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Copper doped carbon dots for selective determination of regulated aniline additives and safe hair dyeing
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-14 DOI: 10.1016/j.aca.2025.344071
Zhanghong Guo, Lin Zhou, Liping Zhang, Haining Cui, Jinxin Ma, Chan Wang, Qijun Song

Background

Hair dyes, as common daily chemical products, have been integrated into human daily life. However, the aniline additives contained in traditional hair dyes pose potential threats to health. Therefore, it is of great importance to develop an eco-friendly and convenient detection method and to explore safe alternatives. In this context, enzymatic catalysis technology has received widespread attention due to its safety and eco-friendliness.

Results

Herein, copper-doped carbon dots (CuCDs) with laccase-like activity were prepared by a one-step calcination of copper sulfate, amaranth and ammonium chloride. The resultant CuCDs are monodispersed ellipsoidal crystals with an average diameter of 3.4 nm and active copper centers similar to that of natural laccase. Enzyme kinetics experiments demonstrated that the maximum rate constant (Vmax) obtained from CuCDs is 59 times greater than that of natural laccase, and the Michaelis-Menten constant (Km) is only about half that of natural laccase, indicating a high affinity for laccase substrate. The CuCDs also exhibited a superior stability in comparison with the natural laccase, as over 90 % of their catalytic activity can be maintained in wide pH, temperatures and more than 30 days storage. In the presence of oxygen, CuCDs can not only catalyze the chromogenic reaction of o-phenylenediamine (OPD) and p-phenylenediamine (PPD), allowing for the selective and rapid quantification of these aniline additives in hair dye products, but also catalyze the polymerization of dopamine (DA) under ambient conditions for hair dyeing.

Significance

This work not only provides an effective method for the determination of aniline additives in hair dyes, but also offers new approaches for safe hair dyeing, and expands the application of carbon nanomaterials in the cosmetics field.
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引用次数: 0
Multiplexed and highly sensitive FRET aptasensor for simultaneous assay of multiple antibiotics via DNAzyme and catalytic strand displacement amplification cascades
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-14 DOI: 10.1016/j.aca.2025.344069
Tingting Gong, Huaifeng Yan, Daxiu Li, Bingying Jiang, Yun Xiang, Ruo Yuan

Background

The emergence of antibiotic-resistant microorganisms poses significant risks to public health. Therefore, the development of technologies capable of detecting antibiotics with high sensitivity and selectivity is essential for monitoring and controlling the spread of antibiotic resistance. Yet, current major available antibody-based antibiotic detection methods often face limitations in sensitivity, complexity, and cost, and commonly one target antibiotic can be detected in one assay.

Results

On the basis of a three-way DNA junction (3-WJ) signal construct, we describe a multiplexed fluorescence resonance energy transfer (FRET) aptasensor strategy for highly sensitive simultaneous detection of sarafloxacin (SAR) and enrofloxacin (ENR) through cyclic DNAzyme and catalytic strand displacement reaction (CSDR) signal amplification cascades. Target antibiotics are recognized separately by the aptamers in DNAzyme/apamer duplexes to release active DNAzyme sequences, which cleave the dumbbell substrate hairpins to free ssDNAs to trigger subsequent CSDR between the assistance hairpins and the 3-WJ constructs for formation of many fluorophores 5-carboxyfluorescein (FAM)- and 2',7'-dimethoxy-4', 5'-dichloro-6-carboxyfluorescein (JOE)/6-carboxy-X-rhodamine (ROX)-labeled DNA duplexes. This leads to the pulling of FAM dye donor in proximity to the ROX and JOE dye acceptors, facilitating the yield of considerably amplified FRET signals at 555 nm and 605 nm for the SAR and ENR assays, respectively, with detection limits of 1.95 pM (0.76 ng/L) and 5.01 pM (1.8 ng/L) within 2.5 hours. Additionally, this sensing method can selectively discriminate SAR and ENR against non-target antibiotics and has been validated for the simultaneous detection of SAR and ENR in milk samples.

Significance

Featured with the advantages of convenient and significant signal amplification capability as well as single excitation for multiplexed detection, the successful demonstration of our method for sensitive and simultaneous detection of two antibiotics therefore shows its promising potential for constructing different multiplexed aptasensors for detecting various low levels of biomolecules.
{"title":"Multiplexed and highly sensitive FRET aptasensor for simultaneous assay of multiple antibiotics via DNAzyme and catalytic strand displacement amplification cascades","authors":"Tingting Gong, Huaifeng Yan, Daxiu Li, Bingying Jiang, Yun Xiang, Ruo Yuan","doi":"10.1016/j.aca.2025.344069","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344069","url":null,"abstract":"<h3>Background</h3>The emergence of antibiotic-resistant microorganisms poses significant risks to public health. Therefore, the development of technologies capable of detecting antibiotics with high sensitivity and selectivity is essential for monitoring and controlling the spread of antibiotic resistance. Yet, current major available antibody-based antibiotic detection methods often face limitations in sensitivity, complexity, and cost, and commonly one target antibiotic can be detected in one assay.<h3>Results</h3>On the basis of a three-way DNA junction (3-WJ) signal construct, we describe a multiplexed fluorescence resonance energy transfer (FRET) aptasensor strategy for highly sensitive simultaneous detection of sarafloxacin (SAR) and enrofloxacin (ENR) through cyclic DNAzyme and catalytic strand displacement reaction (CSDR) signal amplification cascades. Target antibiotics are recognized separately by the aptamers in DNAzyme/apamer duplexes to release active DNAzyme sequences, which cleave the dumbbell substrate hairpins to free ssDNAs to trigger subsequent CSDR between the assistance hairpins and the 3-WJ constructs for formation of many fluorophores 5-carboxyfluorescein (FAM)- and 2',7'-dimethoxy-4', 5'-dichloro-6-carboxyfluorescein (JOE)/6-carboxy-X-rhodamine (ROX)-labeled DNA duplexes. This leads to the pulling of FAM dye donor in proximity to the ROX and JOE dye acceptors, facilitating the yield of considerably amplified FRET signals at 555 nm and 605 nm for the SAR and ENR assays, respectively, with detection limits of 1.95 pM (0.76 ng/L) and 5.01 pM (1.8 ng/L) within 2.5 hours. Additionally, this sensing method can selectively discriminate SAR and ENR against non-target antibiotics and has been validated for the simultaneous detection of SAR and ENR in milk samples.<h3>Significance</h3>Featured with the advantages of convenient and significant signal amplification capability as well as single excitation for multiplexed detection, the successful demonstration of our method for sensitive and simultaneous detection of two antibiotics therefore shows its promising potential for constructing different multiplexed aptasensors for detecting various low levels of biomolecules.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"108 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831818","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
Selection and identification of the ssDNA aptamer against polymyxin B sulfate
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-14 DOI: 10.1016/j.aca.2025.344067
Zhuxin Chang , Jiayue Zhou , Dongmei Li , Haoran Wang , Mengmeng Chen , Linyuan Liu , Jia Ding , Yu Wang , Zhixian Gao , Na Sai

Background

Polymyxin B (PMB) is a potent antibiotic, and its sulfate form, Polymyxin B Sulfate (PMBS), is widely used. When PMBS is used as a veterinary drug, excessive use can lead to drug residues in animal bodies, which is a significant food safety issue and raises serious concerns. Therefore, there is an urgent need to strengthen research in this area. In this study, we obtained a ssDNA aptamer against PMBS using the Capture-SELEX method, which has notable advantages in small molecule selection. Then, we integrated the obtained aptamer with a biosensor based on the CRISPR/Cas14a system for a series of validations.

Results

In this study, specific aptamers against PMBS were discovered via the Capture-SELEX process. The selection process consisted of ten rounds. The affinity of the candidate sequences was determined by Isothermal Titration Calorimetry (ITC), and the PMBS24 aptamer with the highest affinity was ultimately identified, with a dissociation constant (Kd) of 3.89 ± 0.46 μM. To further obtain high-affinity aptamers, we attempted to truncate the PMBS24 aptamer. However, the results demonstrated that the aptamer with the full-length sequence exhibited superior affinity. Subsequently, it was applied in the CRISPR/Cas14a-based sensor for the detection of PMBS. This method had a LOD of 0.99 ng mL−1, with good specificity, and was successfully used for the detection in milk.

Significance

An important recognition element of PMBS has been successfully obtained, filling a part of the gap in the detection of PMBS. Moreover, the aptamer has been applied to the CRISPR/Cas14a-based sensor for amplification-free PMBS detection, yielding favorable detection results. This also opens up the possibility of applying the aptamer to other similar sensors.
{"title":"Selection and identification of the ssDNA aptamer against polymyxin B sulfate","authors":"Zhuxin Chang ,&nbsp;Jiayue Zhou ,&nbsp;Dongmei Li ,&nbsp;Haoran Wang ,&nbsp;Mengmeng Chen ,&nbsp;Linyuan Liu ,&nbsp;Jia Ding ,&nbsp;Yu Wang ,&nbsp;Zhixian Gao ,&nbsp;Na Sai","doi":"10.1016/j.aca.2025.344067","DOIUrl":"10.1016/j.aca.2025.344067","url":null,"abstract":"<div><h3>Background</h3><div>Polymyxin B (PMB) is a potent antibiotic, and its sulfate form, Polymyxin B Sulfate (PMBS), is widely used. When PMBS is used as a veterinary drug, excessive use can lead to drug residues in animal bodies, which is a significant food safety issue and raises serious concerns. Therefore, there is an urgent need to strengthen research in this area. In this study, we obtained a ssDNA aptamer against PMBS using the Capture-SELEX method, which has notable advantages in small molecule selection. Then, we integrated the obtained aptamer with a biosensor based on the CRISPR/Cas14a system for a series of validations.</div></div><div><h3>Results</h3><div>In this study, specific aptamers against PMBS were discovered via the Capture-SELEX process. The selection process consisted of ten rounds. The affinity of the candidate sequences was determined by Isothermal Titration Calorimetry (ITC), and the PMBS24 aptamer with the highest affinity was ultimately identified, with a dissociation constant (Kd) of 3.89 ± 0.46 μM. To further obtain high-affinity aptamers, we attempted to truncate the PMBS24 aptamer. However, the results demonstrated that the aptamer with the full-length sequence exhibited superior affinity. Subsequently, it was applied in the CRISPR/Cas14a-based sensor for the detection of PMBS. This method had a LOD of 0.99 ng mL<sup>−1</sup>, with good specificity, and was successfully used for the detection in milk.</div></div><div><h3>Significance</h3><div>An important recognition element of PMBS has been successfully obtained, filling a part of the gap in the detection of PMBS. Moreover, the aptamer has been applied to the CRISPR/Cas14a-based sensor for amplification-free PMBS detection, yielding favorable detection results. This also opens up the possibility of applying the aptamer to other similar sensors.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1357 ","pages":"Article 344067"},"PeriodicalIF":5.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143828298","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
Highly selective electrochemical sensing of hydroquinone and catechol using Co nanoparticles anchored on N-doped carbon nanotube hollow sphere
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-14 DOI: 10.1016/j.aca.2025.344074
Xiaomin Cheng , Xiaojuan Shui , Quan Yang , Huimin Ma , Yuanyuan Zhang , Ting Zeng , Juan Yang , Zhen Wu , Xiuhua Zhang , Nianjun Yang

Background

Hydroquinone (HQ) and catechol (CC), two important isomers with similar structures, are highly toxic, often coexisting, and impeding each other in the simultaneous detection. Electrochemical technique provides a promising alternative toward the quantification of HQ and CC, due to its inherent advantages in terms of highly sensitive reaction, ease of monitoring, low-cost, simplicity and quick response. Development of a sensing material with outstanding electrocatalytic capabilities and its utilization for the fabrication of an electrochemical sensor for highly selective monitoring of HQ and CC is of great significance.

Results

In this study, a novel hierarchical nanostructure is fabricated where Co nanoparticles are anchored on N-doped carbon nanotube hollow sphere (Co/HNC) through the pyrolysis of ZIF-67@ZIF-8 hollow microsphere. On the Co/HNC modified electrode two well-defined and distinguishable peaks are displayed, resulting from electrochemical oxidation of both isomers. As an electrochemical sensor, the recorded peak current displays a linear relationship to the concentration of both HQ and CC from 0.1 to 100 μM under optimal conditions, coupled with their low detection limit of 23 nM and 37 nM, respectively. The probable application of this sensing platform was also checked for the detection of HQ and CC in real samples (e.g., lake water, tap water, detergents, ointment and orange juice), showing outstanding recovery rates. Moreover, simultaneous analysis of HQ and CC exhibited high reproducibility, selectivity and long-term stability.

Significance

As a highly efficient electrocatalyst, the unique hollow and porous microsphere structure of Co/HNC affords abundant active sites, short ion diffusion path, outstanding electronic conductivity and high electrocatalytic activity, thereby certifying excellent sensing capability for these two important isomers. This study thus efficiently explores the advances of metal/NC with hollow structure for the formation of selective dihydroxybenzene electrochemical sensors.
{"title":"Highly selective electrochemical sensing of hydroquinone and catechol using Co nanoparticles anchored on N-doped carbon nanotube hollow sphere","authors":"Xiaomin Cheng ,&nbsp;Xiaojuan Shui ,&nbsp;Quan Yang ,&nbsp;Huimin Ma ,&nbsp;Yuanyuan Zhang ,&nbsp;Ting Zeng ,&nbsp;Juan Yang ,&nbsp;Zhen Wu ,&nbsp;Xiuhua Zhang ,&nbsp;Nianjun Yang","doi":"10.1016/j.aca.2025.344074","DOIUrl":"10.1016/j.aca.2025.344074","url":null,"abstract":"<div><h3>Background</h3><div>Hydroquinone (HQ) and catechol (CC), two important isomers with similar structures, are highly toxic, often coexisting, and impeding each other in the simultaneous detection. Electrochemical technique provides a promising alternative toward the quantification of HQ and CC, due to its inherent advantages in terms of highly sensitive reaction, ease of monitoring, low-cost, simplicity and quick response. Development of a sensing material with outstanding electrocatalytic capabilities and its utilization for the fabrication of an electrochemical sensor for highly selective monitoring of HQ and CC is of great significance.</div></div><div><h3>Results</h3><div>In this study, a novel hierarchical nanostructure is fabricated where Co nanoparticles are anchored on N-doped carbon nanotube hollow sphere (Co/HNC) through the pyrolysis of ZIF-67@ZIF-8 hollow microsphere. On the Co/HNC modified electrode two well-defined and distinguishable peaks are displayed, resulting from electrochemical oxidation of both isomers. As an electrochemical sensor, the recorded peak current displays a linear relationship to the concentration of both HQ and CC from 0.1 to 100 μM under optimal conditions, coupled with their low detection limit of 23 nM and 37 nM, respectively. The probable application of this sensing platform was also checked for the detection of HQ and CC in real samples (e.g., lake water, tap water, detergents, ointment and orange juice), showing outstanding recovery rates. Moreover, simultaneous analysis of HQ and CC exhibited high reproducibility, selectivity and long-term stability.</div></div><div><h3>Significance</h3><div>As a highly efficient electrocatalyst, the unique hollow and porous microsphere structure of Co/HNC affords abundant active sites, short ion diffusion path, outstanding electronic conductivity and high electrocatalytic activity, thereby certifying excellent sensing capability for these two important isomers. This study thus efficiently explores the advances of metal/NC with hollow structure for the formation of selective dihydroxybenzene electrochemical sensors.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1357 ","pages":"Article 344074"},"PeriodicalIF":5.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827654","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
Nasopharyngeal cancer screening and immunotherapy efficacy evaluation based on plasma separation combined with label-free SERS technology
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-14 DOI: 10.1016/j.aca.2025.344070
Ruiying Lin, Zhangying Jiang, Jinyong Lin, Feifei Tong, Yangmin Wu, Jinquan Hong, Sufang Qiu, Qiong Wu

Background

In recent years, significant progress has been made in the treatment of nasopharyngeal carcinoma (NPC). The application of immunotherapy, especially the use of Programmed Cell Death Protein 1 inhibitors, has demonstrated excellent therapeutic effects. However, inconsistent immunotherapy outcomes due to individual differences in patients remain a major challenge, making the search for specific biomarkers to screen for the population who may benefit from immunotherapy a priority. Surface-enhanced Raman spectroscopy (SERS) has shown great potential as a highly sensitive and specific optical analytical tool for identifying and monitoring tumor-related markers in NPC.

Results

In this study, plasma samples from Nasopharyngeal cancer patients before and after immunotherapy, along with those from healthy volunteers, were tested using label-free SERS combined with plasmapheresis. Especially, the components with varying molecular weight sizes were analyzed via the separation process, thereby preventing the potential loss of diagnostic information that could result from competitive adsorption. Subsequently, a robust machine learning algorithm based on principal component analysis and linear discriminant analysis (PCA-LDA) was used to extract features from plasma SERS data and establish an effective discriminant model. The results showed that in the upper plasma layer, the most optimal discrimination was found between normal patients and those post-treatment, with sensitivity and specificity of 88.5% and 92.3%, respectively. In the lower plasma layer, the most optimal discrimination was found between the pre-treatment and post-treatment patients, with sensitivity and specificity of 84.6% and 80.8%, respectively.

Significance and novelty

Plasmapheresis can reveal latent diagnostic information in the plasma and holds promise for treating NPC, the screening of the population who may benefit from immunotherapy, and the postoperative evaluation of immunotherapy. Further exploration of the feasibility of using SERS to detect tumor markers in the population who may benefit from immunotherapy for NPC will help improve the therapeutic efficacy, optimize clinical practice, and promote the development of individualized treatment strategies.
{"title":"Nasopharyngeal cancer screening and immunotherapy efficacy evaluation based on plasma separation combined with label-free SERS technology","authors":"Ruiying Lin, Zhangying Jiang, Jinyong Lin, Feifei Tong, Yangmin Wu, Jinquan Hong, Sufang Qiu, Qiong Wu","doi":"10.1016/j.aca.2025.344070","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344070","url":null,"abstract":"<h3>Background</h3>In recent years, significant progress has been made in the treatment of nasopharyngeal carcinoma (NPC). The application of immunotherapy, especially the use of Programmed Cell Death Protein 1 inhibitors, has demonstrated excellent therapeutic effects. However, inconsistent immunotherapy outcomes due to individual differences in patients remain a major challenge, making the search for specific biomarkers to screen for the population who may benefit from immunotherapy a priority. Surface-enhanced Raman spectroscopy (SERS) has shown great potential as a highly sensitive and specific optical analytical tool for identifying and monitoring tumor-related markers in NPC.<h3>Results</h3>In this study, plasma samples from Nasopharyngeal cancer patients before and after immunotherapy, along with those from healthy volunteers, were tested using label-free SERS combined with plasmapheresis. Especially, the components with varying molecular weight sizes were analyzed via the separation process, thereby preventing the potential loss of diagnostic information that could result from competitive adsorption. Subsequently, a robust machine learning algorithm based on principal component analysis and linear discriminant analysis (PCA-LDA) was used to extract features from plasma SERS data and establish an effective discriminant model. The results showed that in the upper plasma layer, the most optimal discrimination was found between normal patients and those post-treatment, with sensitivity and specificity of 88.5% and 92.3%, respectively. In the lower plasma layer, the most optimal discrimination was found between the pre-treatment and post-treatment patients, with sensitivity and specificity of 84.6% and 80.8%, respectively.<h3>Significance and novelty</h3>Plasmapheresis can reveal latent diagnostic information in the plasma and holds promise for treating NPC, the screening of the population who may benefit from immunotherapy, and the postoperative evaluation of immunotherapy. Further exploration of the feasibility of using SERS to detect tumor markers in the population who may benefit from immunotherapy for NPC will help improve the therapeutic efficacy, optimize clinical practice, and promote the development of individualized treatment strategies.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"40 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831847","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
Guidelines on the proper selection of greenness and related metric tools in analytical chemistry – a tutorial
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-12 DOI: 10.1016/j.aca.2025.344052
Lutfi Andre Yahya, Christina Vakh, Olha Dushna, Oktawia Kalisz, Szymon Bocian, Marek Tobiszewski

Background

The metric tools that aim to assess greenness, whiteness or related aspects of analytical procedures are gaining in popularity. At the same time, their application is not standardized, leading to unintentional abuses.

Results

Within this study, two datasets are created, consisting of the greenness assessment results for 27 (for general assessment) and 3 (for reproducibility study) analytical procedures, obtained with available greenness and related metric tools. The first dataset was assessed with multivariate statistical tools, and the analysis shows that metric tools give correlated results. The second dataset was used to calculate the reproducibility of metric tools results.

Significance and Novelty

Based on the results of multivariate statistics and reproducibility analyses, we propose guidelines for the application of metric tools. Obeying these guidelines will result in a more standardized approach to assessment, consistency of results, and drawing more meaningful conclusions.
{"title":"Guidelines on the proper selection of greenness and related metric tools in analytical chemistry – a tutorial","authors":"Lutfi Andre Yahya, Christina Vakh, Olha Dushna, Oktawia Kalisz, Szymon Bocian, Marek Tobiszewski","doi":"10.1016/j.aca.2025.344052","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344052","url":null,"abstract":"<h3>Background</h3>The metric tools that aim to assess greenness, whiteness or related aspects of analytical procedures are gaining in popularity. At the same time, their application is not standardized, leading to unintentional abuses.<h3>Results</h3>Within this study, two datasets are created, consisting of the greenness assessment results for 27 (for general assessment) and 3 (for reproducibility study) analytical procedures, obtained with available greenness and related metric tools. The first dataset was assessed with multivariate statistical tools, and the analysis shows that metric tools give correlated results. The second dataset was used to calculate the reproducibility of metric tools results.<h3>Significance and Novelty</h3>Based on the results of multivariate statistics and reproducibility analyses, we propose guidelines for the application of metric tools. Obeying these guidelines will result in a more standardized approach to assessment, consistency of results, and drawing more meaningful conclusions.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"183 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822928","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
Controlled synthesis of superhydrophilic flower-like hierarchical porous diboronate affinity materials for capturing biomarkers
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-11 DOI: 10.1016/j.aca.2025.344053
Jinhua Xu , Minghui Tang , Wenmin Zhang , Shiye Xie , Qianqian Gu , Lan Zhang

Background

Boronate affinity chromatography represents a powerful analytical technique for the selective separation and enrichment of biomolecules containing cis-diol moieties, including carbohydrates, glycoproteins, and other cis-dihydroxy compounds. While boronate affinity materials (BAMs) have shown promise in glycosylation-based separation and analysis, their practical application is hindered by non-biocompatible binding pH, low enrichment efficiency for low-abundance samples, non-specific adsorption, and limited loading capacity. To address these limitations, this work focuses on developing flower-like hierarchical porous diboronate affinity materials (FHP-DBAMs) with enhanced binding strength, selectivity, and capacity for cis-diol-containing biomolecules.

Results

FHP-DBAM was synthesized via a facile sol-gel method, using tetrahydroxydiboron as a hydrophilic diboronic acid monomer. The electron-withdrawing nature and hydrophilicity of diboronate affinity mechanism enable FHP-DBAM to operate at lower pH values (pH ≥ 5), addressing the biocompatibility issue. DFT and experiment calculations confirm the enhanced cis-diol binding affinity of diboronate affinity mechanism compared with monoboronate affinity mechanism, resulting in a remarkably low dissociation constant (DFT Kd = 6.74 × 10−5 M, experiment Kd = 9.95 × 10−5 M) for FHP-DBAM. Furthermore, the unique flower-like hierarchical porous structure provides a high surface area and nanoconfinement effect, significantly boosting target molecule loading capacity and affinity reaction kinetics. Compared to traditional BAMs, FHP-DBAM exhibits over ten times higher loading capacity. As a proof-of-concept, FHP-DBAM successfully captures the biomarker GM1 in breast cancer cells MCF-7 with high efficiency.

Significance and novelty

This work introduces diboronate affinity mechanism and flower-like hierarchical porous structure as new solution to overcome the limitations of conventional BAMs. FHP-DBAMs achieve lower binding pH, enhanced selectivity, and stronger binding stability through diboronate affinity mechanism. The unique flower-like porous structure maximizes surface area and active sites, addressing low enrichment efficiency and loading capacity. These advancements are critical for the efficient and biocompatible separation of cis-diol-containing biomolecules.
{"title":"Controlled synthesis of superhydrophilic flower-like hierarchical porous diboronate affinity materials for capturing biomarkers","authors":"Jinhua Xu ,&nbsp;Minghui Tang ,&nbsp;Wenmin Zhang ,&nbsp;Shiye Xie ,&nbsp;Qianqian Gu ,&nbsp;Lan Zhang","doi":"10.1016/j.aca.2025.344053","DOIUrl":"10.1016/j.aca.2025.344053","url":null,"abstract":"<div><h3>Background</h3><div>Boronate affinity chromatography represents a powerful analytical technique for the selective separation and enrichment of biomolecules containing <em>cis</em>-diol moieties, including carbohydrates, glycoproteins, and other <em>cis</em>-dihydroxy compounds. While boronate affinity materials (BAMs) have shown promise in glycosylation-based separation and analysis, their practical application is hindered by non-biocompatible binding pH, low enrichment efficiency for low-abundance samples, non-specific adsorption, and limited loading capacity. To address these limitations, this work focuses on developing flower-like hierarchical porous diboronate affinity materials (FHP-DBAMs) with enhanced binding strength, selectivity, and capacity for <em>cis</em>-diol-containing biomolecules.</div></div><div><h3>Results</h3><div>FHP-DBAM was synthesized via a facile sol-gel method, using tetrahydroxydiboron as a hydrophilic diboronic acid monomer. The electron-withdrawing nature and hydrophilicity of diboronate affinity mechanism enable FHP-DBAM to operate at lower pH values (pH ≥ 5), addressing the biocompatibility issue. DFT and experiment calculations confirm the enhanced <em>cis</em>-diol binding affinity of diboronate affinity mechanism compared with monoboronate affinity mechanism, resulting in a remarkably low dissociation constant (DFT Kd = 6.74 × 10<sup>−5</sup> M, experiment Kd = 9.95 × 10<sup>−5</sup> M) for FHP-DBAM. Furthermore, the unique flower-like hierarchical porous structure provides a high surface area and nanoconfinement effect, significantly boosting target molecule loading capacity and affinity reaction kinetics. Compared to traditional BAMs, FHP-DBAM exhibits over ten times higher loading capacity. As a proof-of-concept, FHP-DBAM successfully captures the biomarker GM<sub>1</sub> in breast cancer cells MCF-7 with high efficiency.</div></div><div><h3>Significance and novelty</h3><div>This work introduces diboronate affinity mechanism and flower-like hierarchical porous structure as new solution to overcome the limitations of conventional BAMs. FHP-DBAMs achieve lower binding pH, enhanced selectivity, and stronger binding stability through diboronate affinity mechanism. The unique flower-like porous structure maximizes surface area and active sites, addressing low enrichment efficiency and loading capacity. These advancements are critical for the efficient and biocompatible separation of <em>cis</em>-diol-containing biomolecules.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1357 ","pages":"Article 344053"},"PeriodicalIF":5.7,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819890","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
Ion-mediated etching of Au–Ag core-shell nanorods for LSPR-based discrimination of hazardous ions
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-11 DOI: 10.1016/j.aca.2025.344066
Mohamad Shirzad , Mobina Anbarestani , Forough Ghasemi

Background

The detection of metal ions represents a critical analytical challenge due to their persistent environmental accumulation and severe toxic effects on ecosystems and human health. Even at trace concentrations, toxic metal ions can cause irreversible biological damage, necessitating the development of sensitive, selective, and rapid monitoring platforms. Advanced detection systems are urgently needed for environmental surveillance, industrial effluent control, and food/water safety applications where regulatory compliance and early warning capabilities are paramount.

Results

This work presents an etching-based sensor array to identify and discriminate Pb2+, Hg2+, Cu2+, NO2, Cr6+, and As3+ as hazardous ions. Au@Ag core@shell nanorods were utilized as sensing elements in different pH values in the presence of thiosulfate and thiourea as key elements in the oxidation of nanoparticles. Analytes' response patterns in the range of 1.0–30 μM were analyzed via various methods, including heatmap, bar plot, and linear discriminant analysis (LDA), showing perfect discrimination. To ensure the sensor's applicability in real samples, we conducted meticulous testing on different sources, including tap water, well water, tilapia pond water, tomato soil extract, and urine samples.

Significance

The sensor demonstrated excellent performance in classifying mixture samples and providing precise and accurate detection in real samples. This innovation offers a promising future for etching-based sensor arrays by utilizing core-shell nanoparticles as sensitive sensing elements and a significant contribution to global efforts in safeguarding public health and the environment from the threat of pollutants.
{"title":"Ion-mediated etching of Au–Ag core-shell nanorods for LSPR-based discrimination of hazardous ions","authors":"Mohamad Shirzad ,&nbsp;Mobina Anbarestani ,&nbsp;Forough Ghasemi","doi":"10.1016/j.aca.2025.344066","DOIUrl":"10.1016/j.aca.2025.344066","url":null,"abstract":"<div><h3>Background</h3><div>The detection of metal ions represents a critical analytical challenge due to their persistent environmental accumulation and severe toxic effects on ecosystems and human health. Even at trace concentrations, toxic metal ions can cause irreversible biological damage, necessitating the development of sensitive, selective, and rapid monitoring platforms. Advanced detection systems are urgently needed for environmental surveillance, industrial effluent control, and food/water safety applications where regulatory compliance and early warning capabilities are paramount.</div></div><div><h3>Results</h3><div>This work presents an etching-based sensor array to identify and discriminate Pb<sup>2+</sup>, Hg<sup>2+</sup>, Cu<sup>2+</sup>, NO<sub>2</sub><sup>−</sup>, Cr<sup>6+</sup>, and As<sup>3+</sup> as hazardous ions. Au@Ag core@shell nanorods were utilized as sensing elements in different pH values in the presence of thiosulfate and thiourea as key elements in the oxidation of nanoparticles. Analytes' response patterns in the range of 1.0–30 μM were analyzed via various methods, including heatmap, bar plot, and linear discriminant analysis (LDA), showing perfect discrimination. To ensure the sensor's applicability in real samples, we conducted meticulous testing on different sources, including tap water, well water, tilapia pond water, tomato soil extract, and urine samples.</div></div><div><h3>Significance</h3><div>The sensor demonstrated excellent performance in classifying mixture samples and providing precise and accurate detection in real samples. This innovation offers a promising future for etching-based sensor arrays by utilizing core-shell nanoparticles as sensitive sensing elements and a significant contribution to global efforts in safeguarding public health and the environment from the threat of pollutants.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1357 ","pages":"Article 344066"},"PeriodicalIF":5.7,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822923","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
Alkalized MXene/laser-induced graphene-based integrated three-electrode devices for micro-droplet detection of albendazole 基于碱化 MXene/激光诱导石墨烯的集成三电极装置,用于阿苯达唑的微滴检测
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-10 DOI: 10.1016/j.aca.2025.344051
Xin Zhou , Mei Liu , Bin Yang , Can Wu , Kangbing Wu , Shiran Sun

Background

Albendazole is a commonly-used antiparasitic drug that has been extensively applied in animal husbandry and aquaculture to prevent and treat various parasitic infections. However, the potential residues of albendazole in animal-derived foods and the aquatic environment can pose risks to human health and ecological balance. Hence, the development of a highly sensitive and rapid analytical method for albendazole is of utmost importance to safeguard food safety and preserve the ecological environment. MXene nanosheets (Ti3C2Tx) are emerging as promising precursors for the design of such detection systems. (86)

Results

In this work, MXene nanosheets (Ti3C2Tx) were alkalized in NaOH solution to form alkalized Ti3C2Tx (Al-MXene). The treatment caused structural changes such as expanded interlayer spacing, reduced particle size, enhanced Zeta potential, and the formation of amorphous TiO2 on the surface. These modifications gave Al-MXene larger electrochemical active specific area and stronger physical adsorption capacity for albendazole compared to the original MXene nanosheets. When Al-MXene was decorated on the surface of laser-induced graphene (LIG), albendazole was efficiently oxidized due to the unique surface activity of Al-MXene and the abundant three-dimensional porous structure of LIG. An integrated three-electrode device based on the Al-MXene/LIG structure was fabricated for the electrochemical detection of albendazole in micro-droplets for milk sample. The device showed a linear detection range from 10 nM to 1 μM, a sensitivity of 411 μA μmoL−1 cm−2, and a detection limit of 7.5 nM (143)

Significance

The development of the integrated three-electrode device based on Al-MXene/LIG provides a highly sensitive and efficient method for detecting albendazole in milk samples. Moreover, it can also offer guidance for fabricating more innovative electrochemical sensors for the rapid screening of veterinary drug residues. This contribution is of great significance in ensuring food safety and protecting public health. (57)
{"title":"Alkalized MXene/laser-induced graphene-based integrated three-electrode devices for micro-droplet detection of albendazole","authors":"Xin Zhou ,&nbsp;Mei Liu ,&nbsp;Bin Yang ,&nbsp;Can Wu ,&nbsp;Kangbing Wu ,&nbsp;Shiran Sun","doi":"10.1016/j.aca.2025.344051","DOIUrl":"10.1016/j.aca.2025.344051","url":null,"abstract":"<div><h3>Background</h3><div>Albendazole is a commonly-used antiparasitic drug that has been extensively applied in animal husbandry and aquaculture to prevent and treat various parasitic infections. However, the potential residues of albendazole in animal-derived foods and the aquatic environment can pose risks to human health and ecological balance. Hence, the development of a highly sensitive and rapid analytical method for albendazole is of utmost importance to safeguard food safety and preserve the ecological environment. MXene nanosheets (Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) are emerging as promising precursors for the design of such detection systems. (86)</div></div><div><h3>Results</h3><div>In this work, MXene nanosheets (Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>) were alkalized in NaOH solution to form alkalized Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> (Al-MXene). The treatment caused structural changes such as expanded interlayer spacing, reduced particle size, enhanced Zeta potential, and the formation of amorphous TiO<sub>2</sub> on the surface. These modifications gave Al-MXene larger electrochemical active specific area and stronger physical adsorption capacity for albendazole compared to the original MXene nanosheets. When Al-MXene was decorated on the surface of laser-induced graphene (LIG), albendazole was efficiently oxidized due to the unique surface activity of Al-MXene and the abundant three-dimensional porous structure of LIG. An integrated three-electrode device based on the Al-MXene/LIG structure was fabricated for the electrochemical detection of albendazole in micro-droplets for milk sample. The device showed a linear detection range from 10 nM to 1 μM, a sensitivity of 411 μA μmoL<sup>−1</sup> cm<sup>−2</sup>, and a detection limit of 7.5 nM (143)</div></div><div><h3>Significance</h3><div>The development of the integrated three-electrode device based on Al-MXene/LIG provides a highly sensitive and efficient method for detecting albendazole in milk samples. Moreover, it can also offer guidance for fabricating more innovative electrochemical sensors for the rapid screening of veterinary drug residues. This contribution is of great significance in ensuring food safety and protecting public health. (57)</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1356 ","pages":"Article 344051"},"PeriodicalIF":5.7,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819856","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
Development of DNA aptamers towards detection of tuberculosis biomarker Ag85B in a fluorescence-based sensing platform
IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-04-10 DOI: 10.1016/j.aca.2025.344029
Satakshi Hazra, Manish Gupta, Rakesh Bhatnagar, Prithwi Chayan Chatterjee, Sanjukta Patra

Background

Timely diagnosis of tuberculosis (TB) remains a critical challenge, highlighting the need for better screening tools. Traditional antibody-based detection methods for TB are often costly and cumbersome. To address this, we developed a streamlined centrifugal SELEX approach using a 69-nucleotide DNA library and the recombinant TB biomarker Ag85B, towards fabrication of an aptasensing platform offering a simpler and faster alternative.

Results

Two high affinity DNA aptamers were screened through 12 rounds of SELEX and verified with in silico docking, circular dichroism spectroscopy and electrophoretic shift assays for binding interactions with Ag85B. The aptamer with highest binding affinity (KD values 76.36 ± 10.76 nM in binding buffer and 86.62 ± 6.20 nM in spiked serum) was used for fabrication of a fluorescence based aptasensing platform using graphene oxide as a quencher. The aptamer demonstrated specificity towards Ag85B without interference from two other recombinant TB proteins MPT64 and ESAT6. The aptasensing platform offered limits of detection of 5.83 nM in binding buffer and 6.51 nM in spiked serum.

Significance

This work developed a modified SELEX approach combining a centrifugal filter and streptavidin-biotin magnetic separation technique for isolation of DNA aptamers. We report for the first time, a DNA aptamer against Ag85B biomarker that holds high prospects for clinical applications in diagnosing TB.
{"title":"Development of DNA aptamers towards detection of tuberculosis biomarker Ag85B in a fluorescence-based sensing platform","authors":"Satakshi Hazra, Manish Gupta, Rakesh Bhatnagar, Prithwi Chayan Chatterjee, Sanjukta Patra","doi":"10.1016/j.aca.2025.344029","DOIUrl":"https://doi.org/10.1016/j.aca.2025.344029","url":null,"abstract":"<h3>Background</h3>Timely diagnosis of tuberculosis (TB) remains a critical challenge, highlighting the need for better screening tools. Traditional antibody-based detection methods for TB are often costly and cumbersome. To address this, we developed a streamlined centrifugal SELEX approach using a 69-nucleotide DNA library and the recombinant TB biomarker Ag85B, towards fabrication of an aptasensing platform offering a simpler and faster alternative.<h3>Results</h3>Two high affinity DNA aptamers were screened through 12 rounds of SELEX and verified with <em>in silico</em> docking, circular dichroism spectroscopy and electrophoretic shift assays for binding interactions with Ag85B. The aptamer with highest binding affinity (K<sub>D</sub> values 76.36 ± 10.76 nM in binding buffer and 86.62 ± 6.20 nM in spiked serum) was used for fabrication of a fluorescence based aptasensing platform using graphene oxide as a quencher. The aptamer demonstrated specificity towards Ag85B without interference from two other recombinant TB proteins MPT64 and ESAT6. The aptasensing platform offered limits of detection of 5.83 nM in binding buffer and 6.51 nM in spiked serum.<h3>Significance</h3>This work developed a modified SELEX approach combining a centrifugal filter and streptavidin-biotin magnetic separation technique for isolation of DNA aptamers. We report for the first time, a DNA aptamer against Ag85B biomarker that holds high prospects for clinical applications in diagnosing TB.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"22 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Analytica Chimica Acta
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