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2023 Rising Stars in Measurement Science 2023 年测量科学新星
Q3 Chemistry Pub Date : 2024-03-19 DOI: 10.1021/acsmeasuresciau.4c00013
Shelley Minteer*, 
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引用次数: 0
T1 Relaxation of Methane in Mixtures with Gaseous Water T1 甲烷与气态水混合物的弛豫
Q3 Chemistry Pub Date : 2024-03-04 DOI: 10.1021/acsmeasuresciau.4c00001
Harm Ridder*, Wolfgang Dreher and Jorg Thöming, 

Synthetic, ecofriendly fuels and chemicals can be produced through Power-To-X (PtX) processes. To study such catalytic processes operando and spatially resolved, magnetic resonance imaging (MRI) is a versatile tool. A main issue in the application of MRI in reactive studies is a lack of knowledge about how the gathered signals can be interpreted into reaction data like temperature or species concentration. In this work, the interaction of methane and gaseous water is studied regarding their longitudinal relaxation time T1 and the chemical shift. To this end, defined quantities of methane-water mixtures were sealed in glass tubes and probed at temperatures between 130 and 360 °C and pressures from 6 to 20 bar. From the obtained T1 relaxation times, the collision cross section of methane with water σj,CH4-H2O is derived, which can be used to estimate the temperature and molar concentration of methane during the methanation reaction. The obtained T1 relaxation times can additionally be used to improve the timing of MRI sequences involving water vapor or methane. Further, details about the measurement workflow and tube preparation are shared.

通过功率-X(PtX)过程可以生产出合成的环保燃料和化学品。为研究此类催化过程的操作和空间分辨率,磁共振成像(MRI)是一种多功能工具。磁共振成像在反应研究中应用的一个主要问题是,人们对如何将收集到的信号解释为温度或物种浓度等反应数据缺乏了解。在这项工作中,研究了甲烷和气态水在纵向弛豫时间 T1 和化学位移方面的相互作用。为此,将一定量的甲烷-水混合物密封在玻璃管中,在温度为 130 至 360 °C、压力为 6 至 20 巴的条件下进行探测。根据所获得的 T1 驰豫时间,可以推导出甲烷与水的碰撞截面 σj,CH4-H2O,该截面可用于估算甲烷化反应过程中甲烷的温度和摩尔浓度。此外,获得的 T1 驰豫时间还可用于改善涉及水蒸气或甲烷的磁共振成像序列的时间选择。此外,还分享了有关测量工作流程和试管制备的详细信息。
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引用次数: 0
Quantitative Measurement Technique for Anodic Corrosion of BDD Advanced Oxidation Electrodes BDD 高级氧化电极阳极腐蚀定量测量技术
Q3 Chemistry Pub Date : 2024-02-23 DOI: 10.1021/acsmeasuresciau.3c00069
Joshua J. Tully*, Daniel Houghton, Ben G. Breeze, Timothy P. Mollart and Julie V. Macpherson*, 

Electrochemical advanced oxidation (EAO) systems are of significant interest due to their ability to treat a wide range of organic contaminants in water. Boron doped diamond (BDD) electrodes have found considerable use in EAO. Despite their popularity, no laboratory scale method exists to quantify anodic corrosion of BDD electrodes under EAO conditions; all are qualitative using techniques such as scanning electron microscopy, electrochemistry, and spectroscopy. In this work, we present a new method which can be used to quantify average corrosion rates as a function of solution composition, current density, and BDD material properties over relatively short time periods. The method uses white light interferometry (WLI), in conjunction with BDD electrodes integrated into a 3D-printed flow cell, to measure three-dimensional changes in the surface structure due to corrosion over a 72 h period. It is equally applicable to both thin film and thicker, freestanding BDD. A further advantage of WLI is that it lends itself to large area measurements; data are collected herein for 1 cm diameter disk electrodes. Using WLI, corrosion rates as low as 1 nm h–1 can be measured. This enables unequivocal demonstration that organics in the EAO solution are not a prerequisite for BDD anodic corrosion. However, they do increase the corrosion rates. In particular, we quantify that addition of 1 M acetic acid to 0.5 M potassium sulfate results in the average corrosion rate increasing ∼60 times. In the same solution, microcrystalline thin film BDD is also found to corrode ∼twice as fast compared to freestanding polished BDD, attributed to the presence of increased sp2 carbon content. This methodology also represents an important step forward in the prediction of BDD electrode lifetimes for a wide range of EAO applications.

电化学高级氧化(EAO)系统能够处理水中的各种有机污染物,因此备受关注。掺硼金刚石(BDD)电极在 EAO 中得到了广泛应用。尽管它们很受欢迎,但目前还没有实验室规模的方法来量化 BDD 电极在 EAO 条件下的阳极腐蚀;所有方法都是使用扫描电子显微镜、电化学和光谱学等技术进行定性分析。在这项工作中,我们提出了一种新方法,可用于量化相对较短时间内作为溶液成分、电流密度和 BDD 材料特性函数的平均腐蚀率。该方法使用白光干涉仪(WLI),结合集成到三维打印流动池中的 BDD 电极,测量 72 小时内因腐蚀引起的表面结构的三维变化。它同样适用于薄膜和较厚的独立 BDD。WLI 的另一个优点是适合大面积测量;本文收集的数据是直径为 1 厘米的圆盘电极。使用 WLI 可以测量低至 1 nm h-1 的腐蚀速率。这就明确证明了 EAO 溶液中的有机物并不是 BDD 阳极腐蚀的先决条件。但是,有机物确实会增加腐蚀速率。特别是,我们发现在 0.5 M 硫酸钾中加入 1 M 乙酸会使平均腐蚀速率增加 60 倍。在同一溶液中,微晶薄膜 BDD 的腐蚀速度也是独立抛光 BDD 的两倍,这归因于 Sp2 碳含量的增加。这种方法也代表了在预测 BDD 电极寿命方面向前迈出的重要一步,它适用于广泛的 EAO 应用。
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引用次数: 0
A Look into Ocular Diseases: The Pivotal Role of Omics Sciences in Ophthalmology Research 透视眼部疾病:Omics 科学在眼科研究中的关键作用
Q3 Chemistry Pub Date : 2024-02-22 DOI: 10.1021/acsmeasuresciau.3c00067
Maurine Fucito, Matteo Spedicato, Simona Felletti, Angeli Christy Yu, Massimo Busin, Luisa Pasti, Flavio A. Franchina, Alberto Cavazzini, Chiara De Luca* and Martina Catani*, 

Precision medicine is a new medical approach which considers both population characteristics and individual variability to provide customized healthcare. The transition from traditional reactive medicine to personalized medicine is based on a biomarker-driven process and a deep knowledge of biological mechanisms according to which the development of diseases occurs. In this context, the advancements in high-throughput omics technologies represent a unique opportunity to discover novel biomarkers and to provide an unbiased picture of the biological system. One of the medical fields in which omics science has started to be recently applied is that of ophthalmology. Ocular diseases are very common, and some of them could be highly disabling, thus leading to vision loss and blindness. The pathogenic mechanism of most ocular diseases may be dependent on various genetic and environmental factors, whose effect has not been yet completely understood. In this context, large-scale omics approaches are fundamental to have a comprehensive evaluation of the whole system and represent an essential tool for the development of novel therapies. This Review summarizes the recent advancements in omics science applied to ophthalmology in the last ten years, in particular by focusing on proteomics, metabolomics and lipidomics applications from an analytical perspective. The role of high-efficiency separation techniques coupled to (high-resolution) mass spectrometry ((HR)MS) is also discussed, as well as the impact of sampling, sample preparation and data analysis as integrating parts of the analytical workflow.

精准医疗是一种新的医疗方法,它同时考虑了人群特征和个体差异,以提供量身定制的医疗服务。从传统的反应医学到个性化医学的转变是基于生物标志物驱动的过程和对疾病发生发展的生物机制的深入了解。在这种情况下,高通量 omics 技术的进步为发现新型生物标记物和提供生物系统的公正图像提供了一个独特的机会。眼科是最近开始应用全息技术的医学领域之一。眼部疾病非常常见,其中一些可能会造成严重的残疾,从而导致视力丧失和失明。大多数眼科疾病的致病机制可能取决于各种遗传和环境因素,而这些因素的影响尚未完全明了。在这种情况下,大规模全息方法是对整个系统进行全面评估的基础,也是开发新型疗法的重要工具。本综述总结了过去十年中应用于眼科的全局组学科学的最新进展,特别是从分析的角度重点介绍了蛋白质组学、代谢组学和脂质组学的应用。文章还讨论了高效分离技术与(高分辨率)质谱联用((HR)MS)的作用,以及作为分析工作流程整合部分的取样、样品制备和数据分析的影响。
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引用次数: 0
ACS Measurement Science Au in 2024 2024 年的 ACS 测量科学区
Q3 Chemistry Pub Date : 2024-02-21 DOI: 10.1021/acsmeasuresciau.4c00006
Shelley Minteer*, 
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引用次数: 0
Recent Developments in Machine Learning for Mass Spectrometry 质谱分析机器学习的最新进展
Q3 Chemistry Pub Date : 2024-02-21 DOI: 10.1021/acsmeasuresciau.3c00060
Armen G. Beck, Matthew Muhoberac, Caitlin E. Randolph, Connor H. Beveridge, Prageeth R. Wijewardhane, Hilkka I. Kenttämaa and Gaurav Chopra*, 

Statistical analysis and modeling of mass spectrometry (MS) data have a long and rich history with several modern MS-based applications using statistical and chemometric methods. Recently, machine learning (ML) has experienced a renaissance due to advents in computational hardware and the development of new algorithms for artificial neural networks (ANN) and deep learning architectures. Moreover, recent successes of new ANN and deep learning architectures in several areas of science, engineering, and society have further strengthened the ML field. Importantly, modern ML methods and architectures have enabled new approaches for tasks related to MS that are now widely adopted in several popular MS-based subdisciplines, such as mass spectrometry imaging and proteomics. Herein, we aim to provide an introductory summary of the practical aspects of ML methodology relevant to MS. Additionally, we seek to provide an up-to-date review of the most recent developments in ML integration with MS-based techniques while also providing critical insights into the future direction of the field.

质谱(MS)数据的统计分析和建模有着悠久而丰富的历史,一些基于质谱的现代应用都使用了统计和化学计量方法。最近,由于计算硬件的进步以及人工神经网络(ANN)和深度学习架构新算法的开发,机器学习(ML)经历了一次复兴。此外,新的人工神经网络和深度学习架构最近在科学、工程和社会的多个领域取得了成功,进一步加强了 ML 领域。重要的是,现代 ML 方法和架构为 MS 相关任务提供了新的方法,这些方法目前已在质谱成像和蛋白质组学等多个基于 MS 的热门子学科中被广泛采用。在此,我们旨在对与 MS 相关的 ML 方法的实际方面进行介绍性总结。此外,我们还将对 ML 与基于 MS 的技术相结合方面的最新发展进行综述,同时对该领域的未来发展方向提出重要见解。
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引用次数: 0
Labeling of Mucin-Type O-Glycans for Quantification Using Liquid Chromatography and Fluorescence Detection 利用液相色谱法和荧光检测法标记粘蛋白型 O-糖以进行定量分析
Q3 Chemistry Pub Date : 2024-02-14 DOI: 10.1021/acsmeasuresciau.3c00071
Marc Safferthal, Leïla Bechtella, Andreas Zappe, Gaël M. Vos and Kevin Pagel*, 

O-glycosylation is a common post-translational modification that is essential for the defensive properties of mucus barriers. Incomplete and altered O-glycosylation is often linked to severe diseases, such as cancer, cystic fibrosis, and chronic obstructive pulmonary disease. Originating from a nontemplate-driven biosynthesis, mucin-type O-glycan structures are very complex. They are often present as heterogeneous mixtures containing multiple isomers. Therefore, the analysis of complex O-glycan mixtures usually requires hyphenation of orthogonal techniques such as liquid chromatography (LC), ion mobility spectrometry, and mass spectrometry (MS). However, MS-based techniques are mainly qualitative. Moreover, LC separation of O-glycans often lacks reproducibility and requires sophisticated data treatment and analysis. Here we present a mucin-type O-glycomics analysis workflow that utilizes hydrophilic interaction liquid chromatography for separation and fluorescence labeling for detection and quantification. In combination with mass spectrometry, a detailed analysis on the relative abundance of specific mucin-type O-glycan compositions and features, such as fucose, sialic acids, and sulfates, is performed. Furthermore, the average number of monosaccharide units of O-glycans in different samples was determined. To demonstrate universal applicability, the method was tested on mucins from different tissue types and mammals, such as bovine submaxillary mucins, porcine gastric mucins, and human milk mucins. To account for day-to-day retention time shifts in O-glycan separations and increase the comparability between different instruments and laboratories, we included fluorescently labeled dextran ladders in our workflow. In addition, we set up a library of glucose unit values for all identified O-glycans, which can be used to simplify the identification process of glycans in future analyses.

O 型糖基化是一种常见的翻译后修饰,对粘液屏障的防御特性至关重要。O-糖基化不完全或发生改变往往与癌症、囊性纤维化和慢性阻塞性肺病等严重疾病有关。源自非模板驱动的生物合成,粘蛋白型 O 型糖结构非常复杂。它们通常是含有多种异构体的异质混合物。因此,分析复杂的 O-聚糖混合物通常需要采用正交技术,如液相色谱法(LC)、离子迁移谱法和质谱法(MS)。然而,基于质谱的技术主要是定性的。此外,液相色谱分离 O 型糖往往缺乏重现性,需要复杂的数据处理和分析。在此,我们介绍一种利用亲水相互作用液相色谱进行分离、利用荧光标记进行检测和定量的粘蛋白型 O-聚糖分析工作流程。结合质谱法,我们可以详细分析特定粘蛋白型 O-糖组成和特征(如岩藻糖、硅酸和硫酸盐)的相对丰度。此外,还测定了不同样本中 O 型聚糖单糖单位的平均数量。为了证明该方法的普遍适用性,对来自不同组织类型和哺乳动物的粘蛋白(如牛颌下腺粘蛋白、猪胃粘蛋白和人奶粘蛋白)进行了测试。为了考虑到O-糖分离过程中每天的保留时间变化,并提高不同仪器和实验室之间的可比性,我们在工作流程中加入了荧光标记的葡聚糖阶梯。此外,我们还为所有已鉴定的 O 型聚糖建立了葡萄糖单位值库,可用于简化今后分析中聚糖的鉴定过程。
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引用次数: 0
Ultratrace eNose Sensing of VOCs toward Breath Analysis Applications Utilizing an eNose-Based Analyzer 利用基于电子鼻的分析仪对挥发性有机化合物进行超痕量电子鼻传感,以实现呼吸分析应用
Q3 Chemistry Pub Date : 2024-02-05 DOI: 10.1021/acsmeasuresciau.3c00053
Johannes Glöckler, Carsten Jaeschke, Marta Padilla, Jan Mitrovics and Boris Mizaikoff*, 

This proof-of-principle study presents the ability of the recently developed iLovEnose to measure ultratrace levels of volatile organic compounds (VOCs) in simulated human breath based on the combination of multiple gas sensors. The iLovEnose was developed by our research team as a test bed for gas sensors that can be hosted in three serially connected compact low-volume and temperature-controlled compartments. Herein, the eNose system was equipped with conventional semiconducting metal oxide (MOX) gas sensors using a variety of base technologies providing 11 different sensor signals that were evaluated to determine six VOCs of interest at eight low to ultralow concentration levels (i.e., ranging from 3 to 0.075 ppm) at humid conditions (90% rh at 22 °C). The measurements were randomized and performed four times over a period of 2 weeks. Partial least-squares regression analysis was applied to estimate the concentration of these six analytes. It was shown that the iLovEnose system is able to discriminate between these VOCs and provide reliable quantitative information relevant for future applications in exhaled breath analysis as a diagnostic disease detection or monitoring device.

这项原理验证研究展示了最近开发的 iLovEnose 在多个气体传感器组合的基础上测量模拟人体呼吸中超微量挥发性有机化合物 (VOC) 的能力。iLovEnose 由我们的研究团队开发,作为气体传感器的试验平台,可安装在三个串行连接的紧凑型低容量温控舱内。在这里,eNose 系统配备了传统的半导体金属氧化物(MOX)气体传感器,采用多种基础技术,提供 11 种不同的传感器信号,在潮湿条件下(90% rh,22 °C),在 8 个低到超低浓度水平(即从 3 到 0.075 ppm 不等)对 6 种相关挥发性有机化合物进行了评估测定。测量是随机进行的,在两周内进行了四次。应用偏最小二乘回归分析来估算这六种分析物的浓度。结果表明,iLovEnose 系统能够区分这些挥发性有机化合物,并提供可靠的定量信息,适用于未来作为疾病诊断检测或监测设备的呼气分析应用。
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引用次数: 0
Two-Dimensional Fluctuation Correlation Spectroscopy (2D-FlucCS): A Method to Determine the Origin of Relaxation Rate Dispersion 二维波动相关光谱(2D-FlucCS):一种确定弛豫率散布起源的方法
Q3 Chemistry Pub Date : 2024-02-01 DOI: 10.1021/acsmeasuresciau.3c00048
Ruchir Gupta,  and , Sachin Dev Verma*, 

Relaxation rate dispersion, i.e., nonexponential or multicomponent kinetics, is observed in complex systems when measuring relaxation kinetics. Often, the origin of rate dispersion is associated with the heterogeneity in the system. However, both homogeneous (where all molecules experience the same rate but inherently nonexponential) and heterogeneous (where all molecules experience different rates) systems can exhibit rate dispersion. A multidimensional correlation analysis method has been demonstrated to detect and quantify rate dispersion observed in molecular rotation, diffusion, solvation, and reaction kinetics. One-dimensional (1D) autocorrelation function detects rate dispersion and measures its extent. Two-dimensional (2D) autocorrelation function measures the origin of rate dispersion and distinguishes homogeneous from heterogeneous. In a heterogeneous system, implicitly there exist subensembles of molecules experiencing different rates. A three-dimensional (3D) autocorrelation function measures subensemble exchange if present and reveals if the system possesses static or dynamic heterogeneity. This perspective discusses the principles, applications, and potential and also presents a future outlook of two-dimensional fluctuation correlation spectroscopy (2D-FlucCS). The method is applicable to any experiment or simulation where a time series of fluctuation in an observable (emission, scattering, current, etc.) around a mean value can be obtained in steady state (equilibrium or nonequilibrium), provided the system is ergodic.

在测量弛豫动力学时,会在复杂系统中观察到弛豫速率分散,即非指数或多组分动力学。通常,速率离散的起源与系统中的异质性有关。然而,同质(所有分子的速率相同,但本质上是非指数)和异质(所有分子的速率不同)系统都会出现速率离散现象。已证明一种多维相关分析方法可以检测和量化在分子旋转、扩散、溶解和反应动力学中观察到的速率离散性。一维(1D)自相关函数可检测速率离散并测量其程度。二维(2D)自相关函数测量速率离散的起源,并区分均相和异相。在异质系统中,隐含地存在着经历不同速率的分子子系统。三维(3D)自相关函数可测量是否存在亚集合交换,并揭示系统是否具有静态或动态异质性。本视角讨论了二维波动相关光谱法(2D-FlucCS)的原理、应用和潜力,并对其未来进行了展望。该方法适用于任何实验或模拟,只要系统是遍历的,就能在稳态(平衡或非平衡)下获得观测值(发射、散射、电流等)围绕平均值波动的时间序列。
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引用次数: 0
Self-Immolative Electrochemical Redox Substrates: Emerging Artificial Receptors in Sensing and Biosensing 自惰性电化学氧化还原底物:传感和生物传感领域的新兴人工受体
Q3 Chemistry Pub Date : 2024-01-18 DOI: 10.1021/acsmeasuresciau.3c00057
Kesavan Manibalan, Ponnusamy Arul, Hsin-Jay Wu, Sheng-Tung Huang* and Veerappan Mani*, 

The development of artificial receptors has great significance in measurement science and technology. The need for a robust version of natural receptors is getting increased attention because the cost of natural receptors is still high along with storage difficulties. Aptamers, imprinted polymers, and nanozymes are some of the matured artificial receptors in analytical chemistry. Recently, a new direction has been discovered by organic chemists, who can synthesize robust, activity-based, self-immolative organic molecules that have artificial receptor properties for the targeted analytes. Specifically designed trigger moieties implant selectivity and sensitivity. These latent electrochemical redox substrates are highly stable, mass-producible, inexpensive, and eco-friendly. Combining redox substrates with the merits of electrochemical techniques is a good opportunity to establish a new direction in artificial receptors. This Review provides an overview of electrochemical redox substrate design, anatomy, benefits, and biosensing potential. A proper understanding of molecular design can lead to the development of a library of novel self-immolative redox molecules that would have huge implications for measurement science and technology.

人工受体的开发在测量科学和技术领域具有重要意义。由于天然受体的成本仍然很高,而且难以储存,因此对天然受体的稳健版本的需求日益受到关注。在分析化学领域,一些成熟的人工受体包括肽聚体、印迹聚合物和纳米酶。最近,有机化学家发现了一个新的方向,他们可以合成稳健的、基于活性的、具有目标分析物人工受体特性的自惰性有机分子。专门设计的触发分子可植入选择性和灵敏度。这些潜在的电化学氧化还原底物高度稳定、可大规模生产、价格低廉且环保。将氧化还原底物与电化学技术的优点相结合,是开创人工受体新方向的良机。本综述概述了电化学氧化还原底物的设计、解剖、优点和生物传感潜力。正确理解分子设计可以开发出新型自惰性氧化还原分子库,这将对测量科学和技术产生巨大影响。
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引用次数: 0
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ACS Measurement Science Au
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