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Rapid and sensitive detection of pharmaceutical pollutants in aquaculture by aluminum foil substrate based SERS method combined with deep learning algorithm
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-08 DOI: 10.1016/j.aca.2025.343920
Zixi Huang , Yongqian Lei , Weixin Liang , Yili Cai , Pengran Guo , Jian Sun

Background

Pharmaceutical residual such as antibiotics and disinfectants in aquaculture wastewater have significant potential risks for environment and human health. Surface enhanced Raman spectroscopy (SERS) has been widely used for the detection of pharmaceuticals due to its high sensitivity, low cost, and rapidity. However, it is remain a challenge for high-sensitivity SERS detection and accurate identification of complex pollutants.

Results

Hence, in this work, we developed an aluminum foil (AlF) based SERS detection substrate and established a multilayer perceptron (MLP) deep learning model for the rapid identification of antibiotic components in a mixture. The detection method demonstrated exceptional performance, achieving a high SERS enhancement factor of 4.2 × 105 and excellent sensitivity for trace amounts of fleroxacin (2.7 × 10−8 mol/L), levofloxacin (1.95 × 10−8 mol/L), and pefloxacin (6.9 × 10−8 mol/L),sulfadiazine, methylene blue, and malachite green at a concentration of 1 × 10−8 mol/L can all be detected, the concentrations of the six target compounds and their Raman intensities exhibit a good linear relationship. Moreover, the AlF SERS substrate can be prepared rapidly without adding organic reagents, and it exhibited good reproducibility, with RSD<9.6 %. Additionally, the algorithm model can accurately identify the contaminants mixture of sulfadiazine, methylene blue, and malachite green with a recognition accuracy of 97.8 %, an F1-score of 98.2 %, and a 5-fold cross validation score of 97.4 %, the interpretation analysis using Shapley Additive Explanations (SHAP) reveals that MLP model can specifically concentrate on the distribution of characteristic peaks.

Significance

The experimental results indicated that the MLP model demonstrated strong performance and good robustness in complex matrices. This research provides a promising detection and identification method for the antibiotics and disinfectants in actual aquaculture wastewater treatment.
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引用次数: 0
Development of disease diagnosis technology based on coattention cross-fusion of multiomics data
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343919
Mingtao Wu , Chen Chen , Xuguang Zhou , Hao Liu , Yujia Ren , Jin Gu , Xiaoyi Lv , Cheng Chen

Background

Early diagnosis is vital for increasing the rates of curing diseases and patient survival in medicine. With the advancement of biotechnology, the types of bioomics data are increasing. The integration of multiomics data can provide more comprehensive biological information, thereby achieving more accurate diagnoses than single-omics data can. Nevertheless, current multiomics research is often limited to the intelligent diagnosis of a single disease or a few types of omics data and lacks a multiomics disease diagnosis model that can be widely applied to different diseases. Therefore, developing a model that can effectively utilize multiomics data and accurately diagnose diseases has become an important challenge in medical research.

Results

On the basis of vibrational spectroscopy and metabolomics data, this study proposes an innovative coattention cross-fusion model for disease diagnosis on the basis of interactions of multiomics data. The model not only integrates the information of different omics data but also simulates the interactions between these data to achieve accurate diagnosis of diseases. Through comprehensive experiments, our method achieved accuracies of 95.00 %, 94.95 %, and 97.22 % and area under the curve (AUC) values of 95.00 %, 96.77 %, and 99.31 % on the cervical lymph node metastasis of the thyroid, systemic lupus erythematosus, and cancer datasets, respectively, indicating excellent performance in the diagnosis of multiple diseases.

Significance

The proposed model outperforms existing multiomics models, enhancing medical diagnostic accuracy and offering new approaches for multiomics data use in disease diagnosis. The innovative coattention cross-fusion module enables more effective multiomics data processing and analysis, serving as a potent tool for early and precise disease diagnosis with substantial clinical and research implications.
{"title":"Development of disease diagnosis technology based on coattention cross-fusion of multiomics data","authors":"Mingtao Wu ,&nbsp;Chen Chen ,&nbsp;Xuguang Zhou ,&nbsp;Hao Liu ,&nbsp;Yujia Ren ,&nbsp;Jin Gu ,&nbsp;Xiaoyi Lv ,&nbsp;Cheng Chen","doi":"10.1016/j.aca.2025.343919","DOIUrl":"10.1016/j.aca.2025.343919","url":null,"abstract":"<div><h3>Background</h3><div>Early diagnosis is vital for increasing the rates of curing diseases and patient survival in medicine. With the advancement of biotechnology, the types of bioomics data are increasing. The integration of multiomics data can provide more comprehensive biological information, thereby achieving more accurate diagnoses than single-omics data can. Nevertheless, current multiomics research is often limited to the intelligent diagnosis of a single disease or a few types of omics data and lacks a multiomics disease diagnosis model that can be widely applied to different diseases. Therefore, developing a model that can effectively utilize multiomics data and accurately diagnose diseases has become an important challenge in medical research.</div></div><div><h3>Results</h3><div>On the basis of vibrational spectroscopy and metabolomics data, this study proposes an innovative coattention cross-fusion model for disease diagnosis on the basis of interactions of multiomics data. The model not only integrates the information of different omics data but also simulates the interactions between these data to achieve accurate diagnosis of diseases. Through comprehensive experiments, our method achieved accuracies of 95.00 %, 94.95 %, and 97.22 % and area under the curve (AUC) values of 95.00 %, 96.77 %, and 99.31 % on the cervical lymph node metastasis of the thyroid, systemic lupus erythematosus, and cancer datasets, respectively, indicating excellent performance in the diagnosis of multiple diseases.</div></div><div><h3>Significance</h3><div>The proposed model outperforms existing multiomics models, enhancing medical diagnostic accuracy and offering new approaches for multiomics data use in disease diagnosis. The innovative coattention cross-fusion module enables more effective multiomics data processing and analysis, serving as a potent tool for early and precise disease diagnosis with substantial clinical and research implications.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1351 ","pages":"Article 343919"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570265","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
Investigation on effects of TiO2 on cucumber seedlings using ICP-OES and LA-ICP-MS
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343917
Yu Wang , Qi Liu , Zhen Shao , Xue-Sheng Wang , Ya-Fei Chen , Jun-Jie Bai , Ming-Li Chen , Jian-Hua Wang
With the expansion of TiO2 applications in various fields, TiO2 inevitably enters the soil, increasing the possibility of plant roots being exposed to high concentrations of TiO2. Therefore, it is important to study plant growth under TiO2 exposure conditions. In this study, the combination method of inductively coupled plasma emission spectroscopy (ICP-OES) and laser ablation inductively coupled plasma mass spectroscopy (LA-ICP-MS) was used to evaluate the effect of TiO2 on the content and distribution of nutrient elements in different parts of cucumber seedlings. The results showed that the low concentrations (50 mg/L, 100 mg/L and 200 mg/L) of TiO2 had gradually enhanced the growth of cucumber seedlings, while the high concentration (500 mg/L) of TiO2 had a significant inhibitory effect on the plant. The contents of elements (Ti, K, Ca, Mg, Mn, Fe, Zn, and Cu) in cucumber seedling roots, stems and leaves incubated with 200 mg/L TiO2 were determined by ICP-OES, and the results showed that the uptake of TiO2 increased the content of nutrient elements in the plant. High-resolution imaging of Ti, Ca, Mg, Mn, Fe, Zn, and Cu in roots, stems, and leaves using LA-ICP-MS showed that Ti accumulated mainly at the margins of the leaves. Ca, Mg, Mn, Fe, Zn, and Cu in the leaves were mainly concentrated in the main veins and lateral veins. By evaluating the content and distribution of elements in the plant with ICP-OES and LA-ICP-MS, it provides a new idea to study the mechanism of nanoparticles in the plant. It provides a theoretical basis for the correct use of nanomaterials, which is of great significance in promoting the sustainable development of agriculture.
{"title":"Investigation on effects of TiO2 on cucumber seedlings using ICP-OES and LA-ICP-MS","authors":"Yu Wang ,&nbsp;Qi Liu ,&nbsp;Zhen Shao ,&nbsp;Xue-Sheng Wang ,&nbsp;Ya-Fei Chen ,&nbsp;Jun-Jie Bai ,&nbsp;Ming-Li Chen ,&nbsp;Jian-Hua Wang","doi":"10.1016/j.aca.2025.343917","DOIUrl":"10.1016/j.aca.2025.343917","url":null,"abstract":"<div><div>With the expansion of TiO<sub>2</sub> applications in various fields, TiO<sub>2</sub> inevitably enters the soil, increasing the possibility of plant roots being exposed to high concentrations of TiO<sub>2</sub>. Therefore, it is important to study plant growth under TiO<sub>2</sub> exposure conditions. In this study, the combination method of inductively coupled plasma emission spectroscopy (ICP-OES) and laser ablation inductively coupled plasma mass spectroscopy (LA-ICP-MS) was used to evaluate the effect of TiO<sub>2</sub> on the content and distribution of nutrient elements in different parts of cucumber seedlings. The results showed that the low concentrations (50 mg/L, 100 mg/L and 200 mg/L) of TiO<sub>2</sub> had gradually enhanced the growth of cucumber seedlings, while the high concentration (500 mg/L) of TiO<sub>2</sub> had a significant inhibitory effect on the plant. The contents of elements (Ti, K, Ca, Mg, Mn, Fe, Zn, and Cu) in cucumber seedling roots, stems and leaves incubated with 200 mg/L TiO<sub>2</sub> were determined by ICP-OES, and the results showed that the uptake of TiO<sub>2</sub> increased the content of nutrient elements in the plant. High-resolution imaging of Ti, Ca, Mg, Mn, Fe, Zn, and Cu in roots, stems, and leaves using LA-ICP-MS showed that Ti accumulated mainly at the margins of the leaves. Ca, Mg, Mn, Fe, Zn, and Cu in the leaves were mainly concentrated in the main veins and lateral veins. By evaluating the content and distribution of elements in the plant with ICP-OES and LA-ICP-MS, it provides a new idea to study the mechanism of nanoparticles in the plant. It provides a theoretical basis for the correct use of nanomaterials, which is of great significance in promoting the sustainable development of agriculture.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1352 ","pages":"Article 343917"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570264","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
Rapid detection of organophosphorus pesticide monocrotophos by pore size-regulated amplified fluorescence “turn-on” response of Zr-MOF
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343915
Xinying Gong , Yulu Tian , Yuanjun Tong , Yibin Yuan , Shiyu Peng , Dongmei Wang , Hongqun Tao , Qinwen Tan , Zhengjun Gong

Background

Organophosphorus pesticides pose a severe threat to human health even at trace levels in the environment, owing to their high persistence and neurotoxic effects. Rapid detection methods based on luminescent metal organic frameworks (LMOFs) have great advantages in environmental applications, attributing to their unique luminescence characteristics, structural flexibility, high porosity, and tunable synthesis. Therefore, an effective strategy for adjusting pore size in LMOFs is essential to enhance the sensitivity and selectivity of fluorescence recognition.

Results

In this study, a fluorescence probe NH2-UiO-66@cur was synthesized, where curcumin was utilized to modulate the pore size of NH2-UiO-66, resulting in a fluorescence “turn-on” response for the rapid detection of monocrotophos (MCP). The incorporation of curcumin increased the average pore size of NH2-UiO-66 from 2.01 to 3.61 nm, thereby facilitating the mass transfer of MCP in NH2-UiO-66@cur. Additionally, the coordinating of MCP with the zirconium node effectively block the ligand-to-metal charge transfer (LMCT) process, significantly improving sensitivity with an ultra-low detection limit of 0.41 μg L−1 for MCP. The NH2-UiO-66@cur sensor exhibited excellent selectivity for MCP compared to other organosphosphorus compounds, as well as robust interference resistance. In practical applications, the fluorescence probe showed stable and accurate detection potential, with spiking recoveries ranging from 84.2 % to 105 % in environmental water samples.

Significance

This work provides a novel strategy for tailoring the pore size for a MOF sensor platform, which notably enhances the mass transfer and fluorescence emission intensity by blocking LMCT effect. As a result, it improves the detection sensitivity and selectivity on trace organophosphate pollutants in the environment samples, addressing critical concerns in environmental monitoring.
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引用次数: 0
A microneedle sensor for in-vivo sodium ion detection in plants
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343892
Cheng-Xiao Fan, Zhuo Wang, Zhi-Hao Wang, Ao-Wen Wang, Zhong-Yi Wang, Lan Huang
This study introduces a novel microneedle-type potentiometric sensor designed for the in-vivo detection of sodium ions (Na+) in plant tissues. The development of this sensor is crucial for advancing our understanding of plant responses to salinity stress. The microneedle sensor employs a highly selective Na+ ion carrier and integrates a solid-contact layer made of poly(3,4-ethylenedioxythiophene)-poly (sodium 4-styrenesulfonate) (PEDOT: PSS) prepared by electropolymerization. Due to its excellent conductivity and high chemical stability, PEDOT:PSS significantly reduces the surface impedance of the electrode, enhances charge transfer efficiency, and thereby improves the sensor's response sensitivity and stability. The sensor achieves a linear detection range of 1 × 10−2 to 1 × 10−5 M, with a slope of 56.55 ± 0.25 mV/decade and a detection limit of 1.94 × 10−6 M. The fabrication process was optimized by refining the membrane formulation, ensuring precise control over membrane thickness, and determining the optimal conditioning time, all essential for large-scale production and agricultural applications. In addition, we evaluated the sensor's ability to detect Na+ concentration changes in both artificial culture media and actual plant tissue samples. The sensor's performance was assessed through its capability to monitor Na+ concentration changes in both artificial culture media and real plant tissue samples, with results benchmarked against the standard method (ICP-OES), confirming its accuracy and reliability. Moreover, application trials involving rice seedlings validated the microneedle sensor's efficacy for in vivo detection of Na+, providing a robust tool for understanding plant physiological responses to salt stress. These findings not only offer new insights into plant adaptation mechanisms but also establish a practical platform for selecting salt-tolerant cultivars and enabling rapid salt-level assessment in agricultural practices.
{"title":"A microneedle sensor for in-vivo sodium ion detection in plants","authors":"Cheng-Xiao Fan,&nbsp;Zhuo Wang,&nbsp;Zhi-Hao Wang,&nbsp;Ao-Wen Wang,&nbsp;Zhong-Yi Wang,&nbsp;Lan Huang","doi":"10.1016/j.aca.2025.343892","DOIUrl":"10.1016/j.aca.2025.343892","url":null,"abstract":"<div><div>This study introduces a novel microneedle-type potentiometric sensor designed for the <em>in-vivo</em> detection of sodium ions (Na<sup>+</sup>) in plant tissues. The development of this sensor is crucial for advancing our understanding of plant responses to salinity stress. The microneedle sensor employs a highly selective Na<sup>+</sup> ion carrier and integrates a solid-contact layer made of poly(3,4-ethylenedioxythiophene)-poly (sodium 4-styrenesulfonate) (PEDOT: PSS) prepared by electropolymerization. Due to its excellent conductivity and high chemical stability, PEDOT:PSS significantly reduces the surface impedance of the electrode, enhances charge transfer efficiency, and thereby improves the sensor's response sensitivity and stability. The sensor achieves a linear detection range of 1 × 10<sup>−2</sup> to 1 × 10<sup>−5</sup> M, with a slope of 56.55 ± 0.25 mV/decade and a detection limit of 1.94 × 10<sup>−6</sup> M. The fabrication process was optimized by refining the membrane formulation, ensuring precise control over membrane thickness, and determining the optimal conditioning time, all essential for large-scale production and agricultural applications. In addition, we evaluated the sensor's ability to detect Na<sup>+</sup> concentration changes in both artificial culture media and actual plant tissue samples. The sensor's performance was assessed through its capability to monitor Na<sup>+</sup> concentration changes in both artificial culture media and real plant tissue samples, with results benchmarked against the standard method (ICP-OES), confirming its accuracy and reliability. Moreover, application trials involving rice seedlings validated the microneedle sensor's efficacy for in vivo detection of Na<sup>+</sup>, providing a robust tool for understanding plant physiological responses to salt stress. These findings not only offer new insights into plant adaptation mechanisms but also establish a practical platform for selecting salt-tolerant cultivars and enabling rapid salt-level assessment in agricultural practices.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1352 ","pages":"Article 343892"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569846","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
Lysine enhances the photoresponsive oxidase-like activity of twin Cd0.7Zn0.3S for direct colorimetric detection of lysine
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343914
Xiaorong Sun, Zhongfang Hu, Qing Zhou, Guang-Li Wang

Background

Lysine (Lys) is one of the eight essential amino acids for the human body, which can't be synthesized by the body and must be obtained from external sources. And the detection of Lys is of significance for disease monitoring. The construction of photoresponsive nanozymes based analytical methods have received increasing attention and have been successfully achieved for the detection of metal ions, small molecules and natural enzymes. However, the exploration of photoresponsive nanozyme in amino acids detection has not been tapped.

Results

This study presents an innovative method based on surface passivation by Lys to stimulate the photoresponsive nanozyme activity of twin Cd0.7Zn0.3S nanomaterials. Specifically, Lys can bind with twin Cd0.7Zn0.3S, which filled the dangling bonds on the surface of Cd0.7Zn0.3S and caused passivation of the surface state, resulting in the promotion of the separation efficiency of electrons and holes, along with the facilitation of the production of active intermediates. Therefore, the Cd0.7Zn0.3S in the presence of Lys showed a high catalytic oxidation ability for the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to oxidized TMB (oxTMB). This new kind of photoresponsive oxidase-like activity could be regulated by switching visible light sources and showed the specificity of being only affected by Lys without influenced by other amino acids, thus achieved direct colorimetric detection of Lys. The linear range for Lys detection was 1–100 μM, with a detection limit of 0.18 μM (S/N = 3).

Significance

This study developed a new nanozyme of twin Cd0.7Zn0.3S, whose activity leverages on Lys as a stimulator. Moreover, the Lys detection method proposed by us had the characteristics of high sensitivity, good selectivity, fast detection speed, and low cost. Therefore, it holds significant potential application value, making it a promising candidate in the field of Lys detection and related research areas.
{"title":"Lysine enhances the photoresponsive oxidase-like activity of twin Cd0.7Zn0.3S for direct colorimetric detection of lysine","authors":"Xiaorong Sun,&nbsp;Zhongfang Hu,&nbsp;Qing Zhou,&nbsp;Guang-Li Wang","doi":"10.1016/j.aca.2025.343914","DOIUrl":"10.1016/j.aca.2025.343914","url":null,"abstract":"<div><h3>Background</h3><div>Lysine (Lys) is one of the eight essential amino acids for the human body, which can't be synthesized by the body and must be obtained from external sources. And the detection of Lys is of significance for disease monitoring. The construction of photoresponsive nanozymes based analytical methods have received increasing attention and have been successfully achieved for the detection of metal ions, small molecules and natural enzymes. However, the exploration of photoresponsive nanozyme in amino acids detection has not been tapped.</div></div><div><h3>Results</h3><div>This study presents an innovative method based on surface passivation by Lys to stimulate the photoresponsive nanozyme activity of twin Cd<sub>0.7</sub>Zn<sub>0.3</sub>S nanomaterials. Specifically, Lys can bind with twin Cd<sub>0.7</sub>Zn<sub>0.3</sub>S, which filled the dangling bonds on the surface of Cd<sub>0.7</sub>Zn<sub>0.3</sub>S and caused passivation of the surface state, resulting in the promotion of the separation efficiency of electrons and holes, along with the facilitation of the production of active intermediates. Therefore, the Cd<sub>0.7</sub>Zn<sub>0.3</sub>S in the presence of Lys showed a high catalytic oxidation ability for the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to oxidized TMB (oxTMB). This new kind of photoresponsive oxidase-like activity could be regulated by switching visible light sources and showed the specificity of being only affected by Lys without influenced by other amino acids, thus achieved direct colorimetric detection of Lys. The linear range for Lys detection was 1–100 μM, with a detection limit of 0.18 μM (S/N = 3).</div></div><div><h3>Significance</h3><div>This study developed a new nanozyme of twin Cd<sub>0.7</sub>Zn<sub>0.3</sub>S, whose activity leverages on Lys as a stimulator. Moreover, the Lys detection method proposed by us had the characteristics of high sensitivity, good selectivity, fast detection speed, and low cost. Therefore, it holds significant potential application value, making it a promising candidate in the field of Lys detection and related research areas.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1352 ","pages":"Article 343914"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570263","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
A compact on-chip microsensor for dual-channel measurement of potassium and creatinine in whole blood
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343893
Haijing Tian , Ruo Wu , Qi Lv , Jie Shi , Xiaoqin Guo , Duo Li , Chunli Liu , Qi Li , Weijia Zheng , Haojun Fan , Xuexin Duan , Qiannan Xue
Blood potassium and creatinine levels are critical indicators for managing chronic kidney disease (CKD). In response to the need for home monitoring and emergency care, point-of-care diagnostic technologies based on microsystems have emerged, nevertheless they remain limited in portability and speed for direct in whole blood samples measurement. To enable direct blood detection of potassium and creatinine for effective CKD management, this study presents a novel on-chip self-driven dual-channel optical microsensor designed for real-time monitoring of potassium and creatinine levels in whole blood. Utilizing 3D printing technology to design and fabricate microstructures, and integrating microchannels with a filtration layer, this microsensor requires only 10 μL of blood for single-pass sample filtration and dual-parameter detection. A novel passive blood sample pumping method is proposed, utilizing internal and external pressure differentials along with internal hydrophilic properties to facilitate sample flow into the detection chambers. Light-emitting diodes (LEDs) and photodiodes, positioned on either side of the detection chamber, are employed to measure the concentrations of blood indicators. The detection results can be instantly handheld read and uploaded to the cloud via intelligent terminal, enabling seamless follow-up diagnostics and treatment. Through multiple rounds of testing on animal serum samples, whole blood samples, and real porcine blood samples, this microsensor demonstrated excellent linearity and accuracy. This innovative microsensor, designed for direct testing from a minimal volume of whole blood, holds significant potential for improving CKD management, offering a portable, reliable alternative for preoperative diagnostics and home-based chronic disease monitoring.
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引用次数: 0
Colorimetric plasmonic sensing of formaldehyde by in situ formation of core-shell bimetallic gold–silver nanoparticles in liquid films
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343918
Nerea Villarino, Isela Lavilla, Francisco Pena-Pereira, Carlos Bendicho

Background

Plasmonic sensing approaches involving in-drop enrichment/sensing of volatiles have significantly improved the sensitivity and selectivity of noble metal nanoparticle (NP)-based analytical methods. Colloidal solutions act in these approaches both as acceptor phases and as recognizing elements for optical detection. However, the reduced surface area-to-volume (SA/V) ratio associated to the spherical configuration of NPs-containing microdrops hinders the mass transfer in the acceptor phase and thus results in suboptimal analytical performance. In this sense, the assessment of alternative geometries that could potentially enhance the mass transfer while ensuring ease of operation would be highly desirable.

Results

The present work evaluates the suitability of liquid films of plasmonic NPs for enrichment/colorimetric sensing purposes. For this, the circular section of affordable stainless steel safety pins is employed as holder of stable microvolume films with enhanced SA/V ratio. As a proof of concept, liquid films of spherical gold NPs containing Tollens’ reagent have been evaluated as acceptor phases for formaldehyde enrichment and sensing via in situ formation of core-shell bimetallic gold-silver nanoparticles. The performance of the proposed approach has been compared with that of alternative LPME approaches, showing 2.2–3.0-fold higher enrichment factors and improved sensitivity. The method yielded a limit of detection of 56.7 nM and a repeatability of 6.8 % (N = 8) when a portable cuvetteless microvolume UV–vis spectrophotometric system was used, and has been successfully applied to the determination of formaldehyde in different waters and textile samples.

Significance

The present study represents the first report that evaluates planar liquid films for simultaneous enrichment and optical sensing, and provides an effective and straightforward way to obtain liquid film-like configurations of variable volumes of acceptor phase for improved mass transfer. The proposed approach shows substantial potential for the development of sensors and nanosensors with enhanced sensitivity.
{"title":"Colorimetric plasmonic sensing of formaldehyde by in situ formation of core-shell bimetallic gold–silver nanoparticles in liquid films","authors":"Nerea Villarino,&nbsp;Isela Lavilla,&nbsp;Francisco Pena-Pereira,&nbsp;Carlos Bendicho","doi":"10.1016/j.aca.2025.343918","DOIUrl":"10.1016/j.aca.2025.343918","url":null,"abstract":"<div><h3>Background</h3><div>Plasmonic sensing approaches involving in-drop enrichment/sensing of volatiles have significantly improved the sensitivity and selectivity of noble metal nanoparticle (NP)-based analytical methods. Colloidal solutions act in these approaches both as acceptor phases and as recognizing elements for optical detection. However, the reduced surface area-to-volume (SA/V) ratio associated to the spherical configuration of NPs-containing microdrops hinders the mass transfer in the acceptor phase and thus results in suboptimal analytical performance. In this sense, the assessment of alternative geometries that could potentially enhance the mass transfer while ensuring ease of operation would be highly desirable.</div></div><div><h3>Results</h3><div>The present work evaluates the suitability of liquid films of plasmonic NPs for enrichment/colorimetric sensing purposes. For this, the circular section of affordable stainless steel safety pins is employed as holder of stable microvolume films with enhanced SA/V ratio. As a proof of concept, liquid films of spherical gold NPs containing Tollens’ reagent have been evaluated as acceptor phases for formaldehyde enrichment and sensing via <em>in situ</em> formation of core-shell bimetallic gold-silver nanoparticles. The performance of the proposed approach has been compared with that of alternative LPME approaches, showing 2.2–3.0-fold higher enrichment factors and improved sensitivity. The method yielded a limit of detection of 56.7 nM and a repeatability of 6.8 % (N = 8) when a portable cuvetteless microvolume UV–vis spectrophotometric system was used, and has been successfully applied to the determination of formaldehyde in different waters and textile samples.</div></div><div><h3>Significance</h3><div>The present study represents the first report that evaluates planar liquid films for simultaneous enrichment and optical sensing, and provides an effective and straightforward way to obtain liquid film-like configurations of variable volumes of acceptor phase for improved mass transfer. The proposed approach shows substantial potential for the development of sensors and nanosensors with enhanced sensitivity.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1352 ","pages":"Article 343918"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570262","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
Triphenylmethyl-based carbon biradical nanoparticles for magnetic resonance imaging
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-07 DOI: 10.1016/j.aca.2025.343897
Wenjia Tan , Xinru Li , Jiajing Zhu , Yihan Zhao , Wenzhao Wang , Feng Li
In recent years, luminescent carbon radicals have emerged as a promising functionalized material, with a primary focus on harnessing the potential of mono-radicals. The greater spin density exhibited by a single molecule in biradicals undoubtedly provides greater research value for its magnetic properties. Conventional metallic contrast agents represent the predominant choice in magnetic resonance imaging (MRI) of clinical applications. However, the accumulation of metal ions within the body poses potential safety risks. Hence, the exploration of innovative metal-free organic magnetic nanomaterials offers a safer alternative. This work introduces an innovative approach, presenting the first metal-free carbon-radical-based MRI contrast agent by encapsulating luminescent triphenylmethyl biradicals into nanoparticles (TTM-PhTTM NPs). These biradical NPs exhibit high water solubility, low cytotoxicity, and stability in highly reductive environments. Notably, TTM-PhTTM NPs maintained a strong electron paramagnetic resonance (EPR) signal even after exposure to ascorbic acid for 24 h, and cell viability remained above 80 % even at concentrations up to 1400 μg/mL. Moreover, TTM-PhTTM NPs demonstrated a T1 longitudinal relaxation rate of 0.35 mM−1s−1, one of the highest recorded for metal-free organic magnetic nanomaterials. Following a 6-h incubation period, significant enhancements in imaging contrast were observed, with T1 signal intensities increasing as the concentration of TTM-PhTTM NPs increased. This study paves the way for the utilization of stable, biocompatible carbon-based radicals as MRI contrast agents, underscoring their potential for safe and effective biomedical imaging applications and providing a solid foundation for further development of carbon radical-based imaging technologies.
{"title":"Triphenylmethyl-based carbon biradical nanoparticles for magnetic resonance imaging","authors":"Wenjia Tan ,&nbsp;Xinru Li ,&nbsp;Jiajing Zhu ,&nbsp;Yihan Zhao ,&nbsp;Wenzhao Wang ,&nbsp;Feng Li","doi":"10.1016/j.aca.2025.343897","DOIUrl":"10.1016/j.aca.2025.343897","url":null,"abstract":"<div><div>In recent years, luminescent carbon radicals have emerged as a promising functionalized material, with a primary focus on harnessing the potential of mono-radicals. The greater spin density exhibited by a single molecule in biradicals undoubtedly provides greater research value for its magnetic properties. Conventional metallic contrast agents represent the predominant choice in magnetic resonance imaging (MRI) of clinical applications. However, the accumulation of metal ions within the body poses potential safety risks. Hence, the exploration of innovative metal-free organic magnetic nanomaterials offers a safer alternative. This work introduces an innovative approach, presenting the first metal-free carbon-radical-based MRI contrast agent by encapsulating luminescent triphenylmethyl biradicals into nanoparticles (TTM-PhTTM NPs). These biradical NPs exhibit high water solubility, low cytotoxicity, and stability in highly reductive environments. Notably, TTM-PhTTM NPs maintained a strong electron paramagnetic resonance (EPR) signal even after exposure to ascorbic acid for 24 h, and cell viability remained above 80 % even at concentrations up to 1400 μg/mL. Moreover, TTM-PhTTM NPs demonstrated a T<sub>1</sub> longitudinal relaxation rate of 0.35 mM<sup>−1</sup>s<sup>−1</sup>, one of the highest recorded for metal-free organic magnetic nanomaterials. Following a 6-h incubation period, significant enhancements in imaging contrast were observed, with T<sub>1</sub> signal intensities increasing as the concentration of TTM-PhTTM NPs increased. This study paves the way for the utilization of stable, biocompatible carbon-based radicals as MRI contrast agents, underscoring their potential for safe and effective biomedical imaging applications and providing a solid foundation for further development of carbon radical-based imaging technologies.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1352 ","pages":"Article 343897"},"PeriodicalIF":5.7,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570261","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
Rapid separation and quantification of trace titanium dioxide with sizes down to 20 nm in environmental waters
IF 5.7 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-03-06 DOI: 10.1016/j.aca.2025.343905
Lijie Dong , Xiao He , Jingbo Chao

Background

Titanium dioxide nanoparticles (TiO2 NPs) are commonly used in consumer products, leading to their release into the environment and raising concerns about their potential human health risks. Smaller TiO2 NPs penetrate cell membranes more easily and exhibit stronger bio-toxicity than larger particles. However, methods for analyzing small TiO2 NPs are limited.

Results

A robust method to identify and quantify TiO2 NPs with size down to 20 nm within 5 min was developed, based on size-exclusion chromatography coupled with inductively coupled plasma mass spectrometry. To address the issue of column adsorption, salicylaldoxime (SO, 0.1 %) was used to complex ionic Ti and surfactant FL-70 (2 %) was used as the coating agent for TiO2 NPs in the mobile phase. Work conditions including column type, SO concentration, and FL-70 content were optimized. Consequently, the method successfully separated and quantified TiO2 NPs and ionic Ti species, with detection limits of 2.23 ng/mL for TiO2 NPs and 2.10 ng/mL for ionic Ti, meeting most application needs. Spiked recoveries of TiO2 NPs in environmental water samples ranged from 82.75 % to 95.09 %, verifying the method's practicality.

Significance

This method provides a powerful tool for rapid screening of smaller TiO2 NPs-containing environmental waters. Furthermore, the strategy proposed in this study to overcome column adsorption provides a useful model for the SEC separation and determination of other trace metal nanoparticles.
{"title":"Rapid separation and quantification of trace titanium dioxide with sizes down to 20 nm in environmental waters","authors":"Lijie Dong ,&nbsp;Xiao He ,&nbsp;Jingbo Chao","doi":"10.1016/j.aca.2025.343905","DOIUrl":"10.1016/j.aca.2025.343905","url":null,"abstract":"<div><h3>Background</h3><div>Titanium dioxide nanoparticles (TiO<sub>2</sub> NPs) are commonly used in consumer products, leading to their release into the environment and raising concerns about their potential human health risks. Smaller TiO<sub>2</sub> NPs penetrate cell membranes more easily and exhibit stronger bio-toxicity than larger particles. However, methods for analyzing small TiO<sub>2</sub> NPs are limited.</div></div><div><h3>Results</h3><div>A robust method to identify and quantify TiO<sub>2</sub> NPs with size down to 20 nm within 5 min was developed, based on size-exclusion chromatography coupled with inductively coupled plasma mass spectrometry. To address the issue of column adsorption, salicylaldoxime (SO, 0.1 %) was used to complex ionic Ti and surfactant FL-70 (2 %) was used as the coating agent for TiO<sub>2</sub> NPs in the mobile phase. Work conditions including column type, SO concentration, and FL-70 content were optimized. Consequently, the method successfully separated and quantified TiO<sub>2</sub> NPs and ionic Ti species, with detection limits of 2.23 ng/mL for TiO<sub>2</sub> NPs and 2.10 ng/mL for ionic Ti, meeting most application needs. Spiked recoveries of TiO<sub>2</sub> NPs in environmental water samples ranged from 82.75 % to 95.09 %, verifying the method's practicality.</div></div><div><h3>Significance</h3><div>This method provides a powerful tool for rapid screening of smaller TiO<sub>2</sub> NPs-containing environmental waters. Furthermore, the strategy proposed in this study to overcome column adsorption provides a useful model for the SEC separation and determination of other trace metal nanoparticles.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1351 ","pages":"Article 343905"},"PeriodicalIF":5.7,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569847","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
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Analytica Chimica Acta
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