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Rapid and Robust Workflows Using Different Ionization, Computation, and Visualization Approaches for Spatial Metabolome Profiling of Microbial Natural Products in Pseudoalteromonas 利用不同的电离、计算和可视化方法对假互交单胞菌微生物天然产物的空间代谢组分析进行快速和稳健的工作流程
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-21 DOI: 10.1021/acsmeasuresciau.4c0003510.1021/acsmeasuresciau.4c00035
Jian Yu, Haidy Metwally, Jennifer Kolwich, Hailey Tomm, Martin Kaufmann, Rachel Klotz, Chang Liu, J. C. Yves Le Blanc, Thomas R. Covey, John Rudan, Avena C. Ross and Richard D. Oleschuk*, 

Ambient mass spectrometry (MS) technologies have been applied to spatial metabolomic profiling of various samples in an attempt to both increase analysis speed and reduce the length of sample preparation. Recent studies, however, have focused on improving the spatial resolution of ambient approaches. Finer resolution requires greater analysis times and commensurate computing power for more sophisticated data analysis algorithms and larger data sets. Higher resolution provides a more detailed molecular picture of the sample; however, for some applications, this is not required. A liquid microjunction surface sampling probe (LMJ-SSP) based MS platform combined with unsupervised multivariant analysis based hyperspectral visualization is demonstrated for the metabolomic analysis of marine bacteria from the genus Pseudoalteromonas to create a rapid and robust spatial profiling workflow for microbial natural product screening. In our study, metabolomic profiles of different Pseudoalteromonas species are quickly acquired without any sample preparation and distinguished by unsupervised multivariant analysis. Our robust platform is capable of automated direct sampling of microbes cultured on agar without clogging. Hyperspectral visualization-based rapid spatial profiling provides adequate spatial metabolite information on microbial samples through red–green–blue (RGB) color annotation. Both static and temporal metabolome differences can be visualized by straightforward color differences and differentiating m/z values identified afterward. Through this approach, novel analogues and their potential biosynthetic pathways are discovered by applying results from the spatial navigation to chromatography-based metabolome annotation. In this current research, LMJ-SSP is shown to be a robust and rapid spatial profiling method. Unsupervised multivariant analysis based hyperspectral visualization is proven straightforward for facile/rapid data interpretation. The combination of direct analysis and innovative data visualization forms a powerful tool to aid the identification/interpretation of interesting compounds from conventional metabolomics analysis.

环境质谱(MS)技术已被应用于各种样品的空间代谢组学分析,以提高分析速度并缩短样品制备时间。然而,最近的研究集中在提高环境方法的空间分辨率上。对于更复杂的数据分析算法和更大的数据集,更精细的分辨率需要更长的分析时间和相应的计算能力。更高的分辨率提供了样品更详细的分子图像;但是,对于某些应用程序,这不是必需的。基于液体微结表面采样探针(LMJ-SSP)的MS平台结合基于无监督多变量分析的高光谱可视化,用于假互单胞菌属海洋细菌的代谢组学分析,为微生物天然产物筛选创建快速而稳健的空间分析工作流程。在我们的研究中,不需要任何样品制备,就可以快速获得不同假互变单胞菌种类的代谢组学特征,并通过无监督的多变量分析进行区分。我们强大的平台能够在没有堵塞的情况下对琼脂上培养的微生物进行自动直接采样。基于高光谱可视化的快速空间分析通过红-绿-蓝(RGB)颜色注释提供了足够的微生物样品空间代谢物信息。静态和时间代谢组差异都可以通过直接的颜色差异和随后确定的区分m/z值来可视化。通过这种方法,通过将空间导航结果应用于基于色谱的代谢组注释,可以发现新的类似物及其潜在的生物合成途径。在本研究中,LMJ-SSP被证明是一种鲁棒且快速的空间剖面方法。基于无监督多变量分析的高光谱可视化被证明是简单/快速的数据解释。直接分析和创新数据可视化的结合形成了一个强大的工具,可以帮助识别/解释传统代谢组学分析中有趣的化合物。
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引用次数: 0
Plasmon Enhanced IR Spectroelectrochemistry. 等离子体增强红外光谱电化学。
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-21 eCollection Date: 2024-12-18 DOI: 10.1021/acsmeasuresciau.4c00048
Jian Li, Jin Li, Xing-Hua Xia

Plasmon-enhanced infrared (IR) techniques have garnered significant interest for their ability to achieve greatly more sensitive IR detection than conventional surface enhanced IR techniques. However, the difficulty in electrically connecting antennas has limited their application in IR spectroelectrochemistry, a crucial field for catalysis, analysis, and energy storage. Recent technical advancements have enabled the successful application of electrochemical potentials to antennas, making plasmon-enhanced IR spectroelectrochemistry feasible. This perspective aims to summarize the latest strategies and offer insights into future improvements for better design of plasmon enhanced IR spectroelectrochemistry platforms and understanding of IR spectroelectrochemistry.

等离子体增强红外(IR)技术已经获得了显著的兴趣,因为它们能够实现比传统表面增强红外技术更敏感的红外探测。然而,电连接天线的困难限制了它们在红外光谱电化学中的应用,而红外光谱电化学是催化、分析和能量存储的关键领域。最近的技术进步使电化学电位成功应用于天线,使等离子体增强红外光谱电化学成为可能。这一观点旨在总结最新的策略,并为更好地设计等离子体增强红外光谱电化学平台和理解红外光谱电化学提供未来改进的见解。
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引用次数: 0
Rapid and Robust Workflows Using Different Ionization, Computation, and Visualization Approaches for Spatial Metabolome Profiling of Microbial Natural Products in Pseudoalteromonas. 利用不同的电离、计算和可视化方法对假互交单胞菌微生物天然产物的空间代谢组分析进行快速和稳健的工作流程。
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-21 eCollection Date: 2024-12-18 DOI: 10.1021/acsmeasuresciau.4c00035
Jian Yu, Haidy Metwally, Jennifer Kolwich, Hailey Tomm, Martin Kaufmann, Rachel Klotz, Chang Liu, J C Yves Le Blanc, Thomas R Covey, John Rudan, Avena C Ross, Richard D Oleschuk

Ambient mass spectrometry (MS) technologies have been applied to spatial metabolomic profiling of various samples in an attempt to both increase analysis speed and reduce the length of sample preparation. Recent studies, however, have focused on improving the spatial resolution of ambient approaches. Finer resolution requires greater analysis times and commensurate computing power for more sophisticated data analysis algorithms and larger data sets. Higher resolution provides a more detailed molecular picture of the sample; however, for some applications, this is not required. A liquid microjunction surface sampling probe (LMJ-SSP) based MS platform combined with unsupervised multivariant analysis based hyperspectral visualization is demonstrated for the metabolomic analysis of marine bacteria from the genus Pseudoalteromonas to create a rapid and robust spatial profiling workflow for microbial natural product screening. In our study, metabolomic profiles of different Pseudoalteromonas species are quickly acquired without any sample preparation and distinguished by unsupervised multivariant analysis. Our robust platform is capable of automated direct sampling of microbes cultured on agar without clogging. Hyperspectral visualization-based rapid spatial profiling provides adequate spatial metabolite information on microbial samples through red-green-blue (RGB) color annotation. Both static and temporal metabolome differences can be visualized by straightforward color differences and differentiating m/z values identified afterward. Through this approach, novel analogues and their potential biosynthetic pathways are discovered by applying results from the spatial navigation to chromatography-based metabolome annotation. In this current research, LMJ-SSP is shown to be a robust and rapid spatial profiling method. Unsupervised multivariant analysis based hyperspectral visualization is proven straightforward for facile/rapid data interpretation. The combination of direct analysis and innovative data visualization forms a powerful tool to aid the identification/interpretation of interesting compounds from conventional metabolomics analysis.

环境质谱(MS)技术已被应用于各种样品的空间代谢组学分析,以提高分析速度并缩短样品制备时间。然而,最近的研究集中在提高环境方法的空间分辨率上。对于更复杂的数据分析算法和更大的数据集,更精细的分辨率需要更长的分析时间和相应的计算能力。更高的分辨率提供了样品更详细的分子图像;但是,对于某些应用程序,这不是必需的。基于液体微结表面采样探针(LMJ-SSP)的MS平台结合基于无监督多变量分析的高光谱可视化,用于假互单胞菌属海洋细菌的代谢组学分析,为微生物天然产物筛选创建快速而稳健的空间分析工作流程。在我们的研究中,不需要任何样品制备,就可以快速获得不同假互变单胞菌种类的代谢组学特征,并通过无监督的多变量分析进行区分。我们强大的平台能够在没有堵塞的情况下对琼脂上培养的微生物进行自动直接采样。基于高光谱可视化的快速空间分析通过红-绿-蓝(RGB)颜色注释提供了足够的微生物样品空间代谢物信息。静态和时间代谢组差异都可以通过直接的颜色差异和随后确定的区分m/z值来可视化。通过这种方法,通过将空间导航结果应用于基于色谱的代谢组注释,可以发现新的类似物及其潜在的生物合成途径。在本研究中,LMJ-SSP被证明是一种鲁棒且快速的空间剖面方法。基于无监督多变量分析的高光谱可视化被证明是简单/快速的数据解释。直接分析和创新数据可视化的结合形成了一个强大的工具,可以帮助识别/解释传统代谢组学分析中有趣的化合物。
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引用次数: 0
Plasmon Enhanced IR Spectroelectrochemistry 等离子体增强型红外光谱电化学
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-21 DOI: 10.1021/acsmeasuresciau.4c0004810.1021/acsmeasuresciau.4c00048
Jian Li*, Jin Li and Xing-Hua Xia*, 

Plasmon-enhanced infrared (IR) techniques have garnered significant interest for their ability to achieve greatly more sensitive IR detection than conventional surface enhanced IR techniques. However, the difficulty in electrically connecting antennas has limited their application in IR spectroelectrochemistry, a crucial field for catalysis, analysis, and energy storage. Recent technical advancements have enabled the successful application of electrochemical potentials to antennas, making plasmon-enhanced IR spectroelectrochemistry feasible. This perspective aims to summarize the latest strategies and offer insights into future improvements for better design of plasmon enhanced IR spectroelectrochemistry platforms and understanding of IR spectroelectrochemistry.

等离子体增强红外(IR)技术已经获得了显著的兴趣,因为它们能够实现比传统表面增强红外技术更敏感的红外探测。然而,电连接天线的困难限制了它们在红外光谱电化学中的应用,而红外光谱电化学是催化、分析和能量存储的关键领域。最近的技术进步使电化学电位成功应用于天线,使等离子体增强红外光谱电化学成为可能。这一观点旨在总结最新的策略,并为更好地设计等离子体增强红外光谱电化学平台和理解红外光谱电化学提供未来改进的见解。
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引用次数: 0
Closing the Knowledge Gap of Post-Acquisition Sample Normalization in Untargeted Metabolomics. 缩小非靶向代谢组学中采集后样本归一化的知识差距。
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-14 eCollection Date: 2024-12-18 DOI: 10.1021/acsmeasuresciau.4c00047
Brian Low, Yukai Wang, Tingting Zhao, Huaxu Yu, Tao Huan

Sample normalization is a crucial step in metabolomics for fair quantitative comparisons. It aims to minimize sample-to-sample variations due to differences in the total metabolite amount. When samples lack a specific metabolic quantity to accurately represent their total metabolite amounts, post-acquisition sample normalization becomes essential. Despite many proposed normalization algorithms, understanding remains limited of their differences, hindering the selection of the most suitable one for a given metabolomics study. This study bridges this knowledge gap by employing data simulation, experimental simulation, and real experiments to elucidate the differences in the mechanism and performance among common post-acquisition sample normalization methods. Using public datasets, we first demonstrated the dramatic discrepancies between the outcomes of different sample normalization methods. Then, we benchmarked six normalization methods: sum, median, probabilistic quotient normalization (PQN), maximal density fold change (MDFC), quantile, and class-specific quantile. Our results show that most normalization methods are biased when there is unbalanced data, a phenomenon where the percentages of up- and downregulated metabolites are unequal. Notably, unbalanced data can be sourced from the underlying biological differences, experimental perturbations, and metabolic interference. Beyond normalization algorithms and data structure, our study also emphasizes the importance of considering additional factors contributed by data quality, such as background noise, signal saturation, and missingness. Based on these findings, we propose an evidence-based normalization strategy to maximize sample normalization outcomes, providing a robust bioinformatic solution for advancing metabolomics research with a fair quantitative comparison.

样本归一化是代谢组学中公平定量比较的关键步骤。它的目的是尽量减少样品之间的差异,由于总代谢物量的差异。当样品缺乏特定的代谢量来准确地表示其总代谢物量时,采集后的样品规范化就变得至关重要。尽管提出了许多归一化算法,但对它们之间差异的理解仍然有限,这阻碍了为给定代谢组学研究选择最合适的算法。本研究通过数据模拟、实验模拟和实际实验来弥补这一知识差距,阐明了常见的采集后样本归一化方法在机制和性能上的差异。使用公共数据集,我们首先证明了不同样本归一化方法的结果之间的巨大差异。然后,我们对六种归一化方法进行了基准测试:和、中位数、概率商归一化(PQN)、最大密度折叠变化(MDFC)、分位数和类别特定分位数。我们的结果表明,当存在不平衡数据时,大多数归一化方法是有偏差的,这是一种向上和向下调节代谢物的百分比不相等的现象。值得注意的是,不平衡数据可能来自潜在的生物学差异、实验扰动和代谢干扰。除了归一化算法和数据结构之外,我们的研究还强调了考虑数据质量带来的其他因素的重要性,例如背景噪声、信号饱和度和缺失。基于这些发现,我们提出了一种基于证据的归一化策略,以最大化样本归一化结果,为推进代谢组学研究提供了一个强大的生物信息学解决方案,并进行了公平的定量比较。
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引用次数: 0
Closing the Knowledge Gap of Post-Acquisition Sample Normalization in Untargeted Metabolomics 缩小非靶向代谢组学中采集后样本归一化的知识差距
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-13 DOI: 10.1021/acsmeasuresciau.4c0004710.1021/acsmeasuresciau.4c00047
Brian Low, Yukai Wang, Tingting Zhao, Huaxu Yu and Tao Huan*, 

Sample normalization is a crucial step in metabolomics for fair quantitative comparisons. It aims to minimize sample-to-sample variations due to differences in the total metabolite amount. When samples lack a specific metabolic quantity to accurately represent their total metabolite amounts, post-acquisition sample normalization becomes essential. Despite many proposed normalization algorithms, understanding remains limited of their differences, hindering the selection of the most suitable one for a given metabolomics study. This study bridges this knowledge gap by employing data simulation, experimental simulation, and real experiments to elucidate the differences in the mechanism and performance among common post-acquisition sample normalization methods. Using public datasets, we first demonstrated the dramatic discrepancies between the outcomes of different sample normalization methods. Then, we benchmarked six normalization methods: sum, median, probabilistic quotient normalization (PQN), maximal density fold change (MDFC), quantile, and class-specific quantile. Our results show that most normalization methods are biased when there is unbalanced data, a phenomenon where the percentages of up- and downregulated metabolites are unequal. Notably, unbalanced data can be sourced from the underlying biological differences, experimental perturbations, and metabolic interference. Beyond normalization algorithms and data structure, our study also emphasizes the importance of considering additional factors contributed by data quality, such as background noise, signal saturation, and missingness. Based on these findings, we propose an evidence-based normalization strategy to maximize sample normalization outcomes, providing a robust bioinformatic solution for advancing metabolomics research with a fair quantitative comparison.

样本归一化是代谢组学中公平定量比较的关键步骤。它的目的是尽量减少样品之间的差异,由于总代谢物量的差异。当样品缺乏特定的代谢量来准确地表示其总代谢物量时,采集后的样品规范化就变得至关重要。尽管提出了许多归一化算法,但对它们之间差异的理解仍然有限,这阻碍了为给定代谢组学研究选择最合适的算法。本研究通过数据模拟、实验模拟和实际实验来弥补这一知识差距,阐明了常见的采集后样本归一化方法在机制和性能上的差异。使用公共数据集,我们首先证明了不同样本归一化方法的结果之间的巨大差异。然后,我们对六种归一化方法进行了基准测试:和、中位数、概率商归一化(PQN)、最大密度折叠变化(MDFC)、分位数和类别特定分位数。我们的结果表明,当存在不平衡数据时,大多数归一化方法是有偏差的,这是一种向上和向下调节代谢物的百分比不相等的现象。值得注意的是,不平衡数据可能来自潜在的生物学差异、实验扰动和代谢干扰。除了归一化算法和数据结构之外,我们的研究还强调了考虑数据质量带来的其他因素的重要性,例如背景噪声、信号饱和度和缺失。基于这些发现,我们提出了一种基于证据的归一化策略,以最大化样本归一化结果,为推进代谢组学研究提供了一个强大的生物信息学解决方案,并进行了公平的定量比较。
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引用次数: 0
From Insulin Measurement to Partial Exocytosis Model: Advances in Single Pancreatic Beta Cell Amperometry over Four Decades. 从胰岛素测量到部分胞吐模型:四十年来单个胰腺β细胞电流测量的进展。
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-10 eCollection Date: 2024-12-18 DOI: 10.1021/acsmeasuresciau.4c00058
Amir Hatamie, Xiulan He, Andrew Ewing, Patrik Rorsman

Single cell Amperometry (SCA) is a powerful, sensitive, high temporal resolution electrochemical technique used to quantify secreted molecular messengers from individual cells and vesicles. This technique has been extensively applied to study the process of exocytosis, and it has also been applied, albeit less frequently, to investigate insulin exocytosis from single pancreatic beta cells. Insufficient insulin release can lead to diabetes, a chronic lifestyle disorder that affects millions of people worldwide. This review aims to summarize and highlight electrochemical measurements of insulin via monitoring its secretion from beta cells by SCA with micro- and nanoelectrodes since the 1990s and to explain how and why serotonin is used as a proxy for monitoring insulin during exocytosis from single beta cells. Finally, we describe how the combination of SCA measurements with the intracellular vesicle impact electrochemical cytometry (IVIEC) technique has led to important findings regarding fractional release types in beta cells. These findings, reported recently, have opened a new window in the study of pore formation, exocytosis from single vesicles, and the mechanisms of insulin secretion. This sensitive cellular electroanalysis approach should help in the development of novel therapeutic strategies targeting diabetes in the future.

单细胞安培法(SCA)是一种强大、灵敏、高时间分辨率的电化学技术,用于定量单个细胞和囊泡分泌的分子信使。该技术已被广泛应用于研究胞吐过程,也被应用于研究单个胰腺β细胞的胰岛素胞吐,尽管频率较低。胰岛素释放不足可导致糖尿病,这是一种影响全球数百万人的慢性生活方式紊乱。本综述旨在总结和强调自20世纪90年代以来,通过使用微电极和纳米电极的SCA监测β细胞分泌胰岛素的电化学测量,并解释血清素如何以及为什么被用作单个β细胞分泌过程中监测胰岛素的代理。最后,我们描述了SCA测量与细胞内囊泡冲击电化学细胞术(IVIEC)技术的结合如何导致关于β细胞中分数释放类型的重要发现。最近报道的这些发现为研究单个囊泡的孔隙形成、胞吐和胰岛素分泌机制打开了一扇新的窗口。这种敏感的细胞电分析方法应该有助于未来针对糖尿病的新治疗策略的发展。
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引用次数: 0
Gas-Liquid-Solid Three-Phase Boundary in Scanning Electrochemical Cell Microscopy. 扫描电化学细胞显微镜中的气-液-固三相边界。
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-10 eCollection Date: 2024-12-18 DOI: 10.1021/acsmeasuresciau.4c00061
C Hyun Ryu, Debasree Mandal, Hang Ren

The gas-liquid-solid interface plays a crucial role in various electrochemical energy conversion devices, including fuel cells and electrolyzers. Understanding the effect of gas transfer on the electrochemistry at this three-phase interface is a grand challenge. Scanning electrochemical cell microscopy (SECCM) is an emerging technique for mapping the heterogeneity in electrochemical activity; it also inherently features a three-phase boundary at the nanodroplet cell. Herein, we quantitatively analyze the role of the three-phase boundary in SECCM involving gas via finite element simulation. Oxygen reduction reaction is used as an example for reaction with a gas reactant, which shows that interfacial gas transfer can enhance the overall mass transport of reactant, allowing measuring current density of several A/cm2. The hydrogen evolution reaction is used as an example for reaction with a gas product, and fast interfacial gas transfer kinetics can significantly reduce the concentration of dissolved gas near the electrode. This helps to measure electrode kinetics at a high current density without the complication of gas bubble formation. The contribution of interfacial gas transfer can be understood by directly comparing its kinetics to the mass transfer coefficient from the solution. Our findings aid the quantitative application of SECCM in studying electrochemical reactions involving gases, establishing a basis for investigating electrochemistry at the three-phase boundary.

气液固界面在各种电化学能量转换装置中起着至关重要的作用,包括燃料电池和电解槽。了解三相界面上气体传递对电化学的影响是一个巨大的挑战。扫描电化学细胞显微镜(SECCM)是一种新兴的电化学活性非均质性成像技术;它本身也具有纳米液滴细胞的三相边界。本文通过有限元模拟,定量分析了三相边界在含气SECCM中的作用。以氧还原反应与气态反应物的反应为例,表明界面气体传递可以增强反应物的整体传质,可以测量到数a /cm2的电流密度。以气体产物的析氢反应为例,快速的界面气体传递动力学可以显著降低电极附近溶解气体的浓度。这有助于在高电流密度下测量电极动力学,而没有气泡形成的复杂性。界面气体传递的贡献可以通过直接将其动力学与溶液的传质系数进行比较来理解。我们的发现有助于SECCM在气体电化学反应研究中的定量应用,为研究三相边界的电化学奠定了基础。
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引用次数: 0
From Insulin Measurement to Partial Exocytosis Model: Advances in Single Pancreatic Beta Cell Amperometry over Four Decades 从胰岛素测量到部分胞吐模型:四十年来单个胰腺β细胞电流测量的进展
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-10 DOI: 10.1021/acsmeasuresciau.4c0005810.1021/acsmeasuresciau.4c00058
Amir Hatamie*, Xiulan He, Andrew Ewing and Patrik Rorsman, 

Single cell Amperometry (SCA) is a powerful, sensitive, high temporal resolution electrochemical technique used to quantify secreted molecular messengers from individual cells and vesicles. This technique has been extensively applied to study the process of exocytosis, and it has also been applied, albeit less frequently, to investigate insulin exocytosis from single pancreatic beta cells. Insufficient insulin release can lead to diabetes, a chronic lifestyle disorder that affects millions of people worldwide. This review aims to summarize and highlight electrochemical measurements of insulin via monitoring its secretion from beta cells by SCA with micro- and nanoelectrodes since the 1990s and to explain how and why serotonin is used as a proxy for monitoring insulin during exocytosis from single beta cells. Finally, we describe how the combination of SCA measurements with the intracellular vesicle impact electrochemical cytometry (IVIEC) technique has led to important findings regarding fractional release types in beta cells. These findings, reported recently, have opened a new window in the study of pore formation, exocytosis from single vesicles, and the mechanisms of insulin secretion. This sensitive cellular electroanalysis approach should help in the development of novel therapeutic strategies targeting diabetes in the future.

单细胞安培法(SCA)是一种强大、灵敏、高时间分辨率的电化学技术,用于定量单个细胞和囊泡分泌的分子信使。该技术已被广泛应用于研究胞吐过程,也被应用于研究单个胰腺β细胞的胰岛素胞吐,尽管频率较低。胰岛素释放不足可导致糖尿病,这是一种影响全球数百万人的慢性生活方式紊乱。本综述旨在总结和强调自20世纪90年代以来,通过使用微电极和纳米电极的SCA监测β细胞分泌胰岛素的电化学测量,并解释血清素如何以及为什么被用作单个β细胞分泌过程中监测胰岛素的代理。最后,我们描述了SCA测量与细胞内囊泡冲击电化学细胞术(IVIEC)技术的结合如何导致关于β细胞中分数释放类型的重要发现。最近报道的这些发现为研究单个囊泡的孔隙形成、胞吐和胰岛素分泌机制打开了一扇新的窗口。这种敏感的细胞电分析方法应该有助于未来针对糖尿病的新治疗策略的发展。
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引用次数: 0
Gas–Liquid–Solid Three-Phase Boundary in Scanning Electrochemical Cell Microscopy 扫描电化学细胞显微镜中的气-液-固三相边界
IF 4.6 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-10 DOI: 10.1021/acsmeasuresciau.4c0006110.1021/acsmeasuresciau.4c00061
C. Hyun Ryu, Debasree Mandal and Hang Ren*, 

The gas–liquid–solid interface plays a crucial role in various electrochemical energy conversion devices, including fuel cells and electrolyzers. Understanding the effect of gas transfer on the electrochemistry at this three-phase interface is a grand challenge. Scanning electrochemical cell microscopy (SECCM) is an emerging technique for mapping the heterogeneity in electrochemical activity; it also inherently features a three-phase boundary at the nanodroplet cell. Herein, we quantitatively analyze the role of the three-phase boundary in SECCM involving gas via finite element simulation. Oxygen reduction reaction is used as an example for reaction with a gas reactant, which shows that interfacial gas transfer can enhance the overall mass transport of reactant, allowing measuring current density of several A/cm2. The hydrogen evolution reaction is used as an example for reaction with a gas product, and fast interfacial gas transfer kinetics can significantly reduce the concentration of dissolved gas near the electrode. This helps to measure electrode kinetics at a high current density without the complication of gas bubble formation. The contribution of interfacial gas transfer can be understood by directly comparing its kinetics to the mass transfer coefficient from the solution. Our findings aid the quantitative application of SECCM in studying electrochemical reactions involving gases, establishing a basis for investigating electrochemistry at the three-phase boundary.

气液固界面在各种电化学能量转换装置中起着至关重要的作用,包括燃料电池和电解槽。了解三相界面上气体传递对电化学的影响是一个巨大的挑战。扫描电化学细胞显微镜(SECCM)是一种新兴的电化学活性非均质性成像技术;它本身也具有纳米液滴细胞的三相边界。本文通过有限元模拟,定量分析了三相边界在含气SECCM中的作用。以氧还原反应与气态反应物的反应为例,表明界面气体传递可以增强反应物的整体传质,可以测量到数a /cm2的电流密度。以气体产物的析氢反应为例,快速的界面气体传递动力学可以显著降低电极附近溶解气体的浓度。这有助于在高电流密度下测量电极动力学,而没有气泡形成的复杂性。界面气体传递的贡献可以通过直接将其动力学与溶液的传质系数进行比较来理解。我们的发现有助于SECCM在气体电化学反应研究中的定量应用,为研究三相边界的电化学奠定了基础。
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引用次数: 0
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ACS Measurement Science Au
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