首页 > 最新文献

ACS Measurement Science Au最新文献

英文 中文
Cross-Species Applications of Peptide Substrate Reporters to Quantitative Measurements of Kinase Activity 多肽底物报告器在激酶活性定量测量中的跨物种应用
Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-08-02 DOI: 10.1021/acsmeasuresciau.4c00030
Mengqi Jonathan Fan, Misha Mehra, Kunwei Yang, Rahuljeet S. Chadha, Sababa Anber, Michelle L. Kovarik
Peptide substrate reporters are short chains of amino acids designed to act as substrates for enzymes of interest. Combined with capillary electrophoresis and laser-induced fluorescence detection (CE-LIF), they are powerful molecular tools for quantitative measurements of enzyme activity even at the level of single cells. Although most peptide substrate reporters have been optimized for human or murine cells in health-related applications, their performance in nonmammalian organisms remains largely unexplored. In this study, we evaluated three peptide substrate reporters for protein kinase B (PKB) in two eukaryotic microbes, Dictyostelium discoideum and Tetrahymena thermophila, which are evolutionarily distant from mammals and from each other yet express PKB homologues. All three peptide substrate reporters were phosphorylated in lysates from both organisms but with varying phosphorylation kinetics and stability. To demonstrate reporter utility, we used one to screen for and identify the previously unknown stimulus needed to activate PHK5, the PKB homologue in T. thermophila. In D. discoideum, we employed the highly quantitative nature of these assays using CE-LIF to make precise measurements of PKB activity in response to transient stimulation, drug treatment, and genetic mutation. These results underscore the broad applicability of peptide substrate reporters across diverse species while highlighting the need for further research to determine effective peptide stabilization strategies across different biological contexts.
多肽底物报告物是由氨基酸组成的短链,可作为相关酶的底物。它们与毛细管电泳和激光诱导荧光检测(CE-LIF)相结合,是即使在单细胞水平上也能定量测量酶活性的强大分子工具。虽然大多数肽底物报告物都已针对人类或鼠类细胞的健康相关应用进行了优化,但它们在非哺乳动物中的性能在很大程度上仍未得到探索。在这项研究中,我们评估了两种真核微生物--盘基竹荪(Dictyostelium discoideum)和嗜热四膜虫(Tetrahymena thermophila)--中蛋白激酶 B(PKB)的三种多肽底物报告物。在这两种生物的裂解液中,所有三种肽底物报告物都发生了磷酸化,但磷酸化动力学和稳定性各不相同。为了证明报告物的效用,我们用其中一种报告物筛选并确定了激活嗜热菌中 PKB 同源物 PHK5 所需的未知刺激。在 Discoideum 中,我们利用 CE-LIF 这些检测方法的高度定量性,精确测量了 PKB 在瞬时刺激、药物治疗和基因突变下的活性。这些结果凸显了多肽底物报告物在不同物种中的广泛适用性,同时也强调了在不同生物环境中确定有效多肽稳定策略的进一步研究的必要性。
{"title":"Cross-Species Applications of Peptide Substrate Reporters to Quantitative Measurements of Kinase Activity","authors":"Mengqi Jonathan Fan, Misha Mehra, Kunwei Yang, Rahuljeet S. Chadha, Sababa Anber, Michelle L. Kovarik","doi":"10.1021/acsmeasuresciau.4c00030","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00030","url":null,"abstract":"Peptide substrate reporters are short chains of amino acids designed to act as substrates for enzymes of interest. Combined with capillary electrophoresis and laser-induced fluorescence detection (CE-LIF), they are powerful molecular tools for quantitative measurements of enzyme activity even at the level of single cells. Although most peptide substrate reporters have been optimized for human or murine cells in health-related applications, their performance in nonmammalian organisms remains largely unexplored. In this study, we evaluated three peptide substrate reporters for protein kinase B (PKB) in two eukaryotic microbes, <i>Dictyostelium discoideum</i> and <i>Tetrahymena thermophila</i>, which are evolutionarily distant from mammals and from each other yet express PKB homologues. All three peptide substrate reporters were phosphorylated in lysates from both organisms but with varying phosphorylation kinetics and stability. To demonstrate reporter utility, we used one to screen for and identify the previously unknown stimulus needed to activate PHK5, the PKB homologue in <i>T. thermophila</i>. In <i>D. discoideum</i>, we employed the highly quantitative nature of these assays using CE-LIF to make precise measurements of PKB activity in response to transient stimulation, drug treatment, and genetic mutation. These results underscore the broad applicability of peptide substrate reporters across diverse species while highlighting the need for further research to determine effective peptide stabilization strategies across different biological contexts.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141881272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cross-Species Applications of Peptide Substrate Reporters to Quantitative Measurements of Kinase Activity 多肽底物报告器在激酶活性定量测量中的跨物种应用
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-08-02 DOI: 10.1021/acsmeasuresciau.4c0003010.1021/acsmeasuresciau.4c00030
Mengqi Jonathan Fan, Misha Mehra, Kunwei Yang, Rahuljeet S. Chadha, Sababa Anber and Michelle L. Kovarik*, 

Peptide substrate reporters are short chains of amino acids designed to act as substrates for enzymes of interest. Combined with capillary electrophoresis and laser-induced fluorescence detection (CE-LIF), they are powerful molecular tools for quantitative measurements of enzyme activity even at the level of single cells. Although most peptide substrate reporters have been optimized for human or murine cells in health-related applications, their performance in nonmammalian organisms remains largely unexplored. In this study, we evaluated three peptide substrate reporters for protein kinase B (PKB) in two eukaryotic microbes, Dictyostelium discoideum and Tetrahymena thermophila, which are evolutionarily distant from mammals and from each other yet express PKB homologues. All three peptide substrate reporters were phosphorylated in lysates from both organisms but with varying phosphorylation kinetics and stability. To demonstrate reporter utility, we used one to screen for and identify the previously unknown stimulus needed to activate PHK5, the PKB homologue in T. thermophila. In D. discoideum, we employed the highly quantitative nature of these assays using CE-LIF to make precise measurements of PKB activity in response to transient stimulation, drug treatment, and genetic mutation. These results underscore the broad applicability of peptide substrate reporters across diverse species while highlighting the need for further research to determine effective peptide stabilization strategies across different biological contexts.

多肽底物报告物是由氨基酸组成的短链,可作为相关酶的底物。它们与毛细管电泳和激光诱导荧光检测(CE-LIF)相结合,是即使在单细胞水平上也能定量测量酶活性的强大分子工具。虽然大多数肽底物报告物都已针对人类或鼠类细胞的健康相关应用进行了优化,但它们在非哺乳动物中的性能在很大程度上仍未得到探索。在这项研究中,我们评估了两种真核微生物--盘基竹荪(Dictyostelium discoideum)和嗜热四膜虫(Tetrahymena thermophila)--中蛋白激酶 B(PKB)的三种多肽底物报告物。在这两种生物的裂解液中,所有三种多肽底物报告物都发生了磷酸化,但磷酸化动力学和稳定性各不相同。为了证明报告物的效用,我们用其中一种报告物筛选并确定了激活嗜热菌中 PKB 同源物 PHK5 所需的未知刺激。在 Discoideum 中,我们利用 CE-LIF 这些检测方法的高度定量性,精确测量了 PKB 在瞬时刺激、药物治疗和基因突变下的活性。这些结果凸显了多肽底物报告物在不同物种中的广泛适用性,同时也强调了在不同生物环境中确定有效多肽稳定策略的进一步研究的必要性。
{"title":"Cross-Species Applications of Peptide Substrate Reporters to Quantitative Measurements of Kinase Activity","authors":"Mengqi Jonathan Fan,&nbsp;Misha Mehra,&nbsp;Kunwei Yang,&nbsp;Rahuljeet S. Chadha,&nbsp;Sababa Anber and Michelle L. Kovarik*,&nbsp;","doi":"10.1021/acsmeasuresciau.4c0003010.1021/acsmeasuresciau.4c00030","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00030https://doi.org/10.1021/acsmeasuresciau.4c00030","url":null,"abstract":"<p >Peptide substrate reporters are short chains of amino acids designed to act as substrates for enzymes of interest. Combined with capillary electrophoresis and laser-induced fluorescence detection (CE-LIF), they are powerful molecular tools for quantitative measurements of enzyme activity even at the level of single cells. Although most peptide substrate reporters have been optimized for human or murine cells in health-related applications, their performance in nonmammalian organisms remains largely unexplored. In this study, we evaluated three peptide substrate reporters for protein kinase B (PKB) in two eukaryotic microbes, <i>Dictyostelium discoideum</i> and <i>Tetrahymena thermophila</i>, which are evolutionarily distant from mammals and from each other yet express PKB homologues. All three peptide substrate reporters were phosphorylated in lysates from both organisms but with varying phosphorylation kinetics and stability. To demonstrate reporter utility, we used one to screen for and identify the previously unknown stimulus needed to activate PHK5, the PKB homologue in <i>T. thermophila</i>. In <i>D. discoideum</i>, we employed the highly quantitative nature of these assays using CE-LIF to make precise measurements of PKB activity in response to transient stimulation, drug treatment, and genetic mutation. These results underscore the broad applicability of peptide substrate reporters across diverse species while highlighting the need for further research to determine effective peptide stabilization strategies across different biological contexts.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.4c00030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436873","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}
引用次数: 0
Waveform Optimization for the In Vitro Detection of Caffeic Acid by Fast-Scan Cyclic Voltammetry 快速扫描循环伏安法体外检测咖啡酸的波形优化
Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-31 DOI: 10.1021/acsmeasuresciau.4c00029
Joseph N. Tonn, Richard B. Keithley
Caffeic acid is a polyphenol of critical importance in plants, involved in a variety of physiological processes including lignin formation, cellular growth, stress response, and external signaling. This small molecule also acts as a powerful antioxidant and thus has therapeutic potential for a variety of health conditions. Traditional methods of detecting caffeic acid lack appropriate temporal resolution to monitor real time concentration changes on a subsecond time scale with nM detection limits. Here we report on the first usage of fast-scan cyclic voltammetry with carbon fiber microelectrodes for the detection of caffeic acid. Through the use of flow injection analysis, the optimal waveform for its detection under acidic conditions at a scan rate of 400 V/s was determined to be sawtooth-shaped, from 0 to 1.4 to −0.4 to 0 V. Signal was linear with concentration up to 1 μM with a sensitivity of 44.8 ± 1.3 nA/μM and a detection limit of 2.3 ± 0.2 nM. The stability of its detection was exceptional, with an average of 0.96% relative standard deviation across 32 consecutive injections. This waveform was also successful in detecting other catechol-based plant antioxidants including 5-chlorogenic acid, oleuropein, rosmarinic acid, chicoric acid, and caffeic acid phenethyl ester. Finally, we show the successful use of fast-scan cyclic voltammetry in monitoring the degradation of caffeic acid by polyphenol oxidase on a subsecond time scale via a novel modification of a Ramsson cell. This work demonstrates that fast-scan cyclic voltammetry can be used to successfully monitor real-time dynamic changes in the concentrations of catechol-containing plant polyphenols.
咖啡酸是一种对植物至关重要的多酚,参与木质素形成、细胞生长、应激反应和外部信号传递等多种生理过程。这种小分子还具有强大的抗氧化作用,因此对多种健康状况具有治疗潜力。传统的咖啡酸检测方法缺乏适当的时间分辨率,无法监测亚秒级的实时浓度变化,检测极限为 nM。在此,我们报告了首次使用碳纤维微电极快速扫描循环伏安法检测咖啡酸的情况。通过使用流动注射分析法,确定了在酸性条件下以 400 V/s 的扫描速率检测咖啡酸的最佳波形为锯齿形,从 0 到 1.4 到 -0.4 到 0 V。其检测稳定性极佳,连续 32 次注射的平均相对标准偏差为 0.96%。该波形还能成功检测其他儿茶酚类植物抗氧化剂,包括 5-氯原酸、油菜素、迷迭香酸、菊苣酸和咖啡酸苯乙酯。最后,我们展示了快速扫描循环伏安法的成功应用,通过对拉姆森电池的新颖改造,在亚秒级时间内监测多酚氧化酶对咖啡酸的降解。这项工作表明,快速扫描循环伏安法可用于成功监测含儿茶酚植物多酚浓度的实时动态变化。
{"title":"Waveform Optimization for the In Vitro Detection of Caffeic Acid by Fast-Scan Cyclic Voltammetry","authors":"Joseph N. Tonn, Richard B. Keithley","doi":"10.1021/acsmeasuresciau.4c00029","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00029","url":null,"abstract":"Caffeic acid is a polyphenol of critical importance in plants, involved in a variety of physiological processes including lignin formation, cellular growth, stress response, and external signaling. This small molecule also acts as a powerful antioxidant and thus has therapeutic potential for a variety of health conditions. Traditional methods of detecting caffeic acid lack appropriate temporal resolution to monitor real time concentration changes on a subsecond time scale with nM detection limits. Here we report on the first usage of fast-scan cyclic voltammetry with carbon fiber microelectrodes for the detection of caffeic acid. Through the use of flow injection analysis, the optimal waveform for its detection under acidic conditions at a scan rate of 400 V/s was determined to be sawtooth-shaped, from 0 to 1.4 to −0.4 to 0 V. Signal was linear with concentration up to 1 μM with a sensitivity of 44.8 ± 1.3 nA/μM and a detection limit of 2.3 ± 0.2 nM. The stability of its detection was exceptional, with an average of 0.96% relative standard deviation across 32 consecutive injections. This waveform was also successful in detecting other catechol-based plant antioxidants including 5-chlorogenic acid, oleuropein, rosmarinic acid, chicoric acid, and caffeic acid phenethyl ester. Finally, we show the successful use of fast-scan cyclic voltammetry in monitoring the degradation of caffeic acid by polyphenol oxidase on a subsecond time scale <i>via</i> a novel modification of a Ramsson cell. This work demonstrates that fast-scan cyclic voltammetry can be used to successfully monitor real-time dynamic changes in the concentrations of catechol-containing plant polyphenols.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141867838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Waveform Optimization for the In Vitro Detection of Caffeic Acid by Fast-Scan Cyclic Voltammetry 快速扫描循环伏安法体外检测咖啡酸的波形优化
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-31 DOI: 10.1021/acsmeasuresciau.4c0002910.1021/acsmeasuresciau.4c00029
Joseph N. Tonn,  and , Richard B. Keithley*, 

Caffeic acid is a polyphenol of critical importance in plants, involved in a variety of physiological processes including lignin formation, cellular growth, stress response, and external signaling. This small molecule also acts as a powerful antioxidant and thus has therapeutic potential for a variety of health conditions. Traditional methods of detecting caffeic acid lack appropriate temporal resolution to monitor real time concentration changes on a subsecond time scale with nM detection limits. Here we report on the first usage of fast-scan cyclic voltammetry with carbon fiber microelectrodes for the detection of caffeic acid. Through the use of flow injection analysis, the optimal waveform for its detection under acidic conditions at a scan rate of 400 V/s was determined to be sawtooth-shaped, from 0 to 1.4 to −0.4 to 0 V. Signal was linear with concentration up to 1 μM with a sensitivity of 44.8 ± 1.3 nA/μM and a detection limit of 2.3 ± 0.2 nM. The stability of its detection was exceptional, with an average of 0.96% relative standard deviation across 32 consecutive injections. This waveform was also successful in detecting other catechol-based plant antioxidants including 5-chlorogenic acid, oleuropein, rosmarinic acid, chicoric acid, and caffeic acid phenethyl ester. Finally, we show the successful use of fast-scan cyclic voltammetry in monitoring the degradation of caffeic acid by polyphenol oxidase on a subsecond time scale via a novel modification of a Ramsson cell. This work demonstrates that fast-scan cyclic voltammetry can be used to successfully monitor real-time dynamic changes in the concentrations of catechol-containing plant polyphenols.

咖啡酸是一种对植物至关重要的多酚,参与木质素形成、细胞生长、应激反应和外部信号传递等多种生理过程。这种小分子也是一种强大的抗氧化剂,因此具有治疗各种健康状况的潜力。传统的咖啡酸检测方法缺乏适当的时间分辨率,无法监测亚秒级的实时浓度变化,检测极限为 nM。在此,我们报告了首次使用碳纤维微电极快速扫描循环伏安法检测咖啡酸的情况。通过使用流动注射分析法,确定了在酸性条件下以 400 V/s 的扫描速率检测咖啡酸的最佳波形为锯齿形,从 0 到 1.4 到 -0.4 到 0 V。其检测稳定性极佳,连续 32 次注射的平均相对标准偏差为 0.96%。该波形还能成功检测其他儿茶酚类植物抗氧化剂,包括 5-氯原酸、油菜素、迷迭香酸、菊苣酸和咖啡酸苯乙酯。最后,我们展示了快速扫描循环伏安法的成功应用,通过对拉姆森电池的新颖改造,在亚秒级时间内监测多酚氧化酶对咖啡酸的降解。这项工作表明,快速扫描循环伏安法可用于成功监测含儿茶酚植物多酚浓度的实时动态变化。
{"title":"Waveform Optimization for the In Vitro Detection of Caffeic Acid by Fast-Scan Cyclic Voltammetry","authors":"Joseph N. Tonn,&nbsp; and ,&nbsp;Richard B. Keithley*,&nbsp;","doi":"10.1021/acsmeasuresciau.4c0002910.1021/acsmeasuresciau.4c00029","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00029https://doi.org/10.1021/acsmeasuresciau.4c00029","url":null,"abstract":"<p >Caffeic acid is a polyphenol of critical importance in plants, involved in a variety of physiological processes including lignin formation, cellular growth, stress response, and external signaling. This small molecule also acts as a powerful antioxidant and thus has therapeutic potential for a variety of health conditions. Traditional methods of detecting caffeic acid lack appropriate temporal resolution to monitor real time concentration changes on a subsecond time scale with nM detection limits. Here we report on the first usage of fast-scan cyclic voltammetry with carbon fiber microelectrodes for the detection of caffeic acid. Through the use of flow injection analysis, the optimal waveform for its detection under acidic conditions at a scan rate of 400 V/s was determined to be sawtooth-shaped, from 0 to 1.4 to −0.4 to 0 V. Signal was linear with concentration up to 1 μM with a sensitivity of 44.8 ± 1.3 nA/μM and a detection limit of 2.3 ± 0.2 nM. The stability of its detection was exceptional, with an average of 0.96% relative standard deviation across 32 consecutive injections. This waveform was also successful in detecting other catechol-based plant antioxidants including 5-chlorogenic acid, oleuropein, rosmarinic acid, chicoric acid, and caffeic acid phenethyl ester. Finally, we show the successful use of fast-scan cyclic voltammetry in monitoring the degradation of caffeic acid by polyphenol oxidase on a subsecond time scale <i>via</i> a novel modification of a Ramsson cell. This work demonstrates that fast-scan cyclic voltammetry can be used to successfully monitor real-time dynamic changes in the concentrations of catechol-containing plant polyphenols.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.4c00029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436615","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}
引用次数: 0
E.Co.Tech Breathalyzer: A Pilot Study of a Non-invasive COVID-19 Diagnostic Tool for Light and Non-smokers E.Co.Tech 呼吸分析仪:针对轻度和非吸烟者的无创 COVID-19 诊断工具试点研究
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-25 DOI: 10.1021/acsmeasuresciau.4c00020
I. Banga, Kordel France, A. Paul, Shalini Prasad
{"title":"E.Co.Tech Breathalyzer: A Pilot Study of a Non-invasive COVID-19 Diagnostic Tool for Light and Non-smokers","authors":"I. Banga, Kordel France, A. Paul, Shalini Prasad","doi":"10.1021/acsmeasuresciau.4c00020","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00020","url":null,"abstract":"","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141803897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
E.Co.Tech Breathalyzer: A Pilot Study of a Non-invasive COVID-19 Diagnostic Tool for Light and Non-smokers E.Co.Tech 呼吸分析仪:针对轻度和非吸烟者的无创 COVID-19 诊断工具试点研究
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-25 DOI: 10.1021/acsmeasuresciau.4c0002010.1021/acsmeasuresciau.4c00020
Ivneet Banga, Kordel France, Anirban Paul and Shalini Prasad*, 

Analysis of exhaled breath offers a noninvasive approach to understanding the metabolic state of the body. This study focuses on the efficacy of an innovative Electrochemical Hand-held Breathalyzer COVID-19 Sensing Technology (E.Co.Tech) for predicting COVID-19 infection, specifically in populations of never or former light smokers. The electrochemical nose technology used in this device aims to discriminate changes in exhaled nitric oxide levels, which are associated with COVID-19-linked respiratory inflammation. The methodology combines the device with a machine learning-based algorithm trained on a diverse data set of breath profiles from both infected and noninfected individuals. A cohort of 46 participants, consisting of never or former light smokers, was recruited. Each participant was tested using the E.Co.Tech prototype device and an iHealth COVID-19 antigen rapid test. The performance of the device was assessed by calculating sensitivity, specificity, positive predictive value, and negative predictive value (NPV). The results demonstrated high specificity (91.11%) and NPV (97.62%) for the device in this demographic group. This case study underscores the potential of E.Co.Tech as a valuable tool for point-of-care COVID-19 diagnosis, particularly in populations with unique smoking histories. The technology’s high sensitivity and specificity, along with its rapid results, make it a promising candidate for deployment in resource-limited settings and situations where timely detection is crucial for effective public health management. Further large-scale clinical trials and real-world validations are necessary to establish the device’s utility across diverse population groups.

呼出气体分析是了解人体新陈代谢状态的一种无创方法。本研究的重点是创新型电化学手持式呼吸分析仪 COVID-19 传感技术(E.Co.Tech)在预测 COVID-19 感染方面的功效,尤其是在从不吸烟或曾经吸烟的人群中。该设备采用的电化学鼻技术旨在分辨呼出一氧化氮水平的变化,而一氧化氮水平的变化与 COVID-19 相关的呼吸道炎症有关。该方法将该设备与基于机器学习的算法相结合,该算法是在来自感染者和非感染者的不同呼吸曲线数据集上训练出来的。研究人员招募了 46 名参与者,其中包括从不吸烟或曾经吸烟的人。每位参与者都使用 E.Co.Tech 原型设备和 iHealth COVID-19 抗原快速检测仪进行了测试。通过计算灵敏度、特异性、阳性预测值和阴性预测值 (NPV) 来评估该设备的性能。结果表明,该设备在这一人群中的特异性(91.11%)和 NPV(97.62%)都很高。该案例研究强调了 E.Co.Tech 作为 COVID-19 床旁诊断的重要工具的潜力,尤其是在有特殊吸烟史的人群中。该技术灵敏度高、特异性强、结果迅速,因此很有希望在资源有限的环境和及时检测对有效公共卫生管理至关重要的情况下应用。有必要进一步开展大规模临床试验和实际验证,以确定该设备在不同人群中的实用性。
{"title":"E.Co.Tech Breathalyzer: A Pilot Study of a Non-invasive COVID-19 Diagnostic Tool for Light and Non-smokers","authors":"Ivneet Banga,&nbsp;Kordel France,&nbsp;Anirban Paul and Shalini Prasad*,&nbsp;","doi":"10.1021/acsmeasuresciau.4c0002010.1021/acsmeasuresciau.4c00020","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00020https://doi.org/10.1021/acsmeasuresciau.4c00020","url":null,"abstract":"<p >Analysis of exhaled breath offers a noninvasive approach to understanding the metabolic state of the body. This study focuses on the efficacy of an innovative Electrochemical Hand-held Breathalyzer COVID-19 Sensing Technology (E.Co.Tech) for predicting COVID-19 infection, specifically in populations of never or former light smokers. The electrochemical nose technology used in this device aims to discriminate changes in exhaled nitric oxide levels, which are associated with COVID-19-linked respiratory inflammation. The methodology combines the device with a machine learning-based algorithm trained on a diverse data set of breath profiles from both infected and noninfected individuals. A cohort of 46 participants, consisting of never or former light smokers, was recruited. Each participant was tested using the E.Co.Tech prototype device and an iHealth COVID-19 antigen rapid test. The performance of the device was assessed by calculating sensitivity, specificity, positive predictive value, and negative predictive value (NPV). The results demonstrated high specificity (91.11%) and NPV (97.62%) for the device in this demographic group. This case study underscores the potential of E.Co.Tech as a valuable tool for point-of-care COVID-19 diagnosis, particularly in populations with unique smoking histories. The technology’s high sensitivity and specificity, along with its rapid results, make it a promising candidate for deployment in resource-limited settings and situations where timely detection is crucial for effective public health management. Further large-scale clinical trials and real-world validations are necessary to establish the device’s utility across diverse population groups.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.4c00020","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436611","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}
引用次数: 0
Scanning Gas Diffusion Electrode Setup for Real-Time Analysis of Catalyst Layers 用于实时分析催化剂层的扫描气体扩散电极装置
Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1021/acsmeasuresciau.4c00018
Ina Reichmann, Vicent Lloret, Konrad Ehelebe, Pascal Lauf, Ken Jenewein, Karl J. J. Mayrhofer, Serhiy Cherevko
The scanning gas diffusion electrode (S-GDE) half-cell is introduced as a new tool to improve the evaluation of electrodes used in electrochemical energy conversion technologies. It allows both fast screening and fundamental studies of real catalyst layers by applying coupled mass spectrometry techniques such as inductively coupled plasma mass spectrometry and online gas mass spectrometry. Hence, the proposed setup overcomes the limitations of aqueous model systems and full cell-level studies, bridging the gap between the two approaches. In this proof-of-concept work, standard fuel cell electrodes are investigated at elevated oxygen reduction reaction current densities, while dissolved Ptx+ ions in the electrolyte and gaseous CO2 in the outlet gas stream are detected to track platinum dissolution and carbon corrosion, respectively. Relevant current densities of up to 0.75 A cm–2 are demonstrated. The electrochemically active surface area, oxygen reduction reaction activity, and Pt dissolution rates are quantified and benchmarked to the values obtained in the conventional stationary GDE half-cell. Moreover, it is found that Pt dissolution is suppressed when O2 is purged into the catalyst layer. Overall, this work demonstrates the feasibility of fast fuel cell electrode screening obtaining, complementary to electrochemical, mass spectrometry data necessary in fundamental studies on structure/performance relationships under actual reaction conditions. While Pt/C, in relevance to its fuel cell application, is used in this study, the proposed setup can be applied in water electrolysis, CO2 conversion, metal-air batteries, and other neighbor technologies.
扫描气体扩散电极(S-GDE)半电池是改进电化学能量转换技术中所用电极评估的一种新工具。它通过应用电感耦合等离子体质谱法和在线气体质谱法等耦合质谱技术,实现了对真实催化剂层的快速筛选和基础研究。因此,拟议的装置克服了水模型系统和完整细胞级研究的局限性,弥补了这两种方法之间的差距。在这项概念验证工作中,研究人员在较高的氧还原反应电流密度下对标准燃料电池电极进行了研究,同时检测了电解液中溶解的铂x+离子和出口气流中的气态二氧化碳,以分别跟踪铂溶解和碳腐蚀情况。相关的电流密度高达 0.75 A cm-2。对电化学活性表面积、氧还原反应活性和铂溶解速率进行了量化,并与传统固定式 GDE 半电池中获得的数值进行了比较。此外,研究还发现,当 O2 进入催化剂层时,铂的溶解会受到抑制。总之,这项工作证明了燃料电池电极快速筛选的可行性,除了电化学数据外,还能获得在实际反应条件下进行结构/性能关系基础研究所需的质谱数据。本研究中使用的 Pt/C 与燃料电池的应用相关,但所建议的设置可用于水电解、二氧化碳转化、金属空气电池和其他邻近技术。
{"title":"Scanning Gas Diffusion Electrode Setup for Real-Time Analysis of Catalyst Layers","authors":"Ina Reichmann, Vicent Lloret, Konrad Ehelebe, Pascal Lauf, Ken Jenewein, Karl J. J. Mayrhofer, Serhiy Cherevko","doi":"10.1021/acsmeasuresciau.4c00018","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00018","url":null,"abstract":"The scanning gas diffusion electrode (S-GDE) half-cell is introduced as a new tool to improve the evaluation of electrodes used in electrochemical energy conversion technologies. It allows both fast screening and fundamental studies of real catalyst layers by applying coupled mass spectrometry techniques such as inductively coupled plasma mass spectrometry and online gas mass spectrometry. Hence, the proposed setup overcomes the limitations of aqueous model systems and full cell-level studies, bridging the gap between the two approaches. In this proof-of-concept work, standard fuel cell electrodes are investigated at elevated oxygen reduction reaction current densities, while dissolved Pt<sup><i>x</i>+</sup> ions in the electrolyte and gaseous CO<sub>2</sub> in the outlet gas stream are detected to track platinum dissolution and carbon corrosion, respectively. Relevant current densities of up to 0.75 A cm<sup>–2</sup> are demonstrated. The electrochemically active surface area, oxygen reduction reaction activity, and Pt dissolution rates are quantified and benchmarked to the values obtained in the conventional stationary GDE half-cell. Moreover, it is found that Pt dissolution is suppressed when O<sub>2</sub> is purged into the catalyst layer. Overall, this work demonstrates the feasibility of fast fuel cell electrode screening obtaining, complementary to electrochemical, mass spectrometry data necessary in fundamental studies on structure/performance relationships under actual reaction conditions. While Pt/C, in relevance to its fuel cell application, is used in this study, the proposed setup can be applied in water electrolysis, CO<sub>2</sub> conversion, metal-air batteries, and other neighbor technologies.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141610731","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Scanning Gas Diffusion Electrode Setup for Real-Time Analysis of Catalyst Layers 用于实时分析催化剂层的扫描气体扩散电极装置
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1021/acsmeasuresciau.4c0001810.1021/acsmeasuresciau.4c00018
Ina Reichmann*, Vicent Lloret, Konrad Ehelebe, Pascal Lauf, Ken Jenewein, Karl J. J. Mayrhofer and Serhiy Cherevko*, 

The scanning gas diffusion electrode (S-GDE) half-cell is introduced as a new tool to improve the evaluation of electrodes used in electrochemical energy conversion technologies. It allows both fast screening and fundamental studies of real catalyst layers by applying coupled mass spectrometry techniques such as inductively coupled plasma mass spectrometry and online gas mass spectrometry. Hence, the proposed setup overcomes the limitations of aqueous model systems and full cell-level studies, bridging the gap between the two approaches. In this proof-of-concept work, standard fuel cell electrodes are investigated at elevated oxygen reduction reaction current densities, while dissolved Ptx+ ions in the electrolyte and gaseous CO2 in the outlet gas stream are detected to track platinum dissolution and carbon corrosion, respectively. Relevant current densities of up to 0.75 A cm–2 are demonstrated. The electrochemically active surface area, oxygen reduction reaction activity, and Pt dissolution rates are quantified and benchmarked to the values obtained in the conventional stationary GDE half-cell. Moreover, it is found that Pt dissolution is suppressed when O2 is purged into the catalyst layer. Overall, this work demonstrates the feasibility of fast fuel cell electrode screening obtaining, complementary to electrochemical, mass spectrometry data necessary in fundamental studies on structure/performance relationships under actual reaction conditions. While Pt/C, in relevance to its fuel cell application, is used in this study, the proposed setup can be applied in water electrolysis, CO2 conversion, metal-air batteries, and other neighbor technologies.

扫描气体扩散电极(S-GDE)半电池是改进电化学能量转换技术中所用电极评估的一种新工具。它通过应用电感耦合等离子体质谱法和在线气体质谱法等耦合质谱技术,实现了对真实催化剂层的快速筛选和基础研究。因此,拟议的装置克服了水模型系统和完整细胞级研究的局限性,弥补了这两种方法之间的差距。在这项概念验证工作中,研究人员在较高的氧还原反应电流密度下对标准燃料电池电极进行了研究,同时检测了电解液中溶解的铂x+离子和出口气流中的气态二氧化碳,以分别跟踪铂溶解和碳腐蚀情况。相关的电流密度高达 0.75 A cm-2。对电化学活性表面积、氧还原反应活性和铂溶解速率进行了量化,并与传统固定式 GDE 半电池中获得的数值进行了比较。此外,研究还发现,当 O2 进入催化剂层时,铂的溶解会受到抑制。总之,这项工作证明了燃料电池电极快速筛选的可行性,除了电化学数据外,还能获得在实际反应条件下进行结构/性能关系基础研究所需的质谱数据。本研究中使用的 Pt/C 与燃料电池的应用相关,但所建议的设置可用于水电解、二氧化碳转化、金属空气电池和其他邻近技术。
{"title":"Scanning Gas Diffusion Electrode Setup for Real-Time Analysis of Catalyst Layers","authors":"Ina Reichmann*,&nbsp;Vicent Lloret,&nbsp;Konrad Ehelebe,&nbsp;Pascal Lauf,&nbsp;Ken Jenewein,&nbsp;Karl J. J. Mayrhofer and Serhiy Cherevko*,&nbsp;","doi":"10.1021/acsmeasuresciau.4c0001810.1021/acsmeasuresciau.4c00018","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00018https://doi.org/10.1021/acsmeasuresciau.4c00018","url":null,"abstract":"<p >The scanning gas diffusion electrode (S-GDE) half-cell is introduced as a new tool to improve the evaluation of electrodes used in electrochemical energy conversion technologies. It allows both fast screening and fundamental studies of real catalyst layers by applying coupled mass spectrometry techniques such as inductively coupled plasma mass spectrometry and online gas mass spectrometry. Hence, the proposed setup overcomes the limitations of aqueous model systems and full cell-level studies, bridging the gap between the two approaches. In this proof-of-concept work, standard fuel cell electrodes are investigated at elevated oxygen reduction reaction current densities, while dissolved Pt<sup><i>x</i>+</sup> ions in the electrolyte and gaseous CO<sub>2</sub> in the outlet gas stream are detected to track platinum dissolution and carbon corrosion, respectively. Relevant current densities of up to 0.75 A cm<sup>–2</sup> are demonstrated. The electrochemically active surface area, oxygen reduction reaction activity, and Pt dissolution rates are quantified and benchmarked to the values obtained in the conventional stationary GDE half-cell. Moreover, it is found that Pt dissolution is suppressed when O<sub>2</sub> is purged into the catalyst layer. Overall, this work demonstrates the feasibility of fast fuel cell electrode screening obtaining, complementary to electrochemical, mass spectrometry data necessary in fundamental studies on structure/performance relationships under actual reaction conditions. While Pt/C, in relevance to its fuel cell application, is used in this study, the proposed setup can be applied in water electrolysis, CO<sub>2</sub> conversion, metal-air batteries, and other neighbor technologies.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.4c00018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436722","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}
引用次数: 0
Impedimetric Measurement of Exchange Currents and Ionic Diffusion Coefficients in Individual Pseudocapacitive Nanoparticles 单个伪电容纳米粒子中交换电流和离子扩散系数的浸渍测量法
Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-11 DOI: 10.1021/acsmeasuresciau.4c00017
Brian Roehrich, Lior Sepunaru
Among electroanalytical techniques, electrochemical impedance spectroscopy (EIS) offers the unique advantage of a high degree of frequency resolution. This enables EIS to readily deconvolute between the capacitive, resistive, and diffusional processes that underlie electrochemical devices. Here, we report the measurement of impedance spectra of individual, pseudocapacitive nanoparticles. We chose Prussian blue as our model system, as it couples an electron-transfer reaction with sodium ion intercalation─processes which, while intrinsically convoluted, can be readily resolved using EIS. We used a scanning electrochemical cell microscope (SECCM) to isolate single Prussian blue particles in a microdroplet and measured their impedance spectra using the multi-sine, fast Fourier transform technique. In doing so, we were able to extract the exchange current density and sodium ion diffusivity for each particle, which respectively inform on their electronic and ionic conductivities. Surprisingly, these parameters vary by over an order of magnitude between particles and are not correlated to particle size nor to each other. The implication of this apparent heterogeneity is that in a hypothetical battery cathode, one active particle may transfer electrons 10 times faster than its neighbor; another may suffer from sluggish sodium ion transport and have restricted charging rate capabilities compared to a better-performing particle elsewhere in the same electrode. Our results inform on this intrinsic heterogeneity while demonstrating the utility of EIS in future single-particle studies.
在电分析技术中,电化学阻抗光谱(EIS)具有频率分辨率高的独特优势。这使得电化学阻抗能谱仪能够轻松地分解电化学装置的电容、电阻和扩散过程。在此,我们报告了对单个伪电容纳米粒子阻抗谱的测量结果。我们选择普鲁士蓝作为我们的模型系统,因为它将电子转移反应与钠离子插层--过程耦合在一起,虽然本质上是复杂的,但使用 EIS 可以很容易地解决。我们使用扫描电化学电池显微镜(SECCM)分离微滴中的单个普鲁士蓝颗粒,并使用多正弦快速傅立叶变换技术测量它们的阻抗谱。在此过程中,我们提取了每个粒子的交换电流密度和钠离子扩散率,它们分别说明了粒子的电子导电性和离子导电性。令人惊讶的是,这些参数在不同颗粒之间的差异超过一个数量级,而且与颗粒大小或相互之间没有关联。这种明显的异质性意味着,在一个假想的电池阴极中,一个活性粒子的电子传输速度可能比其相邻粒子快 10 倍;而另一个活性粒子则可能因钠离子传输迟缓而受到影响,与同一电极中其他地方性能更好的粒子相比,其充电速率能力受到限制。我们的研究结果揭示了这种内在异质性,同时证明了 EIS 在未来单颗粒研究中的实用性。
{"title":"Impedimetric Measurement of Exchange Currents and Ionic Diffusion Coefficients in Individual Pseudocapacitive Nanoparticles","authors":"Brian Roehrich, Lior Sepunaru","doi":"10.1021/acsmeasuresciau.4c00017","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00017","url":null,"abstract":"Among electroanalytical techniques, electrochemical impedance spectroscopy (EIS) offers the unique advantage of a high degree of frequency resolution. This enables EIS to readily deconvolute between the capacitive, resistive, and diffusional processes that underlie electrochemical devices. Here, we report the measurement of impedance spectra of individual, pseudocapacitive nanoparticles. We chose Prussian blue as our model system, as it couples an electron-transfer reaction with sodium ion intercalation─processes which, while intrinsically convoluted, can be readily resolved using EIS. We used a scanning electrochemical cell microscope (SECCM) to isolate single Prussian blue particles in a microdroplet and measured their impedance spectra using the multi-sine, fast Fourier transform technique. In doing so, we were able to extract the exchange current density and sodium ion diffusivity for each particle, which respectively inform on their electronic and ionic conductivities. Surprisingly, these parameters vary by over an order of magnitude between particles and are not correlated to particle size nor to each other. The implication of this apparent heterogeneity is that in a hypothetical battery cathode, one active particle may transfer electrons 10 times faster than its neighbor; another may suffer from sluggish sodium ion transport and have restricted charging rate capabilities compared to a better-performing particle elsewhere in the same electrode. Our results inform on this intrinsic heterogeneity while demonstrating the utility of EIS in future single-particle studies.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141614678","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Impedimetric Measurement of Exchange Currents and Ionic Diffusion Coefficients in Individual Pseudocapacitive Nanoparticles 单个伪电容纳米粒子中交换电流和离子扩散系数的浸渍测量法
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-11 DOI: 10.1021/acsmeasuresciau.4c0001710.1021/acsmeasuresciau.4c00017
Brian Roehrich,  and , Lior Sepunaru*, 

Among electroanalytical techniques, electrochemical impedance spectroscopy (EIS) offers the unique advantage of a high degree of frequency resolution. This enables EIS to readily deconvolute between the capacitive, resistive, and diffusional processes that underlie electrochemical devices. Here, we report the measurement of impedance spectra of individual, pseudocapacitive nanoparticles. We chose Prussian blue as our model system, as it couples an electron-transfer reaction with sodium ion intercalation─processes which, while intrinsically convoluted, can be readily resolved using EIS. We used a scanning electrochemical cell microscope (SECCM) to isolate single Prussian blue particles in a microdroplet and measured their impedance spectra using the multi-sine, fast Fourier transform technique. In doing so, we were able to extract the exchange current density and sodium ion diffusivity for each particle, which respectively inform on their electronic and ionic conductivities. Surprisingly, these parameters vary by over an order of magnitude between particles and are not correlated to particle size nor to each other. The implication of this apparent heterogeneity is that in a hypothetical battery cathode, one active particle may transfer electrons 10 times faster than its neighbor; another may suffer from sluggish sodium ion transport and have restricted charging rate capabilities compared to a better-performing particle elsewhere in the same electrode. Our results inform on this intrinsic heterogeneity while demonstrating the utility of EIS in future single-particle studies.

在电分析技术中,电化学阻抗光谱(EIS)具有频率分辨率高的独特优势。这使得电化学阻抗能谱仪能够轻松地分解电化学装置的电容、电阻和扩散过程。在此,我们报告了对单个伪电容纳米粒子阻抗谱的测量结果。我们选择普鲁士蓝作为我们的模型系统,因为它将电子转移反应与钠离子插层--过程耦合在一起,虽然本质上是复杂的,但使用 EIS 可以很容易地解决。我们使用扫描电化学电池显微镜(SECCM)分离微滴中的单个普鲁士蓝颗粒,并使用多正弦快速傅立叶变换技术测量它们的阻抗谱。在此过程中,我们提取了每个粒子的交换电流密度和钠离子扩散率,它们分别说明了粒子的电子导电性和离子导电性。令人惊讶的是,这些参数在不同颗粒之间的差异超过一个数量级,而且与颗粒大小或相互之间没有关联。这种明显的异质性意味着,在一个假想的电池阴极中,一个活性粒子的电子传输速度可能比其相邻粒子快 10 倍;而另一个活性粒子则可能因钠离子传输迟缓而受到影响,与同一电极中其他地方性能更好的粒子相比,其充电速率能力受到限制。我们的研究结果揭示了这种内在异质性,同时证明了 EIS 在未来单颗粒研究中的实用性。
{"title":"Impedimetric Measurement of Exchange Currents and Ionic Diffusion Coefficients in Individual Pseudocapacitive Nanoparticles","authors":"Brian Roehrich,&nbsp; and ,&nbsp;Lior Sepunaru*,&nbsp;","doi":"10.1021/acsmeasuresciau.4c0001710.1021/acsmeasuresciau.4c00017","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00017https://doi.org/10.1021/acsmeasuresciau.4c00017","url":null,"abstract":"<p >Among electroanalytical techniques, electrochemical impedance spectroscopy (EIS) offers the unique advantage of a high degree of frequency resolution. This enables EIS to readily deconvolute between the capacitive, resistive, and diffusional processes that underlie electrochemical devices. Here, we report the measurement of impedance spectra of individual, pseudocapacitive nanoparticles. We chose Prussian blue as our model system, as it couples an electron-transfer reaction with sodium ion intercalation─processes which, while intrinsically convoluted, can be readily resolved using EIS. We used a scanning electrochemical cell microscope (SECCM) to isolate single Prussian blue particles in a microdroplet and measured their impedance spectra using the multi-sine, fast Fourier transform technique. In doing so, we were able to extract the exchange current density and sodium ion diffusivity for each particle, which respectively inform on their electronic and ionic conductivities. Surprisingly, these parameters vary by over an order of magnitude between particles and are not correlated to particle size nor to each other. The implication of this apparent heterogeneity is that in a hypothetical battery cathode, one active particle may transfer electrons 10 times faster than its neighbor; another may suffer from sluggish sodium ion transport and have restricted charging rate capabilities compared to a better-performing particle elsewhere in the same electrode. Our results inform on this intrinsic heterogeneity while demonstrating the utility of EIS in future single-particle studies.</p>","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmeasuresciau.4c00017","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142010399","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}
引用次数: 0
期刊
ACS Measurement Science Au
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1