was successfully applied to clinical plasma samples, and the results showed good agreement with those obtained by enzyme-linked immunosorbent assay, confirming the accuracy and potential of this aptasensor for clinical application. This aptasensor provides a simple, rapid, and cost-effective strategy for therapeutic drug monitoring of vancomycin in clinical settings.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1383 ","pages":"Article 344895"},"PeriodicalIF":6.0,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145546101","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
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1