Pub Date : 2025-05-01Epub Date: 2025-01-10DOI: 10.1016/j.talanta.2025.127567
Nurimangul Muntiza, Wenbin Zhang, Yuzeng Li, Wenquan Ji, Jin Zhao, Hongfeng Zhang, Qinran Li, Qiliang Deng, Donglan Sun, Tianjun Liu
A novel strategy for cytochrome c selective recognition assisted with cucurbit[6]uril by host-guest interaction via N-terminal epitope imprinting and reversible addition-fragmentation chain transfer (RAFT) polymerization was developed. N-terminal nonapeptide of cytochrome c (GI-9) was used as the epitope template to achieve highly selective recognition of cytochrome c. As a common supramolecule in recent years, cucurbit[6]uril can encapsulate the butyrammonium group of lysine residue to capture the peptide and improve the corresponding spatial orientation by the host-guest interaction for GI-9 or cytochrome c recognition. After cucurbit[6]uril modification and epitope immobilization, the imprinted polymer was synthesized by RAFT polymerization with 2-dodecylsulfanylcarbothioylsulfanyl-2-methylpropanoic acid as chain transfer agent. After template removal, the obtained imprinted particles showed good binding ability to GI-9 (20.28 mg g-1, IF = 4.11) and cytochrome c (36.12 mg g-1, IF = 3.91). With the successive addition of cucurbit[6]uril and RAFT agent, the step-by-step improvement of the IF for cytochrome c recognition further illustrated the effects of supramolecular host-guest interaction and regulation of imprinted polymer chain. The imprinted polymers showed obvious advantages for cytochrome c recognition compared to competitive proteins and had good reusability with the repeated reproduction rate 80.8 % after five cycles of adsorption and desorption. Furthermore, the selective recognition for cytochrome c in adult bovine serum proved its potentiality to be applied in practical samples. All these results demonstrated that the combination of epitope imprinting, cucurbit[6]uril host-guest interaction and RAFT strategy presented an efficient new feasible control method for protein recognition with good selectivity, stability and reusability.
提出了一种通过n端表位印迹和可逆加成-片段链转移(RAFT)聚合的宿主-客体相互作用辅助细胞色素c选择性识别的新策略。以细胞色素c的n端非肽(GI-9)作为表位模板,实现对细胞色素c的高选择性识别。作为近年来常见的超分子,葫芦[6]uril可以包封赖氨酸残基的丁铵基来捕获肽,并通过主客体相互作用提高相应的空间取向,从而实现对GI-9或细胞色素c的识别。以2-十二烷基磺酰碳硫基磺酰-2-甲基丙烷酸为链转移剂,通过RAFT聚合法制备印迹聚合物。模板去除后,印迹颗粒对GI-9 (20.28 mg g-1, IF = 4.11)和细胞色素c (36.12 mg g-1, IF = 3.91)具有良好的结合能力。随着瓜b[6]uril和RAFT试剂的相继加入,IF对细胞色素c识别的逐步提高进一步说明了超分子主客体相互作用和印迹聚合物链调控的作用。印迹聚合物对细胞色素c的识别能力明显优于竞争蛋白,并且具有良好的重复利用性,经过5次吸附和解吸后,重复繁殖率达到80.8%。此外,对成年牛血清中细胞色素c的选择性识别也证明了该方法在实际样品中的应用潜力。这些结果表明,表位印迹、瓜bbbbil宿主-客体相互作用和RAFT策略相结合是一种高效可行的蛋白质识别控制新方法,具有良好的选择性、稳定性和可重用性。
{"title":"Cucurbit[6]uril host-guest interaction assisted N-terminal epitope imprinted particles for cytochrome c recognition prepared by reversible addition-fragmentation chain transfer strategy.","authors":"Nurimangul Muntiza, Wenbin Zhang, Yuzeng Li, Wenquan Ji, Jin Zhao, Hongfeng Zhang, Qinran Li, Qiliang Deng, Donglan Sun, Tianjun Liu","doi":"10.1016/j.talanta.2025.127567","DOIUrl":"10.1016/j.talanta.2025.127567","url":null,"abstract":"<p><p>A novel strategy for cytochrome c selective recognition assisted with cucurbit[6]uril by host-guest interaction via N-terminal epitope imprinting and reversible addition-fragmentation chain transfer (RAFT) polymerization was developed. N-terminal nonapeptide of cytochrome c (GI-9) was used as the epitope template to achieve highly selective recognition of cytochrome c. As a common supramolecule in recent years, cucurbit[6]uril can encapsulate the butyrammonium group of lysine residue to capture the peptide and improve the corresponding spatial orientation by the host-guest interaction for GI-9 or cytochrome c recognition. After cucurbit[6]uril modification and epitope immobilization, the imprinted polymer was synthesized by RAFT polymerization with 2-dodecylsulfanylcarbothioylsulfanyl-2-methylpropanoic acid as chain transfer agent. After template removal, the obtained imprinted particles showed good binding ability to GI-9 (20.28 mg g<sup>-1</sup>, IF = 4.11) and cytochrome c (36.12 mg g<sup>-1</sup>, IF = 3.91). With the successive addition of cucurbit[6]uril and RAFT agent, the step-by-step improvement of the IF for cytochrome c recognition further illustrated the effects of supramolecular host-guest interaction and regulation of imprinted polymer chain. The imprinted polymers showed obvious advantages for cytochrome c recognition compared to competitive proteins and had good reusability with the repeated reproduction rate 80.8 % after five cycles of adsorption and desorption. Furthermore, the selective recognition for cytochrome c in adult bovine serum proved its potentiality to be applied in practical samples. All these results demonstrated that the combination of epitope imprinting, cucurbit[6]uril host-guest interaction and RAFT strategy presented an efficient new feasible control method for protein recognition with good selectivity, stability and reusability.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127567"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982236","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}
Pub Date : 2025-05-01Epub Date: 2025-01-13DOI: 10.1016/j.talanta.2025.127586
Dan Meng, Li Ma, Lei Zhang, Xiaoguang San, Zongsheng Xie, Quan Jin, Jian Qi
Formaldehyde (HCHO) is a harmful volatile organic pollutant, which is commonly found in interior decoration and furniture products. Therefore, it is necessary to develop a gas sensor that can quickly and accurately detect formaldehyde for human health and environmental protection. In order to achieve this goal, in this work, SnS2/SnO2 heterostructure was synthesized by in-situ sulfurization process on the basis of SnO2 nanospheres, and its formaldehyde sensing performance was studied. After testing, it was found that the gas sensor based on SnS2/SnO2 heterojunction has more excellent gas sensing performance than pure SnO2 gas sensor at the same operating temperature (100 °C). Specifically, SnS2/SnO2-2 (Sn:S = 3:2) has the advantages of high sensitivity (4.01 at 0.1 ppm), excellent selectivity, low theoretical detection limit (13.26 ppb), good humidity resistance and long-term stability. The excellent sensing performance of SnS2/SnO2 sensors for formaldehyde detection is mainly attributed to the n-n heterojunction formed by SnS2 and SnO2, which generates a built-in electric field to accelerate the electron transport in the material, the higher oxygen vacancy sites adsorb a large number of reactive gas molecules to promote the oxidation of formaldehyde molecules, and the unique porous structure to promote the transmission and diffusion of gases and increase the surface area to provide more adsorption sites and reactive centers for gas molecules. Therefore, the construction of SnS2/SnO2 heterostructures will be an effective way to develop next-generation formaldehyde gas sensors with higher sensing performance.
{"title":"Oxygen vacancy and interface effect dual modulation of SnS<sub>2</sub>/SnO<sub>2</sub> heterojunction for boosting formaldehyde detection at low temperature.","authors":"Dan Meng, Li Ma, Lei Zhang, Xiaoguang San, Zongsheng Xie, Quan Jin, Jian Qi","doi":"10.1016/j.talanta.2025.127586","DOIUrl":"10.1016/j.talanta.2025.127586","url":null,"abstract":"<p><p>Formaldehyde (HCHO) is a harmful volatile organic pollutant, which is commonly found in interior decoration and furniture products. Therefore, it is necessary to develop a gas sensor that can quickly and accurately detect formaldehyde for human health and environmental protection. In order to achieve this goal, in this work, SnS<sub>2</sub>/SnO<sub>2</sub> heterostructure was synthesized by in-situ sulfurization process on the basis of SnO<sub>2</sub> nanospheres, and its formaldehyde sensing performance was studied. After testing, it was found that the gas sensor based on SnS<sub>2</sub>/SnO<sub>2</sub> heterojunction has more excellent gas sensing performance than pure SnO<sub>2</sub> gas sensor at the same operating temperature (100 °C). Specifically, SnS<sub>2</sub>/SnO<sub>2</sub>-2 (Sn:S = 3:2) has the advantages of high sensitivity (4.01 at 0.1 ppm), excellent selectivity, low theoretical detection limit (13.26 ppb), good humidity resistance and long-term stability. The excellent sensing performance of SnS<sub>2</sub>/SnO<sub>2</sub> sensors for formaldehyde detection is mainly attributed to the n-n heterojunction formed by SnS<sub>2</sub> and SnO<sub>2</sub>, which generates a built-in electric field to accelerate the electron transport in the material, the higher oxygen vacancy sites adsorb a large number of reactive gas molecules to promote the oxidation of formaldehyde molecules, and the unique porous structure to promote the transmission and diffusion of gases and increase the surface area to provide more adsorption sites and reactive centers for gas molecules. Therefore, the construction of SnS<sub>2</sub>/SnO<sub>2</sub> heterostructures will be an effective way to develop next-generation formaldehyde gas sensors with higher sensing performance.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127586"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982300","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}
Pub Date : 2025-05-01Epub Date: 2025-01-08DOI: 10.1016/j.talanta.2025.127560
Yuxiang Du, Qianwen Zhang, Huaxiong Wu, Xiaohuan Liu, Genqiang Chen, Yuesong Liang, Qi Li, Yangxin Gu, Minghui Zhang, Hongxing Wang
Glucose detection is crucial for diagnosis, prevention and treatment of diabetes mellitus. In this work, 10 nm Al2O3 thin film was introduced on the channel of diamond solution-gate field-effect transistor (SGFET) to improve the performance of glucose detection. AFM results show the roughness of channel surface increased after Al2O3 thin film deposition. Then, 1-pyrenebutyric acid-N-hydroxy succinimide ester (Pyr-NHS) and glucose oxidase (GOD) were linked on the channel. The morphology after each modification step was evaluated by SEM, and the result indicated an uneven Al2O3 distribution. XPS spectra further confirmed the effective modification of Pyr-NHS and GOD. In addition, the shifts of transfer characteristics for each concentration of glucose were analyzed, which illustrated a wide linear response (10-8-10-2 M), a high sensitivity (-44.01 mV/log10[glucose concentration]) and a low detection limitation (10-8 M). All these results show an excellent detection performance, which may provide a new idea for the design of diamond SGFET biosensor.
血糖检测对糖尿病的诊断、预防和治疗至关重要。本文在金刚石溶液栅场效应晶体管(SGFET)的沟道上引入10nm Al2O3薄膜,以提高葡萄糖检测的性能。AFM结果表明,Al2O3薄膜沉积后,沟道表面粗糙度增大。然后在通道上连接1-芘丁酸- n -羟基琥珀酰亚胺酯(Pyr-NHS)和葡萄糖氧化酶(GOD)。通过SEM对各改性步骤后的形貌进行了分析,结果表明Al2O3的分布不均匀。XPS光谱进一步证实了Pyr-NHS和GOD的有效修饰。此外,还分析了不同葡萄糖浓度下转移特性的变化,显示出宽线性响应(10-8-10-2 M)、高灵敏度(-44.01 mV/log10[葡萄糖浓度])和低检测限(10-8 M),这些结果显示出良好的检测性能,这可能为金刚石SGFET生物传感器的设计提供新的思路。
{"title":"Improvement of glucose detection using 10 nm Al<sub>2</sub>O<sub>3</sub> thin film on diamond solution-gate field-effect transistor.","authors":"Yuxiang Du, Qianwen Zhang, Huaxiong Wu, Xiaohuan Liu, Genqiang Chen, Yuesong Liang, Qi Li, Yangxin Gu, Minghui Zhang, Hongxing Wang","doi":"10.1016/j.talanta.2025.127560","DOIUrl":"10.1016/j.talanta.2025.127560","url":null,"abstract":"<p><p>Glucose detection is crucial for diagnosis, prevention and treatment of diabetes mellitus. In this work, 10 nm Al<sub>2</sub>O<sub>3</sub> thin film was introduced on the channel of diamond solution-gate field-effect transistor (SGFET) to improve the performance of glucose detection. AFM results show the roughness of channel surface increased after Al<sub>2</sub>O<sub>3</sub> thin film deposition. Then, 1-pyrenebutyric acid-N-hydroxy succinimide ester (Pyr-NHS) and glucose oxidase (GOD) were linked on the channel. The morphology after each modification step was evaluated by SEM, and the result indicated an uneven Al<sub>2</sub>O<sub>3</sub> distribution. XPS spectra further confirmed the effective modification of Pyr-NHS and GOD. In addition, the shifts of transfer characteristics for each concentration of glucose were analyzed, which illustrated a wide linear response (10<sup>-8</sup>-10<sup>-2</sup> M), a high sensitivity (-44.01 mV/log<sub>10</sub>[glucose concentration]) and a low detection limitation (10<sup>-8</sup> M). All these results show an excellent detection performance, which may provide a new idea for the design of diamond SGFET biosensor.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127560"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142998078","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}
Pub Date : 2025-05-01Epub Date: 2025-01-13DOI: 10.1016/j.talanta.2025.127554
Lingyue Guo, Libo Li, Lijun Luo, Tianyan You
Searching for new alternative to tripropylamine (TPrA) with low toxicity and high chemical stability for the tris(4,4'-dicarboxylic acid-2,2'-bipyridyl)ruthenium (II) (Ru(dcbpy)32+) based coreactant electrochemiluminescence (ECL) system is essential for widespread analytical applications. Here, nitrogen-doped graphene quantum dots (NGQDs) have been discovered to significantly amplify the ECL emission and increase the ECL efficiency of Ru(dcbpy)32+ for the first time. However, the mechanism by which NGQDs act as coreactants is not well comprehended. Therefore, various optical and electrochemical technologies were employed to investigate the ECL mechanism. It is proposed that the amino and carboxyl groups on the surface of NGQDs play crucial roles as the coreactant active sites, catalyzing the oxidation of Ru(dcbpy)32+. Based on this foundation, an "on-off-on" ECL aptasensor for the quantification of acetamiprid was developed, exhibiting a broad linear range and a detection limit of 0.056 pM. Satisfactory recoveries, ranging from 98.0 % to 101.6 %, were achieved in pakchoi samples. Consequently, NGQDs could serve as coreactants for Ru(dcbpy)32+, offering new opportunities for constructing a variety of sensors with extensive analytical applications in the ECL field.
{"title":"Amplified electrochemiluminescence of Ru(dcbpy)<sub>3</sub><sup>2+</sup> via coreactant active sites on nitrogen-doped graphene quantum dots.","authors":"Lingyue Guo, Libo Li, Lijun Luo, Tianyan You","doi":"10.1016/j.talanta.2025.127554","DOIUrl":"10.1016/j.talanta.2025.127554","url":null,"abstract":"<p><p>Searching for new alternative to tripropylamine (TPrA) with low toxicity and high chemical stability for the tris(4,4'-dicarboxylic acid-2,2'-bipyridyl)ruthenium (II) (Ru(dcbpy)<sub>3</sub><sup>2+</sup>) based coreactant electrochemiluminescence (ECL) system is essential for widespread analytical applications. Here, nitrogen-doped graphene quantum dots (NGQDs) have been discovered to significantly amplify the ECL emission and increase the ECL efficiency of Ru(dcbpy)<sub>3</sub><sup>2+</sup> for the first time. However, the mechanism by which NGQDs act as coreactants is not well comprehended. Therefore, various optical and electrochemical technologies were employed to investigate the ECL mechanism. It is proposed that the amino and carboxyl groups on the surface of NGQDs play crucial roles as the coreactant active sites, catalyzing the oxidation of Ru(dcbpy)<sub>3</sub><sup>2+</sup>. Based on this foundation, an \"on-off-on\" ECL aptasensor for the quantification of acetamiprid was developed, exhibiting a broad linear range and a detection limit of 0.056 pM. Satisfactory recoveries, ranging from 98.0 % to 101.6 %, were achieved in pakchoi samples. Consequently, NGQDs could serve as coreactants for Ru(dcbpy)<sub>3</sub><sup>2+</sup>, offering new opportunities for constructing a variety of sensors with extensive analytical applications in the ECL field.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127554"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142977187","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}
Polymers and dendrimers are macromolecules, possessing unique and intriguing characteristics, that are widely applied in self-assembled functional materials, green catalysis, drug delivery and sensing devices. Traditional approaches for the structural characterization of polymers and dendrimers involve DLS, GPC, NMR, IR and TG, which provide their physiochemical features and ensemble information, whereas their unimolecular conformation and dispersion also are key features allowing to understand their transporting profile in confined ionic nanochannels. This work demonstrates the nanopore approach for the determination of charged homopolymers, neutral block copolymer and dendrimers under distinct bias potentials and pH conditions. The nanopore translocation properties reveal that the dispersion and transporting of PEI is pH-dependent, and its capture rate is much lower than that of PAA. The neutral block copolymer with longest molecular chain threads through with longest blockage duration, its highest capture rate was achieved in 0.5 M KCl at pH 5 with slow diffusion and high temporal resolution. The two generations of neutral dendrimers could also translocate under bias potentials, probably due to the ions adsorption on the dendrimers and driven by Brownian force. The TEG-81 with larger molecular size translocates with longer residence time and higher blockage ratio, as expected. Both of the dendrimers exhibit a higher blockage ratio at pH 7.4 than either acidic or alkalic condition, indicating a larger stretched conformation adopted under neutral condition. This work presents the analysis of unimolecular charged and neutral polymers and dendrimers, which will be insightful in understanding the self-assembly motion and transfer of synthetic macromolecules in confined space. It also provides a good indication for deciphering the macromolecule-nanopore interplay under electrophoretic condition.
高分子和树状大分子具有独特而有趣的特性,广泛应用于自组装功能材料、绿色催化、药物传递和传感器件等领域。聚合物和树状大分子结构表征的传统方法包括DLS、GPC、NMR、IR和TG,这些方法提供了它们的物理化学特征和系综信息,而它们的单分子构象和分散也是了解它们在受限离子纳米通道中的传输特征的关键特征。这项工作证明了纳米孔方法在不同偏压电位和pH条件下测定带电均聚物、中性嵌段共聚物和树状大分子。纳米孔易位特性表明PEI的分散和输运是ph依赖性的,其捕获率远低于PAA。中性嵌段共聚物分子链最长,阻滞时间最长,在0.5 M KCl、pH 5条件下捕获率最高,扩散速度慢,时间分辨率高。两代中性树状大分子在偏置电位下也会发生转移,这可能是由于离子吸附在树状大分子上,并受到布朗力的驱动。分子尺寸较大的TEG-81易位停留时间较长,堵塞率较高。两种树状大分子在pH 7.4条件下均表现出比酸性或碱性条件下更高的堵塞率,表明在中性条件下采用了更大的拉伸构象。这项工作提出了单分子带电和中性聚合物和树状大分子的分析,这将有助于理解合成大分子在有限空间中的自组装运动和转移。这也为在电泳条件下破译高分子与纳米孔的相互作用提供了良好的指示。
{"title":"Single-molecule resolution of the conformation of polymers and dendrimers with solid-state nanopores.","authors":"Meili Ren, Fupeng Qin, Yue Liu, Daixin Liu, Renata Pereira Lopes, Didier Astruc, Liyuan Liang","doi":"10.1016/j.talanta.2025.127544","DOIUrl":"10.1016/j.talanta.2025.127544","url":null,"abstract":"<p><p>Polymers and dendrimers are macromolecules, possessing unique and intriguing characteristics, that are widely applied in self-assembled functional materials, green catalysis, drug delivery and sensing devices. Traditional approaches for the structural characterization of polymers and dendrimers involve DLS, GPC, NMR, IR and TG, which provide their physiochemical features and ensemble information, whereas their unimolecular conformation and dispersion also are key features allowing to understand their transporting profile in confined ionic nanochannels. This work demonstrates the nanopore approach for the determination of charged homopolymers, neutral block copolymer and dendrimers under distinct bias potentials and pH conditions. The nanopore translocation properties reveal that the dispersion and transporting of PEI is pH-dependent, and its capture rate is much lower than that of PAA. The neutral block copolymer with longest molecular chain threads through with longest blockage duration, its highest capture rate was achieved in 0.5 M KCl at pH 5 with slow diffusion and high temporal resolution. The two generations of neutral dendrimers could also translocate under bias potentials, probably due to the ions adsorption on the dendrimers and driven by Brownian force. The TEG-81 with larger molecular size translocates with longer residence time and higher blockage ratio, as expected. Both of the dendrimers exhibit a higher blockage ratio at pH 7.4 than either acidic or alkalic condition, indicating a larger stretched conformation adopted under neutral condition. This work presents the analysis of unimolecular charged and neutral polymers and dendrimers, which will be insightful in understanding the self-assembly motion and transfer of synthetic macromolecules in confined space. It also provides a good indication for deciphering the macromolecule-nanopore interplay under electrophoretic condition.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127544"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142977263","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}
Pub Date : 2025-05-01Epub Date: 2025-01-10DOI: 10.1016/j.talanta.2025.127570
Qingyang Sha, Xinsheng Li, Xixin Gu, Tao Yuan, Jianli Hua
Hypochlorous acid (HClO/ClO-) is a common ROS that exhibits elevated activity levels in cancer cells. In this study, an ClO--triggered TADF probe, PTZ-MNI, was designed based on a naphthalimide core. PTZ-MNI self-assemble in aqueous environments, exhibiting significantly enhanced fluorescence that demonstrated typical aggregation-induced delayed fluorescence (AIDF) characteristics. The probe not only showed high sensitivity to ClO- but also exhibited remarkable selectivity over other reactive oxygen species and disturbance. PTZ-MNI displayed TADF characteristic, including sensitivity to oxygen in toluene, insensitivity to oxygen in aggregated states that maintain long fluorescence lifetimes, a vertical conformation, and a minimal ΔEST of 0.01 eV. Cell imaging studies showed the probe could trace ClO- by red to green fluorescence in HeLa cell. The colocalization analysis indicated its excellent lysosome-targeting specificity. In addition, PTZ-MNI-O, the compound after oxidation, exhibited effective ROS generation ability and significant PDT effect after irradiation. This work provides guidance for the rational design of responsive TADF luminescent materials used in cell imaging and activatable-PDT.
{"title":"A self-aggregated thermally activated delayed fluorescence nanoprobe for HClO imaging and activatable photodynamic therapy.","authors":"Qingyang Sha, Xinsheng Li, Xixin Gu, Tao Yuan, Jianli Hua","doi":"10.1016/j.talanta.2025.127570","DOIUrl":"10.1016/j.talanta.2025.127570","url":null,"abstract":"<p><p>Hypochlorous acid (HClO/ClO<sup>-</sup>) is a common ROS that exhibits elevated activity levels in cancer cells. In this study, an ClO<sup>-</sup>-triggered TADF probe, PTZ-MNI, was designed based on a naphthalimide core. PTZ-MNI self-assemble in aqueous environments, exhibiting significantly enhanced fluorescence that demonstrated typical aggregation-induced delayed fluorescence (AIDF) characteristics. The probe not only showed high sensitivity to ClO<sup>-</sup> but also exhibited remarkable selectivity over other reactive oxygen species and disturbance. PTZ-MNI displayed TADF characteristic, including sensitivity to oxygen in toluene, insensitivity to oxygen in aggregated states that maintain long fluorescence lifetimes, a vertical conformation, and a minimal ΔE<sub>ST</sub> of 0.01 eV. Cell imaging studies showed the probe could trace ClO<sup>-</sup> by red to green fluorescence in HeLa cell. The colocalization analysis indicated its excellent lysosome-targeting specificity. In addition, PTZ-MNI-O, the compound after oxidation, exhibited effective ROS generation ability and significant PDT effect after irradiation. This work provides guidance for the rational design of responsive TADF luminescent materials used in cell imaging and activatable-PDT.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127570"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982208","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}
Spatial metabolomics offers the combination of molecular identification and localization. As a tool for spatial metabolomics, mass spectrometry imaging (MSI) can provide detailed information on localization. However, molecular annotation with MSI is challenging due to the lack of separation prior to mass spectrometric analysis. Contrarily, surface sampling capillary electrophoresis mass spectrometry (SS-CE-MS) provides detailed molecular information, although the size of the sampling sites is modest. Here, we describe a platform for spatial metabolomics where MSI using pneumatically assisted nanospray desorption electrospray ionization (PA-nano-DESI) is combined with SS-CE-MS to gain both in-depth chemical information and spatial localization from thin tissue sections. We present the workflow, including the user-friendly setup and switching between the techniques, compare the obtained data, and demonstrate a quantitative approach when using the platform for spatial metabolomics of ischemic stroke.
{"title":"Spatial metabolomics platform combining mass spectrometry imaging and in-depth chemical characterization with capillary electrophoresis.","authors":"Leonidas Mavroudakis, Anastasia Golubova, Ingela Lanekoff","doi":"10.1016/j.talanta.2024.127460","DOIUrl":"10.1016/j.talanta.2024.127460","url":null,"abstract":"<p><p>Spatial metabolomics offers the combination of molecular identification and localization. As a tool for spatial metabolomics, mass spectrometry imaging (MSI) can provide detailed information on localization. However, molecular annotation with MSI is challenging due to the lack of separation prior to mass spectrometric analysis. Contrarily, surface sampling capillary electrophoresis mass spectrometry (SS-CE-MS) provides detailed molecular information, although the size of the sampling sites is modest. Here, we describe a platform for spatial metabolomics where MSI using pneumatically assisted nanospray desorption electrospray ionization (PA-nano-DESI) is combined with SS-CE-MS to gain both in-depth chemical information and spatial localization from thin tissue sections. We present the workflow, including the user-friendly setup and switching between the techniques, compare the obtained data, and demonstrate a quantitative approach when using the platform for spatial metabolomics of ischemic stroke.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127460"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976767","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}
Bacterial bloodstream infections cause high morbidity and mortality. Although bacteria can be detected by various methods, culture methods are often used for the detection of live, accurate, reproducible, and selective bacterial identification. However, the culture method is time-consuming, and clinicians often start treatment immediately due to the long determination time. This reduces the bacterial density detectable by culture, and in some cases, makes determination difficult. To overcome this challenge, we propose a method that directly combines bacteriophage-based lysis with quantitative PCR (qPCR). This method enables the simple and rapid detection of bacteria without the need for pre-concentration or DNA extraction steps. Escherichia coli K12 (E. coli K12) was used as the model bacterium, and bacteria lysed by the E. coli K12-specific bacteriophage were detected using qPCR. The total analysis time was less than 3 h, and only live bacterial cells were selectively lysed. The method was also used to detect bacteria spiked into reference plasma samples, and bacterial DNA was detected via qPCR. The results obtained from the calibration graph created with cultured bacteria and the one created by spiking bacteria into reference plasma were consistent. The similarities between the calibration graphs from both methods were found to be in the range of 92-102.7 %. The LOD and LOQ values for bacteria spiked into reference plasma were calculated as 14.80 and 3.5x10³ CFU/mL, respectively.
{"title":"Bacteriophage-based live bacteria detection for rapid infection diagnosis.","authors":"Merve Calimci, Tugba Tezcan, Emine Kubra Tayyarcan, Kubra Guven, Ismail Hakki Boyaci, Ugur Tamer","doi":"10.1016/j.talanta.2025.127569","DOIUrl":"10.1016/j.talanta.2025.127569","url":null,"abstract":"<p><p>Bacterial bloodstream infections cause high morbidity and mortality. Although bacteria can be detected by various methods, culture methods are often used for the detection of live, accurate, reproducible, and selective bacterial identification. However, the culture method is time-consuming, and clinicians often start treatment immediately due to the long determination time. This reduces the bacterial density detectable by culture, and in some cases, makes determination difficult. To overcome this challenge, we propose a method that directly combines bacteriophage-based lysis with quantitative PCR (qPCR). This method enables the simple and rapid detection of bacteria without the need for pre-concentration or DNA extraction steps. Escherichia coli K12 (E. coli K12) was used as the model bacterium, and bacteria lysed by the E. coli K12-specific bacteriophage were detected using qPCR. The total analysis time was less than 3 h, and only live bacterial cells were selectively lysed. The method was also used to detect bacteria spiked into reference plasma samples, and bacterial DNA was detected via qPCR. The results obtained from the calibration graph created with cultured bacteria and the one created by spiking bacteria into reference plasma were consistent. The similarities between the calibration graphs from both methods were found to be in the range of 92-102.7 %. The LOD and LOQ values for bacteria spiked into reference plasma were calculated as 14.80 and 3.5x10³ CFU/mL, respectively.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127569"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982219","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}
Near-infrared (NIR) spectroscopy analysis technology has become a widely utilized analytical tool in various fields due to its convenience and efficiency. However, with the promotion of instrument precision, the spectral dimension can now be expanded to include hundreds of dimensions. This expansion results in time-consuming modeling processes and a decrease in model performance. Hence, it is crucial to carefully choose representative features before constructing models. This paper focuses on the limitations of filter algorithms, which can only sort features and cannot directly determine the best subset of features. A hybrid method of combination of the Max-Relevance Min-Redundancy (mRMR) algorithm and the Genetic Algorithm (GA), as well as filter and wrapper feature selection methods, are combined to select appropriate features automatically. This hybrid algorithm retains the features in each individual that are considered to have a strong correlation and low redundancy by the mRMR algorithms during each iteration of the GA. On the other hand, it deletes the features that are regarded as having little correlation or high redundancy. Through the process of iteration, the feature subset is continuously optimized. We use the proposed hybrid method to select features on two datasets and establish various models to verify our proposed method in this paper. The experimental results indicate the feature selection approach, which combines mRMR with the GA, covers the advantages of both feature selection methods. This approach can select features that show good predictive performance. When compared with other common feature selection methods, such as the Uninformative Variable Elimination algorithm (UVE), Competitive Adaptive Reweighted Sampling algorithm (CARS), Successive Projections Algorithm (SPA), Iteratively Retains Informative Variables (IRIV), and GA, the hybrid algorithm can select a larger number of feature variables that are both representative and informative, additionally, it significantly enhances the predictive performance of the model.
近红外(NIR)光谱分析技术因其便捷、高效的特点,已成为各领域广泛使用的分析工具。然而,随着仪器精度的提高,光谱维度现在可以扩展到数百个维度。这种扩展导致建模过程耗时,模型性能下降。因此,在构建模型之前仔细选择具有代表性的特征至关重要。过滤算法只能对特征进行排序,不能直接确定最佳特征子集,本文重点讨论过滤算法的局限性。本文结合了最大相关性最小冗余(mRMR)算法和遗传算法(GA)的混合方法,以及过滤器和包装特征选择方法,来自动选择合适的特征。在遗传算法的每次迭代中,这种混合算法保留了 mRMR 算法认为每个个体中相关性强、冗余度低的特征。另一方面,它删除了被认为相关性小或冗余度高的特征。通过迭代过程,特征子集不断得到优化。本文使用所提出的混合方法在两个数据集上选择特征,并建立各种模型来验证我们所提出的方法。实验结果表明,mRMR 与 GA 结合的特征选择方法涵盖了两种特征选择方法的优点。这种方法可以选择出具有良好预测性能的特征。与其他常见的特征选择方法,如无信息变量消除算法(UVE)、竞争性自适应重加权采样算法(CARS)、连续投影算法(SPA)、迭代保留有信息变量算法(IRIV)和 GA 相比,混合算法可以选择更多既有代表性又有信息量的特征变量,而且还能显著提高模型的预测性能。
{"title":"Wavelength selection method for near-infrared spectroscopy based on the combination of mutual information and genetic algorithm.","authors":"Xiao-Hui Ma, Zheng-Guang Chen, Shuo Liu, Jin-Ming Liu, Xue-Song Tian","doi":"10.1016/j.talanta.2025.127573","DOIUrl":"10.1016/j.talanta.2025.127573","url":null,"abstract":"<p><p>Near-infrared (NIR) spectroscopy analysis technology has become a widely utilized analytical tool in various fields due to its convenience and efficiency. However, with the promotion of instrument precision, the spectral dimension can now be expanded to include hundreds of dimensions. This expansion results in time-consuming modeling processes and a decrease in model performance. Hence, it is crucial to carefully choose representative features before constructing models. This paper focuses on the limitations of filter algorithms, which can only sort features and cannot directly determine the best subset of features. A hybrid method of combination of the Max-Relevance Min-Redundancy (mRMR) algorithm and the Genetic Algorithm (GA), as well as filter and wrapper feature selection methods, are combined to select appropriate features automatically. This hybrid algorithm retains the features in each individual that are considered to have a strong correlation and low redundancy by the mRMR algorithms during each iteration of the GA. On the other hand, it deletes the features that are regarded as having little correlation or high redundancy. Through the process of iteration, the feature subset is continuously optimized. We use the proposed hybrid method to select features on two datasets and establish various models to verify our proposed method in this paper. The experimental results indicate the feature selection approach, which combines mRMR with the GA, covers the advantages of both feature selection methods. This approach can select features that show good predictive performance. When compared with other common feature selection methods, such as the Uninformative Variable Elimination algorithm (UVE), Competitive Adaptive Reweighted Sampling algorithm (CARS), Successive Projections Algorithm (SPA), Iteratively Retains Informative Variables (IRIV), and GA, the hybrid algorithm can select a larger number of feature variables that are both representative and informative, additionally, it significantly enhances the predictive performance of the model.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127573"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982302","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}
Accurately detecting cysteine (Cys) in vivo is crucial for diagnosing Cys-related diseases. A novel ratiometric fluorescent probe featuring dual near-infrared emission is developed in this study for the in vivo ratio imaging of Cys. The probe comprises a hemicyanine organic small-molecule dye (HCy-CYS) with specific Cys recognition capabilities covalently coupled with carbon dots (CDs) synthesized using glutathione (GSH) as the carbon source (GCDs), forming a unique composite nanofluorescent probe (GCDs@CYS). The probe undergoes a specific reaction with acrylate upon the addition of Cys, converting HCy-CYS to HCy-OH. Consequently, the GCD fluorescence intensity at 685 nm gradually decreases, whereas that of HCy-OH at 720 nm progressively increases, yielding a ratiometric fluorescence signal. Notably, both emission wavelengths of the probe exceed 650 nm, thereby effectively mitigating the interference from background signals during cellular and in vivo imaging. Furthermore, the probe demonstrates high specificity for Cys, enabling its differentiation from homocysteine and GSH. The Cys concentration and fluorescence ratiometric intensity exhibit a strong linear correlation at 10-150 μM with a detection limit of 0.95 μM. These results indicate that the ratiometric fluorescent probe can serve as a valuable tool for monitoring Cys-related physiological or pathological processes.
{"title":"A ratiometric fluorescent probe with dual near infrared emission for in vivo ratio imaging of cysteine.","authors":"Bing Zheng, Shulong Wang, Jiayao Xu, Lixian Huang, Shulin Zhao","doi":"10.1016/j.talanta.2025.127564","DOIUrl":"10.1016/j.talanta.2025.127564","url":null,"abstract":"<p><p>Accurately detecting cysteine (Cys) in vivo is crucial for diagnosing Cys-related diseases. A novel ratiometric fluorescent probe featuring dual near-infrared emission is developed in this study for the in vivo ratio imaging of Cys. The probe comprises a hemicyanine organic small-molecule dye (HCy-CYS) with specific Cys recognition capabilities covalently coupled with carbon dots (CDs) synthesized using glutathione (GSH) as the carbon source (GCDs), forming a unique composite nanofluorescent probe (GCDs@CYS). The probe undergoes a specific reaction with acrylate upon the addition of Cys, converting HCy-CYS to HCy-OH. Consequently, the GCD fluorescence intensity at 685 nm gradually decreases, whereas that of HCy-OH at 720 nm progressively increases, yielding a ratiometric fluorescence signal. Notably, both emission wavelengths of the probe exceed 650 nm, thereby effectively mitigating the interference from background signals during cellular and in vivo imaging. Furthermore, the probe demonstrates high specificity for Cys, enabling its differentiation from homocysteine and GSH. The Cys concentration and fluorescence ratiometric intensity exhibit a strong linear correlation at 10-150 μM with a detection limit of 0.95 μM. These results indicate that the ratiometric fluorescent probe can serve as a valuable tool for monitoring Cys-related physiological or pathological processes.</p>","PeriodicalId":435,"journal":{"name":"Talanta","volume":"286 ","pages":"127564"},"PeriodicalIF":5.6,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968969","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}