Pub Date : 2023-12-11DOI: 10.1021/acsmeasuresciau.3c00061
Robert D. Crapnell, Prashanth S. Adarakatti and Craig E. Banks*,
Mesalamine, known as 5-aminosalicylic acid, is a medication used primarily in the treatment of inflammatory bowel disease, including ulcerative colitis and Crohn’s disease. 5-Aminosalicylic acid can be measured using various benchtop laboratory techniques which involve liquid chromatography–mass spectroscopy, but these are sophisticated and large, meaning that they cannot be used on-site because transportation of the samples, chemicals, and physical and biological reactions can potentially occur, which can affect the sample’s composition and potentially result in inaccurate results. An alternative approach is the use of electrochemical based sensing platforms which has the advantages of portability, cost-efficiency, facile miniaturization, and rapid analysis while nonetheless providing sensitivity and selectivity. We provide an overview of the use of the electroanalytical techniques for the sensing of 5-aminosalicylic acid and compare them to other laboratory-based measurements. The applications, challenges faced, and future opportunities for electroanalytical based sensing platforms are presented in this review.
{"title":"Electroanalytical Overview: The Sensing of Mesalamine (5-Aminosalicylic Acid)","authors":"Robert D. Crapnell, Prashanth S. Adarakatti and Craig E. Banks*, ","doi":"10.1021/acsmeasuresciau.3c00061","DOIUrl":"10.1021/acsmeasuresciau.3c00061","url":null,"abstract":"<p >Mesalamine, known as 5-aminosalicylic acid, is a medication used primarily in the treatment of inflammatory bowel disease, including ulcerative colitis and Crohn’s disease. 5-Aminosalicylic acid can be measured using various benchtop laboratory techniques which involve liquid chromatography–mass spectroscopy, but these are sophisticated and large, meaning that they cannot be used on-site because transportation of the samples, chemicals, and physical and biological reactions can potentially occur, which can affect the sample’s composition and potentially result in inaccurate results. An alternative approach is the use of electrochemical based sensing platforms which has the advantages of portability, cost-efficiency, facile miniaturization, and rapid analysis while nonetheless providing sensitivity and selectivity. We provide an overview of the use of the electroanalytical techniques for the sensing of 5-aminosalicylic acid and compare them to other laboratory-based measurements. The applications, challenges faced, and future opportunities for electroanalytical based sensing platforms are presented in this review.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"42–53"},"PeriodicalIF":0.0,"publicationDate":"2023-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138577084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-12-07DOI: 10.1021/acsmeasuresciau.3c00052
Muhammad Saqib*, Mariam Zafar, Mohamed Ibrahim Halawa, Shahzad Murtaza, Ghulam Mustafa Kamal and Guobao Xu,
Single-particle-level measurements, during the reaction, avoid averaging effects that are inherent limitations of conventional ensemble strategies. It allows revealing structure–activity relationships beyond averaged properties by considering crucial particle-selective descriptors including structure/morphology dynamics, intrinsic heterogeneity, and dynamic fluctuations in reactivity (kinetics, mechanisms). In recent years, numerous luminescence (optical) techniques such as chemiluminescence (CL), electrochemiluminescence (ECL), and fluorescence (FL) microscopies have been emerging as dominant tools to achieve such measurements, owing to their diversified spectroscopy principles, noninvasive nature, higher sensitivity, and sufficient spatiotemporal resolution. Correspondingly, state-of-the-art methodologies and tools are being used for probing (real-time, operando, in situ) diverse applications of single particles in sensing, medicine, and catalysis. Herein, we provide a concise and comprehensive perspective on luminescence-based detection and imaging of single particles by putting special emphasis on their basic principles, mechanistic pathways, advances, challenges, and key applications. This Perspective focuses on the development of emission intensities and imaging based individual particle detection. Moreover, several key examples in the areas of sensing, motion, catalysis, energy, materials, and emerging trends in related areas are documented. We finally conclude with the opportunities and remaining challenges to stimulate further developments in this field.
{"title":"Nanoscale Luminescence Imaging/Detection of Single Particles: State-of-the-Art and Future Prospects","authors":"Muhammad Saqib*, Mariam Zafar, Mohamed Ibrahim Halawa, Shahzad Murtaza, Ghulam Mustafa Kamal and Guobao Xu, ","doi":"10.1021/acsmeasuresciau.3c00052","DOIUrl":"10.1021/acsmeasuresciau.3c00052","url":null,"abstract":"<p >Single-particle-level measurements, during the reaction, avoid averaging effects that are inherent limitations of conventional ensemble strategies. It allows revealing structure–activity relationships beyond averaged properties by considering crucial particle-selective descriptors including structure/morphology dynamics, intrinsic heterogeneity, and dynamic fluctuations in reactivity (kinetics, mechanisms). In recent years, numerous luminescence (optical) techniques such as chemiluminescence (CL), electrochemiluminescence (ECL), and fluorescence (FL) microscopies have been emerging as dominant tools to achieve such measurements, owing to their diversified spectroscopy principles, noninvasive nature, higher sensitivity, and sufficient spatiotemporal resolution. Correspondingly, state-of-the-art methodologies and tools are being used for probing (real-time, operando, in situ) diverse applications of single particles in sensing, medicine, and catalysis. Herein, we provide a concise and comprehensive perspective on luminescence-based detection and imaging of single particles by putting special emphasis on their basic principles, mechanistic pathways, advances, challenges, and key applications. This Perspective focuses on the development of emission intensities and imaging based individual particle detection. Moreover, several key examples in the areas of sensing, motion, catalysis, energy, materials, and emerging trends in related areas are documented. We finally conclude with the opportunities and remaining challenges to stimulate further developments in this field.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"3–24"},"PeriodicalIF":0.0,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00052","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138545847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-12-07DOI: 10.1021/acsmeasuresciau.3c00055
Wei Wang, Carmen R. de Nier, Manfred Wuhrer and Guinevere S.M. Lageveen-Kammeijer*,
Prostate-specific antigen (PSA) is a well-known clinical biomarker in prostate cancer (PCa) diagnosis, but a better test is still needed, as the serum-level-based PSA quantification exhibits limited specificity and comes with poor predictive value. Prior to PSA, prostatic acid phosphatase (PAP) was used, but it was replaced by PSA because PSA improved the early detection of PCa. Upon revisiting PAP and its glycosylation specifically, it appears to be a promising new biomarker candidate. Namely, previous studies have indicated that PAP glycoforms differ between PCa and non-PCa individuals. However, an in-depth characterization of PAP glycosylation is still lacking. In this study, we established an in-depth glycoproteomic assay for urinary PAP by characterizing both the micro- and macroheterogeneity of the PAP glycoprofile. For this purpose, PAP samples were analyzed by capillary electrophoresis coupled to mass spectrometry after affinity purification from urine and proteolytic digestion. The developed urinary PAP assay was applied on a pooled DRE (digital rectal examination) urine sample from nine individuals. Three glycosylation sites were characterized, namely N94, N220, and N333, via N-glycopeptide analysis. Taking sialic acid linkage isomers into account, a total of 63, 27, and 4 N-glycan structures were identified, respectively. The presented PAP glycoproteomic assay will enable the determination of potential glycomic biomarkers for the early detection and prognosis of PCa in cohort studies.
前列腺特异性抗原(PSA)是诊断前列腺癌(PCa)的著名临床生物标志物,但由于基于血清水平的 PSA 定量特异性有限且预测价值不高,因此仍需要更好的检测方法。在 PSA 之前,人们使用前列腺酸性磷酸酶(PAP),但由于 PSA 提高了 PCa 的早期检测率,PAP 被 PSA 所取代。重新审视前列腺酸性磷酸酶及其糖基化特性后,它似乎是一个很有希望的候选生物标记物。也就是说,以前的研究表明 PCa 患者和非 PCa 患者的 PAP 糖基化形式不同。然而,目前仍缺乏对 PAP 糖基化的深入研究。在本研究中,我们通过表征 PAP 糖型的微观和宏观异质性,建立了尿液 PAP 的深入糖蛋白组学检测方法。为此,在对尿液进行亲和纯化和蛋白水解消化后,采用毛细管电泳结合质谱法对 PAP 样品进行了分析。所开发的尿液 PAP 检测方法适用于来自九个人的 DRE(数字直肠检查)尿液样本。通过 N-糖肽分析,确定了三个糖基化位点,即 N94、N220 和 N333。考虑到半乳淀粉酸连接异构体,共鉴定出 63、27 和 4 个 N-糖结构。所介绍的 PAP 糖蛋白组测定方法将有助于确定潜在的糖生物标记物,以便在队列研究中对 PCa 进行早期检测和预后判断。
{"title":"In-Depth Glycoproteomic Assay of Urinary Prostatic Acid Phosphatase","authors":"Wei Wang, Carmen R. de Nier, Manfred Wuhrer and Guinevere S.M. Lageveen-Kammeijer*, ","doi":"10.1021/acsmeasuresciau.3c00055","DOIUrl":"10.1021/acsmeasuresciau.3c00055","url":null,"abstract":"<p >Prostate-specific antigen (PSA) is a well-known clinical biomarker in prostate cancer (PCa) diagnosis, but a better test is still needed, as the serum-level-based PSA quantification exhibits limited specificity and comes with poor predictive value. Prior to PSA, prostatic acid phosphatase (PAP) was used, but it was replaced by PSA because PSA improved the early detection of PCa. Upon revisiting PAP and its glycosylation specifically, it appears to be a promising new biomarker candidate. Namely, previous studies have indicated that PAP glycoforms differ between PCa and non-PCa individuals. However, an in-depth characterization of PAP glycosylation is still lacking. In this study, we established an in-depth glycoproteomic assay for urinary PAP by characterizing both the micro- and macroheterogeneity of the PAP glycoprofile. For this purpose, PAP samples were analyzed by capillary electrophoresis coupled to mass spectrometry after affinity purification from urine and proteolytic digestion. The developed urinary PAP assay was applied on a pooled DRE (digital rectal examination) urine sample from nine individuals. Three glycosylation sites were characterized, namely N<sub>94</sub>, N<sub>220</sub>, and N<sub>333</sub>, via <i>N</i>-glycopeptide analysis. Taking sialic acid linkage isomers into account, a total of 63, 27, and 4 <i>N</i>-glycan structures were identified, respectively. The presented PAP glycoproteomic assay will enable the determination of potential glycomic biomarkers for the early detection and prognosis of PCa in cohort studies.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"117–126"},"PeriodicalIF":0.0,"publicationDate":"2023-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138552272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-12-05DOI: 10.1021/acsmeasuresciau.3c00051
Jana M. Carpenter, Hannah M. Hynds, Kingsley Bimpeh and Kelly M. Hines*,
Although MALDI-ToF platforms for microbial identifications have found great success in clinical microbiology, the sole use of protein fingerprints for the discrimination of closely related species, strain-level identifications, and detection of antimicrobial resistance remains a challenge for the technology. Several alternative mass spectrometry-based methods have been proposed to address the shortcomings of the protein-centric approach, including MALDI-ToF methods for fatty acid/lipid profiling and LC-MS profiling of metabolites. However, the molecular diversity of microbial pathogens suggests that no single “ome” will be sufficient for the accurate and sensitive identification of strain- and susceptibility-level profiling of bacteria. Here, we describe the development of an alternative approach to microorganism profiling that relies upon both metabolites and lipids rather than a single class of biomolecule. Single-phase extractions based on butanol, acetonitrile, and water (the BAW method) were evaluated for the recovery of lipids and metabolites from Gram-positive and -negative microorganisms. We found that BAW extraction solutions containing 45% butanol provided optimal recovery of both molecular classes in a single extraction. The single-phase extraction method was coupled to hydrophilic interaction liquid chromatography (HILIC) and ion mobility-mass spectrometry (IM-MS) to resolve similar-mass metabolites and lipids in three dimensions and provide multiple points of evidence for feature annotation in the absence of tandem mass spectrometry. We demonstrate that the combined use of metabolites and lipids can be used to differentiate microorganisms to the species- and strain-level for four of the ESKAPE pathogens (Enterococcus faecium, Staphylococcus aureus, Acinetobacter baumannii, and Pseudomonas aeruginosa) using data from a single ionization mode. These results present promising, early stage evidence for the use of multiomic signatures for the identification of microorganisms by liquid chromatography, ion mobility, and mass spectrometry that, upon further development, may improve upon the level of identification provided by current methods.
{"title":"HILIC-IM-MS for Simultaneous Lipid and Metabolite Profiling of Bacteria","authors":"Jana M. Carpenter, Hannah M. Hynds, Kingsley Bimpeh and Kelly M. Hines*, ","doi":"10.1021/acsmeasuresciau.3c00051","DOIUrl":"10.1021/acsmeasuresciau.3c00051","url":null,"abstract":"<p >Although MALDI-ToF platforms for microbial identifications have found great success in clinical microbiology, the sole use of protein fingerprints for the discrimination of closely related species, strain-level identifications, and detection of antimicrobial resistance remains a challenge for the technology. Several alternative mass spectrometry-based methods have been proposed to address the shortcomings of the protein-centric approach, including MALDI-ToF methods for fatty acid/lipid profiling and LC-MS profiling of metabolites. However, the molecular diversity of microbial pathogens suggests that no single “ome” will be sufficient for the accurate and sensitive identification of strain- and susceptibility-level profiling of bacteria. Here, we describe the development of an alternative approach to microorganism profiling that relies upon both metabolites and lipids rather than a single class of biomolecule. Single-phase extractions based on butanol, acetonitrile, and water (the BAW method) were evaluated for the recovery of lipids and metabolites from Gram-positive and -negative microorganisms. We found that BAW extraction solutions containing 45% butanol provided optimal recovery of both molecular classes in a single extraction. The single-phase extraction method was coupled to hydrophilic interaction liquid chromatography (HILIC) and ion mobility-mass spectrometry (IM-MS) to resolve similar-mass metabolites and lipids in three dimensions and provide multiple points of evidence for feature annotation in the absence of tandem mass spectrometry. We demonstrate that the combined use of metabolites and lipids can be used to differentiate microorganisms to the species- and strain-level for four of the ESKAPE pathogens (<i>Enterococcus faecium</i>, <i>Staphylococcus aureus</i>, <i>Acinetobacter baumannii</i>, and <i>Pseudomonas aeruginosa</i>) using data from a single ionization mode. These results present promising, early stage evidence for the use of multiomic signatures for the identification of microorganisms by liquid chromatography, ion mobility, and mass spectrometry that, upon further development, may improve upon the level of identification provided by current methods.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"104–116"},"PeriodicalIF":0.0,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138539140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-12-05DOI: 10.1021/acsmeasuresciau.3c00049
Nipunika H. Godage, Song S. Qian, Erasmus Cudjoe and Emanuela Gionfriddo*,
This study addresses the challenges of matrix effects and interspecies plasma protein binding (PPB) on measurement variability during method validation across diverse plasma types (human, rat, rabbit, and bovine). Accurate measurements of small molecules in plasma samples often require matrix-matched calibration approaches with the use of specific plasma types, which may have limited availability or affordability. To mitigate the costs associated with human plasma measurements, we explore in this work the potential of cross-matrix-matched calibration using Bayesian hierarchical modeling (BHM) to correct for matrix effects associated with PPB. We initially developed a targeted quantitative approach utilizing biocompatible solid-phase microextraction coupled with liquid chromatography–mass spectrometry for xenobiotic analysis in plasma. The method was evaluated for absolute matrix effects across human, bovine, rat, and rabbit plasma comparing pre- and postmatrix extraction standards. Absolute matrix effects from 96 to 108% for most analytes across plasma sources indicate that the biocompatibility of the extraction phase minimizes interference coextraction. However, the extent of PPB in different media can still affect the accuracy of the measurement when the extraction of small molecules is carried out via free concentration, as in the case of microextraction techniques. In fact, while matrix-matched calibration revealed high accuracy, cross-matrix calibration (e.g., using a calibration curve generated from bovine plasma) proved inadequate for precise measurements in human plasma. A BHM was used to calculate correction factors for each analyte within each plasma type, successfully mitigating the measurement bias resulting from diverse calibration curve types used to quantify human plasma samples. This work contributes to the development of cost-effective, efficient calibration strategies for biofluids. Leveraging easily accessible plasma sources, like bovine plasma, for method optimization and validation prior to analyzing costly plasma (e.g., human plasma) holds substantial advantages applicable to biomonitoring and pharmacokinetic studies.
{"title":"Enhancing Quantitative Analysis of Xenobiotics in Blood Plasma through Cross-Matrix Calibration and Bayesian Hierarchical Modeling","authors":"Nipunika H. Godage, Song S. Qian, Erasmus Cudjoe and Emanuela Gionfriddo*, ","doi":"10.1021/acsmeasuresciau.3c00049","DOIUrl":"10.1021/acsmeasuresciau.3c00049","url":null,"abstract":"<p >This study addresses the challenges of matrix effects and interspecies plasma protein binding (PPB) on measurement variability during method validation across diverse plasma types (human, rat, rabbit, and bovine). Accurate measurements of small molecules in plasma samples often require matrix-matched calibration approaches with the use of specific plasma types, which may have limited availability or affordability. To mitigate the costs associated with human plasma measurements, we explore in this work the potential of cross-matrix-matched calibration using Bayesian hierarchical modeling (BHM) to correct for matrix effects associated with PPB. We initially developed a targeted quantitative approach utilizing biocompatible solid-phase microextraction coupled with liquid chromatography–mass spectrometry for xenobiotic analysis in plasma. The method was evaluated for absolute matrix effects across human, bovine, rat, and rabbit plasma comparing pre- and postmatrix extraction standards. Absolute matrix effects from 96 to 108% for most analytes across plasma sources indicate that the biocompatibility of the extraction phase minimizes interference coextraction. However, the extent of PPB in different media can still affect the accuracy of the measurement when the extraction of small molecules is carried out via free concentration, as in the case of microextraction techniques. In fact, while matrix-matched calibration revealed high accuracy, cross-matrix calibration (e.g., using a calibration curve generated from bovine plasma) proved inadequate for precise measurements in human plasma. A BHM was used to calculate correction factors for each analyte within each plasma type, successfully mitigating the measurement bias resulting from diverse calibration curve types used to quantify human plasma samples. This work contributes to the development of cost-effective, efficient calibration strategies for biofluids. Leveraging easily accessible plasma sources, like bovine plasma, for method optimization and validation prior to analyzing costly plasma (e.g., human plasma) holds substantial advantages applicable to biomonitoring and pharmacokinetic studies.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"127–135"},"PeriodicalIF":0.0,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00049","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138539128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-12-04DOI: 10.1021/acsmeasuresciau.3c00045
Yiming Zhang, Zexi Zhang, Miaomiao Wu and Run Zhang*,
Gamma-glutamyltransferase (GGT) is a plasma-membrane-bound enzyme that is involved in the γ-glutamyl cycle, like metabolism of glutathione (GSH). This enzyme plays an important role in protecting cells from oxidative stress, thus being tested as a key biomarker for several medical conditions, such as liver injury, carcinogenesis, and tumor progression. For measuring GGT activity, a number of bioanalytical methods have emerged, such as chromatography, colorimetric, electrochemical, and luminescence analyses. Among these approaches, probes that can specifically respond to GGT are contributing significantly to measuring its activity in vitro and in vivo. This review thus aims to highlight the recent advances in the development of responsive probes for GGT measurement and their practical applications. Responsive probes for fluorescence analysis, including “off–on”, near-infrared (NIR), two-photon, and ratiometric fluorescence response probes, are initially summarized, followed by discussing the advances in the development of other probes, such as bioluminescence, chemiluminescence, photoacoustic, Raman, magnetic resonance imaging (MRI), and positron emission tomography (PET). The practical applications of the responsive probes in cancer diagnosis and treatment monitoring and GGT inhibitor screening are then highlighted. Based on this information, the advantages, challenges, and prospects of responsive probe technology for GGT measurement are analyzed.
{"title":"Advances and Perspectives of Responsive Probes for Measuring γ-Glutamyl Transpeptidase","authors":"Yiming Zhang, Zexi Zhang, Miaomiao Wu and Run Zhang*, ","doi":"10.1021/acsmeasuresciau.3c00045","DOIUrl":"10.1021/acsmeasuresciau.3c00045","url":null,"abstract":"<p >Gamma-glutamyltransferase (GGT) is a plasma-membrane-bound enzyme that is involved in the γ-glutamyl cycle, like metabolism of glutathione (GSH). This enzyme plays an important role in protecting cells from oxidative stress, thus being tested as a key biomarker for several medical conditions, such as liver injury, carcinogenesis, and tumor progression. For measuring GGT activity, a number of bioanalytical methods have emerged, such as chromatography, colorimetric, electrochemical, and luminescence analyses. Among these approaches, probes that can specifically respond to GGT are contributing significantly to measuring its activity in vitro and in vivo. This review thus aims to highlight the recent advances in the development of responsive probes for GGT measurement and their practical applications. Responsive probes for fluorescence analysis, including “off–on”, near-infrared (NIR), two-photon, and ratiometric fluorescence response probes, are initially summarized, followed by discussing the advances in the development of other probes, such as bioluminescence, chemiluminescence, photoacoustic, Raman, magnetic resonance imaging (MRI), and positron emission tomography (PET). The practical applications of the responsive probes in cancer diagnosis and treatment monitoring and GGT inhibitor screening are then highlighted. Based on this information, the advantages, challenges, and prospects of responsive probe technology for GGT measurement are analyzed.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"54–75"},"PeriodicalIF":0.0,"publicationDate":"2023-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138539139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-30DOI: 10.1021/acsmeasuresciau.3c00065
Abraham K. Badu-Tawiah*,
{"title":"The Growing Influence of Mass Spectrometry in Measurement Science","authors":"Abraham K. Badu-Tawiah*, ","doi":"10.1021/acsmeasuresciau.3c00065","DOIUrl":"10.1021/acsmeasuresciau.3c00065","url":null,"abstract":"","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"3 6","pages":"390–392"},"PeriodicalIF":0.0,"publicationDate":"2023-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00065","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138539150","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-22DOI: 10.1021/acsmeasuresciau.3c00047
Annina Stuber, Anna Cavaccini, Andreea Manole, Anna Burdina, Yassine Massoud, Tommaso Patriarchi, Theofanis Karayannis and Nako Nakatsuka*,
Aptamer-functionalized biosensors exhibit high selectivity for monitoring neurotransmitters in complex environments. We translated nanoscale aptamer-modified nanopipette sensors to detect endogenous dopamine release in vitro and ex vivo. These sensors employ quartz nanopipettes with nanoscale pores (ca. 10 nm diameter) that are functionalized with aptamers that enable the selective capture of dopamine through target-specific conformational changes. The dynamic behavior of aptamer structures upon dopamine binding leads to the rearrangement of surface charge within the nanopore, resulting in measurable changes in ionic current. To assess sensor performance in real time, we designed a fluidic platform to characterize the temporal dynamics of nanopipette sensors. We then conducted differential biosensing by deploying control sensors modified with nonspecific DNA alongside dopamine-specific sensors in biological milieu. Our results confirm the functionality of aptamer-modified nanopipettes for direct measurements in undiluted complex fluids, specifically in the culture media of human-induced pluripotent stem cell-derived dopaminergic neurons. Moreover, sensor implantation and repeated measurements in acute brain slices was possible, likely owing to the protected sensing area inside nanoscale DNA-filled orifices, minimizing exposure to nonspecific interferents and preventing clogging. Further, differential recordings of endogenous dopamine released through electrical stimulation in the dorsolateral striatum demonstrate the potential of aptamer-modified nanopipettes for ex vivo recordings with unprecedented spatial resolution and reduced tissue damage.
{"title":"Interfacing Aptamer-Modified Nanopipettes with Neuronal Media and Ex Vivo Brain Tissue","authors":"Annina Stuber, Anna Cavaccini, Andreea Manole, Anna Burdina, Yassine Massoud, Tommaso Patriarchi, Theofanis Karayannis and Nako Nakatsuka*, ","doi":"10.1021/acsmeasuresciau.3c00047","DOIUrl":"10.1021/acsmeasuresciau.3c00047","url":null,"abstract":"<p >Aptamer-functionalized biosensors exhibit high selectivity for monitoring neurotransmitters in complex environments. We translated nanoscale aptamer-modified nanopipette sensors to detect endogenous dopamine release <i>in vitro</i> and <i>ex vivo</i>. These sensors employ quartz nanopipettes with nanoscale pores (ca. 10 nm diameter) that are functionalized with aptamers that enable the selective capture of dopamine through target-specific conformational changes. The dynamic behavior of aptamer structures upon dopamine binding leads to the rearrangement of surface charge within the nanopore, resulting in measurable changes in ionic current. To assess sensor performance in real time, we designed a fluidic platform to characterize the temporal dynamics of nanopipette sensors. We then conducted differential biosensing by deploying control sensors modified with nonspecific DNA alongside dopamine-specific sensors in biological milieu. Our results confirm the functionality of aptamer-modified nanopipettes for direct measurements in undiluted complex fluids, specifically in the culture media of human-induced pluripotent stem cell-derived dopaminergic neurons. Moreover, sensor implantation and repeated measurements in acute brain slices was possible, likely owing to the protected sensing area inside nanoscale DNA-filled orifices, minimizing exposure to nonspecific interferents and preventing clogging. Further, differential recordings of endogenous dopamine released through electrical stimulation in the dorsolateral striatum demonstrate the potential of aptamer-modified nanopipettes for <i>ex vivo</i> recordings with unprecedented spatial resolution and reduced tissue damage.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"92–103"},"PeriodicalIF":0.0,"publicationDate":"2023-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00047","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138539171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-11-09DOI: 10.1021/acsmeasuresciau.3c00043
Shan-Chu Yu, Tzu-Yen Huang and Tzu-En Lin*,
This research delves into the development and optimization of MXene nanosheet-based paper electrodes, emphasizing their adaptability in green electronics and diverse applications. Xuan paper, a cellulose-based material, was identified as an ideal substrate for its mechanical attributes and capacity to accommodate MXene, further yielding outstanding electrical conductivity. The MXene paper electrode demonstrated consistent performance under various conditions, showing its potential in the field of wearable electronics and medical devices. Notably, its impressive electrothermal capabilities and environmentally conscious decomposition mechanism make it a promising candidate for future green electronic applications. Overall, this study underscores the electrode’s harmonization of performance and environmental sustainability, paving the way for its integration into futuristic electronic solutions.
{"title":"MXene Nanosheets-Decorated Paper as a Green Electronics Material for Biosensing","authors":"Shan-Chu Yu, Tzu-Yen Huang and Tzu-En Lin*, ","doi":"10.1021/acsmeasuresciau.3c00043","DOIUrl":"10.1021/acsmeasuresciau.3c00043","url":null,"abstract":"<p >This research delves into the development and optimization of MXene nanosheet-based paper electrodes, emphasizing their adaptability in green electronics and diverse applications. Xuan paper, a cellulose-based material, was identified as an ideal substrate for its mechanical attributes and capacity to accommodate MXene, further yielding outstanding electrical conductivity. The MXene paper electrode demonstrated consistent performance under various conditions, showing its potential in the field of wearable electronics and medical devices. Notably, its impressive electrothermal capabilities and environmentally conscious decomposition mechanism make it a promising candidate for future green electronic applications. Overall, this study underscores the electrode’s harmonization of performance and environmental sustainability, paving the way for its integration into futuristic electronic solutions.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"81–91"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135241302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Reactions involving sulfhydryl groups play a critical role in maintaining the structure and function of proteins. However, traditional mechanistic studies have mainly focused on reaction rates and the efficiency in bulk solutions. Herein, we have designed a cysteine-mutated nanopore as a biological protein nanoreactor for electrochemical visualization of the thiol substitute reaction. Statistical analysis of characteristic current signals shows that the apparent reaction rate at the single-molecule level in this confined nanoreactor reached 1400 times higher than that observed in bulk solution. This substantial acceleration of thiol substitution reactions within the nanopore offers promising opportunities for advancing the design and optimization of micro/nanoreactors. Moreover, our results could shed light on the understanding of sulfhydryl reactions and the thiol-involved signal transduction mechanisms in biological systems.
{"title":"Electrochemical Visualization of Single-Molecule Thiol Substitution with Nanopore Measurement","authors":"Chao-Nan Yang, Wei Liu, Hao-Tian Liu, Ji-Chang Zhang, Ru-Jia Yu, Yi-Lun Ying* and Yi-Tao Long, ","doi":"10.1021/acsmeasuresciau.3c00046","DOIUrl":"10.1021/acsmeasuresciau.3c00046","url":null,"abstract":"<p >Reactions involving sulfhydryl groups play a critical role in maintaining the structure and function of proteins. However, traditional mechanistic studies have mainly focused on reaction rates and the efficiency in bulk solutions. Herein, we have designed a cysteine-mutated nanopore as a biological protein nanoreactor for electrochemical visualization of the thiol substitute reaction. Statistical analysis of characteristic current signals shows that the apparent reaction rate at the single-molecule level in this confined nanoreactor reached 1400 times higher than that observed in bulk solution. This substantial acceleration of thiol substitution reactions within the nanopore offers promising opportunities for advancing the design and optimization of micro/nanoreactors. Moreover, our results could shed light on the understanding of sulfhydryl reactions and the thiol-involved signal transduction mechanisms in biological systems.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"4 1","pages":"76–80"},"PeriodicalIF":0.0,"publicationDate":"2023-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.3c00046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135292396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}