Naghmeh Aboualigaledari, Anitha Jayapalan, Panesun Tukur, Mengxin Liu, Frank Tukur, Yanling Zhang, Gerald Ducatte, Madan Verma, Janet Tarus, Simona E. Hunyadi Murph and Jianjun Wei
The widespread distribution of herbicides in the environment poses a significant risk to human health and wildlife. Surface-enhanced Raman scattering (SERS) has emerged as a powerful technique for detecting and analyzing herbicides. However, developing a low-cost, highly sensitive, reproducible, stable, and Raman-active nanostructured substrate for herbicide detection remains a particular challenge. In this research, a nanohybrid substrate consisting of gold nanoparticles@carbon nanodots (AuNPs@CNDs) was synthesized by reducing HAuCl4 in the presence of CNDs at 100 °C. The optical, chemical, and physical properties of CNDs, AuNPs, and the hybrid AuNPs@CND substrates were thoroughly investigated using various techniques including UV-vis spectrometry, Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and CytoViva darkfield and hyperspectral imaging. The SERS effect of the substrates was evaluated using rhodamine 6G (Rh6G), a Raman-active probe, and two groups of herbicides containing mesotrione or S-metolachlor. The results demonstrated a significant signal amplification in the SERS spectra of Rh6G and herbicide molecule detection using the AuNPs@CND substrate compared to bare CNDs and AuNPs alone. This suggests that the nanohybrid AuNPs@CND SERS substrate holds promise for the detection of herbicides and other organic compounds in environmental applications.
{"title":"Surface-enhanced Raman scattering enhancement using a hybrid gold nanoparticles@carbon nanodot substrate for herbicide detection†","authors":"Naghmeh Aboualigaledari, Anitha Jayapalan, Panesun Tukur, Mengxin Liu, Frank Tukur, Yanling Zhang, Gerald Ducatte, Madan Verma, Janet Tarus, Simona E. Hunyadi Murph and Jianjun Wei","doi":"10.1039/D4AN00649F","DOIUrl":"10.1039/D4AN00649F","url":null,"abstract":"<p >The widespread distribution of herbicides in the environment poses a significant risk to human health and wildlife. Surface-enhanced Raman scattering (SERS) has emerged as a powerful technique for detecting and analyzing herbicides. However, developing a low-cost, highly sensitive, reproducible, stable, and Raman-active nanostructured substrate for herbicide detection remains a particular challenge. In this research, a nanohybrid substrate consisting of gold nanoparticles@carbon nanodots (AuNPs@CNDs) was synthesized by reducing HAuCl<small><sub>4</sub></small> in the presence of CNDs at 100 °C. The optical, chemical, and physical properties of CNDs, AuNPs, and the hybrid AuNPs@CND substrates were thoroughly investigated using various techniques including UV-vis spectrometry, Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and CytoViva darkfield and hyperspectral imaging. The SERS effect of the substrates was evaluated using rhodamine 6G (Rh6G), a Raman-active probe, and two groups of herbicides containing mesotrione or S-metolachlor. The results demonstrated a significant signal amplification in the SERS spectra of Rh6G and herbicide molecule detection using the AuNPs@CND substrate compared to bare CNDs and AuNPs alone. This suggests that the nanohybrid AuNPs@CND SERS substrate holds promise for the detection of herbicides and other organic compounds in environmental applications.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 21","pages":" 5277-5286"},"PeriodicalIF":3.6,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/an/d4an00649f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142101711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ying Wang, Xiaohan Li, Wenxiang Lu, Fuyu Li, Lingsong Yao, Zhiyu Liu, Huajuan Shi, Weizhong Zhang and Yunfei Bai
Considering the importance of accurate information of full-length (FL) transcripts in functional analysis, researchers prefer to develop new sequencing methods based on third-generation sequencing (TGS) rather than short-read sequencing. Several FL circRNA sequencing strategies have been developed. However, the current methods are inapplicable to low-biomass samples, since a large amount of total RNAs are acquired for circRNA enrichment before library preparation. In this work, we developed an effective method to detect FL circRNAs from a nanogram level (1–100 ng) of total RNAs based on a nanopore platform. Additionally, prior to the library preparation process, we added a series of 24 nt barcodes for each sample to reduce the cost and operating time. Using this method, we profiled circRNA expression in the striatum, hippocampus and cerebral cortex of a Parkinson's disease (PD) mouse model. Over 6% of reads were effective for FL circRNA identification in most datasets. Notably, a reduction in the RNA initial input resulted in a lower correlation between replicates and the detection efficiency for longer circRNA, but the lowest input (1 ng) was able to detect numerous FL circRNAs. Next, we systematically identified over 263 934 circRNAs in PD and healthy mice using the lower-input FL sequencing method, some of which came from 50.52% of PD-associated genes. Moreover, significant changes were observed in the circRNA expression pattern at an isoform level, and high-confidence protein translation evidence was predicted. Overall, we developed an effective method to characterize FL circRNAs from low-input samples and provide a comprehensive insight into the biological function of circRNAs in PD at an isoform level.
{"title":"Full-length circRNA sequencing method using low-input RNAs and profiling of circRNAs in MPTP-PD mice on a nanopore platform†","authors":"Ying Wang, Xiaohan Li, Wenxiang Lu, Fuyu Li, Lingsong Yao, Zhiyu Liu, Huajuan Shi, Weizhong Zhang and Yunfei Bai","doi":"10.1039/D4AN00715H","DOIUrl":"10.1039/D4AN00715H","url":null,"abstract":"<p >Considering the importance of accurate information of full-length (FL) transcripts in functional analysis, researchers prefer to develop new sequencing methods based on third-generation sequencing (TGS) rather than short-read sequencing. Several FL circRNA sequencing strategies have been developed. However, the current methods are inapplicable to low-biomass samples, since a large amount of total RNAs are acquired for circRNA enrichment before library preparation. In this work, we developed an effective method to detect FL circRNAs from a nanogram level (1–100 ng) of total RNAs based on a nanopore platform. Additionally, prior to the library preparation process, we added a series of 24 nt barcodes for each sample to reduce the cost and operating time. Using this method, we profiled circRNA expression in the striatum, hippocampus and cerebral cortex of a Parkinson's disease (PD) mouse model. Over 6% of reads were effective for FL circRNA identification in most datasets. Notably, a reduction in the RNA initial input resulted in a lower correlation between replicates and the detection efficiency for longer circRNA, but the lowest input (1 ng) was able to detect numerous FL circRNAs. Next, we systematically identified over 263 934 circRNAs in PD and healthy mice using the lower-input FL sequencing method, some of which came from 50.52% of PD-associated genes. Moreover, significant changes were observed in the circRNA expression pattern at an isoform level, and high-confidence protein translation evidence was predicted. Overall, we developed an effective method to characterize FL circRNAs from low-input samples and provide a comprehensive insight into the biological function of circRNAs in PD at an isoform level.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 20","pages":" 5118-5130"},"PeriodicalIF":3.6,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mudita Vats, Berta Cillero-Pastor, Eva Cuypers and Ron M. A. Heeren
Plant health, which affects the nutritional quality and safety of derivative food products, is influenced by symbiotic interactions with microorganisms. These interactions influence the local molecular profile at the tissue level. Therefore, studying the distribution of molecules within plants, microbes, and plant-based food is crucial to assess plant health, ensure the safety and quality of the agricultural products that become part of our food supply, and plan agricultural management practices. Within this framework, the molecular distribution within plant-based samples can be visualized with mass spectrometry imaging (MSI). This review describes key MSI methodologies, highlighting the role they play in unraveling the localization of metabolites, lipids, proteins, pigments, and elemental components across plants, microbes, and food products. Furthermore, investigations that involve multimodal molecular imaging approaches combining MSI with other imaging techniques are described. The advantages and limitations of the different MSI techniques that influence their applicability in diverse agro-food studies are described to enable informed choices for tailored analyses. For example, some MSI technologies involve meticulous sample preparation while others compromise spatial resolution to gain throughput. Key parameters such as sensitivity, ionization bias and fragmentation, reference database and compound class specificity are described and discussed in this review. With the ongoing refinements in instrumentation, data analysis, and integration of complementary techniques, MSI deepens our insight into the molecular biology of the agricultural ecosystem. This in turn empowers the quest for sustainable and productive agricultural practices.
{"title":"Mass spectrometry imaging in plants, microbes, and food: a review†","authors":"Mudita Vats, Berta Cillero-Pastor, Eva Cuypers and Ron M. A. Heeren","doi":"10.1039/D4AN00644E","DOIUrl":"10.1039/D4AN00644E","url":null,"abstract":"<p >Plant health, which affects the nutritional quality and safety of derivative food products, is influenced by symbiotic interactions with microorganisms. These interactions influence the local molecular profile at the tissue level. Therefore, studying the distribution of molecules within plants, microbes, and plant-based food is crucial to assess plant health, ensure the safety and quality of the agricultural products that become part of our food supply, and plan agricultural management practices. Within this framework, the molecular distribution within plant-based samples can be visualized with mass spectrometry imaging (MSI). This review describes key MSI methodologies, highlighting the role they play in unraveling the localization of metabolites, lipids, proteins, pigments, and elemental components across plants, microbes, and food products. Furthermore, investigations that involve multimodal molecular imaging approaches combining MSI with other imaging techniques are described. The advantages and limitations of the different MSI techniques that influence their applicability in diverse agro-food studies are described to enable informed choices for tailored analyses. For example, some MSI technologies involve meticulous sample preparation while others compromise spatial resolution to gain throughput. Key parameters such as sensitivity, ionization bias and fragmentation, reference database and compound class specificity are described and discussed in this review. With the ongoing refinements in instrumentation, data analysis, and integration of complementary techniques, MSI deepens our insight into the molecular biology of the agricultural ecosystem. This in turn empowers the quest for sustainable and productive agricultural practices.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 18","pages":" 4553-4582"},"PeriodicalIF":3.6,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/an/d4an00644e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142078485","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Modern criminal investigations heavily rely on trace bodily fluid evidence as a rich source of DNA. DNA profiling of such evidence can result in the identification of an individual if a matching DNA profile is available. Alternatively, phenotypic profiling based on the analysis of body fluid traces can significantly narrow down the pool of suspects in a criminal investigation. Urine stain is a frequently encountered specimen at the scene of crime. Raman spectroscopy offers great potential as a universal confirmatory method for the identification of all main body fluids, including urine. In this proof-of-concept study, Raman spectroscopy combined with advanced statistics was used for race differentiation based on the analysis of urine stains. Specifically, a Random Forest (RF) model was built, which allowed for differentiating Caucasian (CA) and African American (AA) descent donors with 90% accuracy based on Raman spectra of dried urine samples. Raman spectra were collected from samples of 28 donors varying in age and sex. This novel technology offers great potential as a universal forensic tool for phenotypic profiling of a potential suspect immediately at the scene of a crime, providing invaluable information for a criminal investigation.
现代刑事调查在很大程度上依赖于微量体液证据这一丰富的 DNA 来源。如果有匹配的 DNA 图谱,对这些证据进行 DNA 分析就能确定一个人的身份。另外,基于体液痕迹分析的表型特征分析也可以大大缩小刑事调查中嫌疑人的范围。尿渍是犯罪现场经常遇到的一种样本。拉曼光谱作为一种通用的确证方法,为包括尿液在内的所有主要体液的鉴定提供了巨大的潜力。在这项概念验证研究中,拉曼光谱与先进的统计学相结合,用于根据尿渍分析进行种族区分。具体来说,我们建立了一个随机森林(RF)模型,该模型可根据干燥尿液样本的拉曼光谱对高加索(CA)和非裔美国人(AA)后裔捐献者进行区分,准确率高达 90%。拉曼光谱采集自 28 位不同年龄和性别的捐献者样本。这项新技术作为一种通用的法医工具,可在犯罪现场立即对潜在嫌疑人进行表型分析,为刑事调查提供宝贵的信息,具有巨大的潜力。
{"title":"Phenotypic profiling based on body fluid traces discovered at the scene of crime: Raman spectroscopy of urine stains for race differentiation","authors":"Bhavik Vyas, Lenka Halámková and Igor K. Lednev","doi":"10.1039/D4AN00938J","DOIUrl":"10.1039/D4AN00938J","url":null,"abstract":"<p >Modern criminal investigations heavily rely on trace bodily fluid evidence as a rich source of DNA. DNA profiling of such evidence can result in the identification of an individual if a matching DNA profile is available. Alternatively, phenotypic profiling based on the analysis of body fluid traces can significantly narrow down the pool of suspects in a criminal investigation. Urine stain is a frequently encountered specimen at the scene of crime. Raman spectroscopy offers great potential as a universal confirmatory method for the identification of all main body fluids, including urine. In this proof-of-concept study, Raman spectroscopy combined with advanced statistics was used for race differentiation based on the analysis of urine stains. Specifically, a Random Forest (RF) model was built, which allowed for differentiating Caucasian (CA) and African American (AA) descent donors with 90% accuracy based on Raman spectra of dried urine samples. Raman spectra were collected from samples of 28 donors varying in age and sex. This novel technology offers great potential as a universal forensic tool for phenotypic profiling of a potential suspect immediately at the scene of a crime, providing invaluable information for a criminal investigation.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 20","pages":" 5081-5090"},"PeriodicalIF":3.6,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085381","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
DNA conformations, which encompass the three-dimensional structures of the DNA strand, play a crucial role in genome regulation. During DNA translocation in a nanopore, various conformations occur due to interactions among force fields, the fluidic environment, and polymer features. The most common conformation is folding, where DNA moves through the nanopore in a two-strand or multi-strand manner, influencing the current signature. Factors such as hydrodynamic drag, ionic environments, and DNA length significantly affect these conformations. Notably, conical nanopores, with their asymmetrical geometry, impose unique constraints on DNA translocation. Our findings reveal that during forward translocation, from the narrow (cis) end to the wide (trans) end, DNA experiences less resistance, resulting in shorter translocation times and higher blockade currents. Conversely, backward translocation, from the wide (trans) end to the narrow (cis) end, leads to longer translocation times and more complex conformations due to increased hydrodynamic drag and geometric constraints. This study employs molecular ping-pong methods to confine DNA, further highlighting the intricate dynamics of DNA folding within nanopores. These insights enhance the understanding of DNA behavior in confined environments, contributing to advancements in nanopore-based sensing and sequencing technologies, with implications for genome regulation and biomedical applications.
DNA 构象包括 DNA 链的三维结构,在基因组调控中起着至关重要的作用。DNA 在纳米孔中转运时,由于力场、流体环境和聚合物特征之间的相互作用,会出现各种构象。最常见的构象是折叠,DNA 以双链或多链的方式通过纳米孔,影响电流特征。流体动力阻力、离子环境和 DNA 长度等因素都会对这些构象产生重大影响。值得注意的是,锥形纳米孔具有不对称的几何形状,对 DNA 的转位造成了独特的限制。我们的研究结果表明,在前向转位过程中,即从窄(顺式)端到宽(反式)端,DNA 遇到的阻力较小,因此转位时间较短,阻塞电流较大。相反,从宽(反式)端向窄(顺式)端逆向转位时,由于流体动力阻力和几何限制增加,转位时间更长,构象更复杂。该研究采用分子乒乓方法来限制 DNA,进一步突出了 DNA 在纳米孔内折叠的复杂动态。这些见解加深了人们对 DNA 在封闭环境中行为的理解,有助于推动基于纳米孔的传感和测序技术的发展,并对基因组调控和生物医学应用产生影响。
{"title":"Distinct DNA conformations during forward and backward translocations through a conical nanopore†","authors":"Fei Zheng and Quan Han","doi":"10.1039/D4AN01068J","DOIUrl":"10.1039/D4AN01068J","url":null,"abstract":"<p >DNA conformations, which encompass the three-dimensional structures of the DNA strand, play a crucial role in genome regulation. During DNA translocation in a nanopore, various conformations occur due to interactions among force fields, the fluidic environment, and polymer features. The most common conformation is folding, where DNA moves through the nanopore in a two-strand or multi-strand manner, influencing the current signature. Factors such as hydrodynamic drag, ionic environments, and DNA length significantly affect these conformations. Notably, conical nanopores, with their asymmetrical geometry, impose unique constraints on DNA translocation. Our findings reveal that during forward translocation, from the narrow (<em>cis</em>) end to the wide (<em>trans</em>) end, DNA experiences less resistance, resulting in shorter translocation times and higher blockade currents. Conversely, backward translocation, from the wide (<em>trans</em>) end to the narrow (<em>cis</em>) end, leads to longer translocation times and more complex conformations due to increased hydrodynamic drag and geometric constraints. This study employs molecular ping-pong methods to confine DNA, further highlighting the intricate dynamics of DNA folding within nanopores. These insights enhance the understanding of DNA behavior in confined environments, contributing to advancements in nanopore-based sensing and sequencing technologies, with implications for genome regulation and biomedical applications.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 20","pages":" 5131-5138"},"PeriodicalIF":3.6,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/an/d4an01068j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Felix Frank, Daniela Tomasetig, Peter Nahringbauer, Wolfgang Ipsmiller, Gerd Mauschitz, Karin Wieland and Bernhard Lendl
Cationic surfactants are widely used as corrosion inhibitors for industrial tubings and pipelines. They protect the surface of steel pipes through a film-forming mechanism, providing both anodic and cathodic inhibition. To improve the efficiency of the corrosion protection, it is essential to understand the interactions between the surfactants and metal surfaces. To achieve this, surface enhanced Raman spectroscopy (SERS) can serve as a powerful tool due to its surface sensitivity and potential to detect trace amounts of analytes in complex media. In this contribution, we have investigated the behaviour of in situ prepared AgNPs in the presence of benzalkonium chloride as a model corrosion inhibitor using SERS coupled to visible spectroscopy and combined with light scattering methods. By combining these experimental methods, we were able to correlate the aggregation of silver particles with the concentration of added surfactant in the resulting mixture. Using this insight, we also established a SERS method for the detection of benzalkonium chloride traces in water. For this, we utilised the quenching of the SERS response of methylene blue by competitive adsorption of methylene blue and the surfactant on SERS active AgNPs. We believe that our approach can serve a variety of applications to improve the industrial water treatment. For example, the modelling of the interaction of different surfactants with SERS can be used for process intensification, and ultimately, to move towards the digital twinning of corrosion processes for more efficient corrosion inhibition. Furthermore, the ability to adapt our sensing protocol for on-line corrosion inhibitor monitoring allows a fast response to process changes, hence, enabling resource-efficient, continuous process control.
{"title":"In situ study of the interactions between metal surfaces and cationic surfactant corrosion inhibitors by surface-enhanced Raman spectroscopy coupled with visible spectroscopy†","authors":"Felix Frank, Daniela Tomasetig, Peter Nahringbauer, Wolfgang Ipsmiller, Gerd Mauschitz, Karin Wieland and Bernhard Lendl","doi":"10.1039/D4AN00861H","DOIUrl":"10.1039/D4AN00861H","url":null,"abstract":"<p >Cationic surfactants are widely used as corrosion inhibitors for industrial tubings and pipelines. They protect the surface of steel pipes through a film-forming mechanism, providing both anodic and cathodic inhibition. To improve the efficiency of the corrosion protection, it is essential to understand the interactions between the surfactants and metal surfaces. To achieve this, surface enhanced Raman spectroscopy (SERS) can serve as a powerful tool due to its surface sensitivity and potential to detect trace amounts of analytes in complex media. In this contribution, we have investigated the behaviour of <em>in situ</em> prepared AgNPs in the presence of benzalkonium chloride as a model corrosion inhibitor using SERS coupled to visible spectroscopy and combined with light scattering methods. By combining these experimental methods, we were able to correlate the aggregation of silver particles with the concentration of added surfactant in the resulting mixture. Using this insight, we also established a SERS method for the detection of benzalkonium chloride traces in water. For this, we utilised the quenching of the SERS response of methylene blue by competitive adsorption of methylene blue and the surfactant on SERS active AgNPs. We believe that our approach can serve a variety of applications to improve the industrial water treatment. For example, the modelling of the interaction of different surfactants with SERS can be used for process intensification, and ultimately, to move towards the digital twinning of corrosion processes for more efficient corrosion inhibition. Furthermore, the ability to adapt our sensing protocol for on-line corrosion inhibitor monitoring allows a fast response to process changes, hence, enabling resource-efficient, continuous process control.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 22","pages":" 5372-5380"},"PeriodicalIF":3.6,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/an/d4an00861h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085273","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jian Song, Wenlong Liang, Hongtao Huang, Hongyan Jia, Shouning Yang, Chunlei Wang and Huayan Yang
Typing of bacterial subspecies is urgently needed for the diagnosis and efficient treatment during disease outbreaks. Physicochemical spectroscopy can provide a rapid analysis but its identification accuracy is still far from satisfactory. Herein, a novel feature-extractor-based fusion-assisted machine learning strategy has been developed for high accuracy and rapid strain differentiation using matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) and Raman spectroscopy. Based on this fusion approach, rapid and reliable identification and analysis can be performed within 24 hours. Validation on a panel of important pathogens comprising Staphylococcus aureus, Klebsiella pneumoniae, Escherichia coli, and Acinetobacter baumannii showed that the identification accuracies of k-nearest neighbors (KNNs), support vector machines (SVMs) and artificial neural networks (ANNs) were 100%. In particular, when benchmarked against a MALDI-TOF MS spectral dataset, the new approach improved the identification accuracy of Acinetobacter baumannii from 87.67% to 100%. This work demonstrates the effectiveness of combining MALDI-TOF MS and Raman spectroscopy fusion data in pathogenic bacterial subtyping.
在疾病爆发期间,迫切需要对细菌亚种进行分型,以便进行诊断和有效治疗。理化光谱法可提供快速分析,但其鉴定准确性仍远远不能令人满意。在此,我们开发了一种新颖的基于特征提取器的融合辅助机器学习策略,利用基质辅助激光解吸电离飞行时间质谱(MALDI-TOF MS)和拉曼光谱进行高精度和快速的菌种鉴别。基于这种融合方法,可在 24 小时内进行快速可靠的鉴定和分析。对金黄色葡萄球菌、肺炎克雷伯氏菌、大肠埃希菌和鲍曼不动杆菌等重要病原体的验证表明,K-近邻(KNN)、支持向量机(SVM)和人工神经网络(ANN)的识别准确率均为 100%。特别是在以 MALDI-TOF MS 图谱数据集为基准时,新方法将鲍曼不动杆菌的识别准确率从 87.67% 提高到了 100%。这项工作证明了结合 MALDI-TOF MS 和拉曼光谱融合数据在病原菌亚型鉴定中的有效性。
{"title":"A new fusion strategy for rapid strain differentiation based on MALDI-TOF MS and Raman spectra†","authors":"Jian Song, Wenlong Liang, Hongtao Huang, Hongyan Jia, Shouning Yang, Chunlei Wang and Huayan Yang","doi":"10.1039/D4AN00916A","DOIUrl":"10.1039/D4AN00916A","url":null,"abstract":"<p >Typing of bacterial subspecies is urgently needed for the diagnosis and efficient treatment during disease outbreaks. Physicochemical spectroscopy can provide a rapid analysis but its identification accuracy is still far from satisfactory. Herein, a novel feature-extractor-based fusion-assisted machine learning strategy has been developed for high accuracy and rapid strain differentiation using matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) and Raman spectroscopy. Based on this fusion approach, rapid and reliable identification and analysis can be performed within 24 hours. Validation on a panel of important pathogens comprising <em>Staphylococcus aureus</em>, <em>Klebsiella pneumoniae</em>, <em>Escherichia coli</em>, and <em>Acinetobacter baumannii</em> showed that the identification accuracies of k-nearest neighbors (KNNs), support vector machines (SVMs) and artificial neural networks (ANNs) were 100%. In particular, when benchmarked against a MALDI-TOF MS spectral dataset, the new approach improved the identification accuracy of <em>Acinetobacter baumannii</em> from 87.67% to 100%. This work demonstrates the effectiveness of combining MALDI-TOF MS and Raman spectroscopy fusion data in pathogenic bacterial subtyping.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 21","pages":" 5287-5297"},"PeriodicalIF":3.6,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Glyphosate (GLY) is widely applied in agriculture and horticulture as a herbicide. The development of genetically modified plants has caused abuse of GLY, with excessive residues potentially causing harm to human health. Consequently, a novel method needs to be built to detect GLY in soybeans and corn. Computer simulation was used to design an excellent hapten which was used to produce an anti-GLY monoclonal antibody (mAb) with outstanding sensitivity and affinity, and its 50%-inhibitory concentration (IC50) was 128.59 ng mL−1. Afterwards, an immunochromatographic assay strip was developed based on the mAb. In soybeans and corn, the visual detection limits were 1 mg kg−1 and 0.2 mg kg−1, while the cut-off values were 50 mg kg−1 and 5 mg kg−1, respectively. The reliability of the strips was proved by the existing methods. Thus, a rapid method to detect GLY residues on-site in soybeans and corn was established.
{"title":"A lateral strip assay for ultrasensitive detection of glyphosate in soybeans and corn†","authors":"Xuyang Ma, Liqiang Liu, Shanshan Song, Hua Kuang, Chuanlai Xu and Xinxin Xu","doi":"10.1039/D4AN00958D","DOIUrl":"10.1039/D4AN00958D","url":null,"abstract":"<p >Glyphosate (GLY) is widely applied in agriculture and horticulture as a herbicide. The development of genetically modified plants has caused abuse of GLY, with excessive residues potentially causing harm to human health. Consequently, a novel method needs to be built to detect GLY in soybeans and corn. Computer simulation was used to design an excellent hapten which was used to produce an anti-GLY monoclonal antibody (mAb) with outstanding sensitivity and affinity, and its 50%-inhibitory concentration (IC<small><sub>50</sub></small>) was 128.59 ng mL<small><sup>−1</sup></small>. Afterwards, an immunochromatographic assay strip was developed based on the mAb. In soybeans and corn, the visual detection limits were 1 mg kg<small><sup>−1</sup></small> and 0.2 mg kg<small><sup>−1</sup></small>, while the cut-off values were 50 mg kg<small><sup>−1</sup></small> and 5 mg kg<small><sup>−1</sup></small>, respectively. The reliability of the strips was proved by the existing methods. Thus, a rapid method to detect GLY residues on-site in soybeans and corn was established.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 21","pages":" 5232-5242"},"PeriodicalIF":3.6,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Benting Xie, Shimao Du, Hejun Gao, Juan Zhang, Hongquan Fu and Yunwen Liao
Detecting multiple targets in complex cellular and biological environments yields more reliable results than single-label assays. Here, we introduced an electrochemical biosensor equipped with computing functions, acting as a smart automaton to enable computing-based detection. By defining the logic combinations of miR-21 and miR-122 as detection patterns, we proposed the corresponding AND and OR detection automata. In both logic gate modes, miR-21 and miR-122 could be replaced with single-stranded FO or FA, modified with Fc, binding to the S chain on the electrode surface. This process led to a significant decrease in the square wave voltammetry (SWV) of Fc on the same sensing platform, as numerous ferrocene (Fc)-tagged DNA fragments escaped from the electrode surface. Experimental results indicated that both automata efficiently and sensitively detected the presence of the two targets. This strategy highlighted how a small amount of target could generate a large current signal decrease in the logic automata, significantly reducing the detection limit for monitoring low-abundance targets. Moreover, the short-stranded DNA components of the detection automata exhibited a simple composition and easy programmability of probe sequences, offering an innovative detection mode. This simplified the complex process of detection, data collection, computation, and evaluation. The direct detection result (“0” or “1”) was exported according to the embedded computation code. This approach could be expanded into a detection system for identifying other sets of biomarkers, enhancing its potential for clinical applications.
在复杂的细胞和生物环境中检测多个目标比单标记检测能获得更可靠的结果。在这里,我们介绍了一种配备计算功能的电化学生物传感器,它就像智能自动机一样实现了基于计算的检测。通过定义 miR-21 和 miR-122 的逻辑组合作为检测模式,我们提出了相应的 AND 和 OR 检测自动机。在这两种逻辑门模式中,miR-21 和 miR-122 都可以用单链 FO 或 FA 代替,并用 Fc 修饰,与电极表面的 S 链结合。这一过程导致 Fc 在同一传感平台上的方波伏安法(SWV)显著下降,因为大量二茂铁(Fc)标记的 DNA 片段从电极表面逃逸。实验结果表明,这两种自动装置都能高效、灵敏地判断两个目标的存在。这一策略凸显了少量目标物如何在逻辑自动机中产生较大的电流信号下降,从而大大降低了监测低丰度目标物的检测限。此外,检测自动装置的短链 DNA 组件成分简单,探针序列易于编程,提供了一种创新的检测模式。这简化了复杂的检测、数据收集、计算和评估过程。直接检测结果("0 "或 "1")根据嵌入的计算代码输出。这种方法可扩展为识别其他生物标记物的检测系统,从而提高其临床应用潜力。
{"title":"An electrochemical biosensor equipped with a logic circuit as a smart automaton for two-miRNA pattern detection†","authors":"Benting Xie, Shimao Du, Hejun Gao, Juan Zhang, Hongquan Fu and Yunwen Liao","doi":"10.1039/D4AN00719K","DOIUrl":"10.1039/D4AN00719K","url":null,"abstract":"<p >Detecting multiple targets in complex cellular and biological environments yields more reliable results than single-label assays. Here, we introduced an electrochemical biosensor equipped with computing functions, acting as a smart automaton to enable computing-based detection. By defining the logic combinations of miR-21 and miR-122 as detection patterns, we proposed the corresponding AND and OR detection automata. In both logic gate modes, miR-21 and miR-122 could be replaced with single-stranded F<small><sub>O</sub></small> or F<small><sub>A</sub></small>, modified with Fc, binding to the S chain on the electrode surface. This process led to a significant decrease in the square wave voltammetry (SWV) of Fc on the same sensing platform, as numerous ferrocene (Fc)-tagged DNA fragments escaped from the electrode surface. Experimental results indicated that both automata efficiently and sensitively detected the presence of the two targets. This strategy highlighted how a small amount of target could generate a large current signal decrease in the logic automata, significantly reducing the detection limit for monitoring low-abundance targets. Moreover, the short-stranded DNA components of the detection automata exhibited a simple composition and easy programmability of probe sequences, offering an innovative detection mode. This simplified the complex process of detection, data collection, computation, and evaluation. The direct detection result (“0” or “1”) was exported according to the embedded computation code. This approach could be expanded into a detection system for identifying other sets of biomarkers, enhancing its potential for clinical applications.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 20","pages":" 5110-5117"},"PeriodicalIF":3.6,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085344","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chao Han, Shumu Li, Qingwei Yue, Na Li, Hui Yang and Zhenwen Zhao
Correction for ‘Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain’ by Chao Han et al., Analyst, 2019, 144, 6304–6312, https://doi.org/10.1039/C9AN01361J.
韩超等 "Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain "的更正,《分析家》,2019,144,6304-6312,https://doi.org/10.1039/C9AN01361J。
{"title":"Correction: Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain","authors":"Chao Han, Shumu Li, Qingwei Yue, Na Li, Hui Yang and Zhenwen Zhao","doi":"10.1039/D4AN90066A","DOIUrl":"10.1039/D4AN90066A","url":null,"abstract":"<p >Correction for ‘Polydopamine-capped AgNPs as a novel matrix overcoming the ion suppression of phosphatidylcholine for MALDI MS comprehensive imaging of glycerophospholipids and sphingolipids in impact-induced injured brain’ by Chao Han <em>et al.</em>, <em>Analyst</em>, 2019, <strong>144</strong>, 6304–6312, https://doi.org/10.1039/C9AN01361J.</p>","PeriodicalId":63,"journal":{"name":"Analyst","volume":" 18","pages":" 4757-4757"},"PeriodicalIF":3.6,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/an/d4an90066a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142034552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}