Analytical science advances最新文献

{"title":"Emerging scientists in analytical sciences: Kim Greis","authors":"Kim Greis","doi":"10.1002/ansa.202200036","DOIUrl":"10.1002/ansa.202200036","url":null,"abstract":"<p></p><p><b>Introduction</b></p><p>Kim Greis is a third-year PhD candidate in the lab of Prof. Kevin Pagel at Freie Universität Berlin and Fritz Haber Institute of the Max Planck Society. He joined Humboldt-Universität zu Berlin in 2014 for his bachelor's studies in chemistry and stayed there for his master's degree. During the latter, he went as an exchange student to the University of Melbourne for a research stay. In 2019, he switched to Freie Universität Berlin to start a PhD project in the group of Prof. Kevin Pagel to study reactive intermediates from bioorganic reactions using mass spectrometry-based methods and density-functional theory calculations. Despite his young career he has already published 21 papers (and counting) and collected numerous prestigious awards, such as a Fulbright Grant, which allowed him to do research at Yale University during his PhD.</p><p><b>How did you get involved in the field of analytical sciences?</b></p><p>I did my bachelor's and master's studies at the Humboldt-Universität zu Berlin. In contrast to other chemistry departments, there is a big analytical division at Humboldt-Universität zu Berlin. Hence, a large selection of mandatory analytical chemistry courses was available. For my bachelor thesis, I joined the lab of Prof. Klaus Rademann and developed a cellulose-based sensor to detect low concentrations of toxic metal ions in aqueous solutions.<span><sup>1</sup></span> During my master's studies, I switched fields during an exchange internship at the University of Melbourne, where I joined the lab of Prof. Richard O'Hair. Here, I got hands-on experience with mass spectrometers for the first time. We used a modified ion trap mass spectrometer that allows for ion-molecule reactions to study phenanthroline-ligated transition state metal complexes. With this setup, we got information on the reactivity of these species and in some cases, we were able to reveal catalytic cycles.<span><sup>2, 3</sup></span> Furthermore, I learned in Australia about using computational methods, such as density-functional theory, to support my data from mass spectrometry. Subsequently, I joined the lab of Kevin Pagel at Freie Universität Berlin and the Fritz Haber Institute of the Max Planck Society for my master's thesis and stayed there for my PhD.</p><p><b>What is the topic of your PhD studies?</b></p><p>In my PhD studies, I combine computational methods and cryogenic vibrational spectroscopy in helium nanodroplets to investigate the structure of reactive intermediates. Cryogenic vibrational spectroscopy of ions is a mass spectrometry-based technique that I will introduce in a moment. The method yields highly resolved infrared spectra that, in combination with computed frequencies, are very suitable to determine the structure of ions. We used the technique mainly to study glycosyl cations, the reactive intermediate of glycosynthesis.<span><sup>4-6</sup></span> In a second step, we correlate the structure with the stereosele","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 9-10","pages":"258-261"},"PeriodicalIF":0.0,"publicationDate":"2022-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200036","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"45593293","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}

{"title":"Time-resolved multiparameter analytics on a cell-free production platform for acyl-CoA precursors","authors":"Dominic Maehler,&nbsp;Sandra Hoefgen,&nbsp;Ute Münchberg,&nbsp;Oliver J. Schmitz,&nbsp;Julia Rautschek,&nbsp;Ying Huang,&nbsp;Erik Freier,&nbsp;Vito Valiante","doi":"10.1002/ansa.202200021","DOIUrl":"10.1002/ansa.202200021","url":null,"abstract":"<p>Cell-free biosynthesis is emerging as a very attractive alternative for the production of market-relevant molecules. The free combination of enzymes, regardless of where they are isolated from, raises the possibility to build more efficient synthetic routes but at the same time leads to higher complexity regarding the analysis of the different enzymatic steps. Here we present an analytical method for the real-time analysis of acyl-CoA blocks forming and consuming during multi-step catalyses. We focused on malonyl-Coenzyme A and acetyl-CoA, which are the most used acyl-CoA units for carbon chain elongations. By employing capillary electrophoresis, we could detect the decrease of educts and the formation of products in a time-resolved fashion.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 11-12","pages":"289-296"},"PeriodicalIF":0.0,"publicationDate":"2022-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200021","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43605994","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}

{"title":"Precision evaluation of nitrogen isotope ratios by Raman spectrometry","authors":"Junji Yamamoto,&nbsp;Yuuki Hagiwara","doi":"10.1002/ansa.202200020","DOIUrl":"10.1002/ansa.202200020","url":null,"abstract":"<p>We measured Raman spectra of N₂ fluids obtained at 0.1–25 MPa at room temperature. The ¹⁴N¹⁵N peak in the Raman spectrum of a low-pressure N₂ fluid is difficult to detect because of the prevalence of a group of peaks attributed to rotational vibration of ¹⁴N₂. The Raman peaks of ¹⁴N¹⁵N and ¹⁴N₂ of N₂ fluid at 25 MPa were acquired at various exposure times. The mean values and standard deviations of the peak height ratios and peak area ones of ¹⁴N¹⁵N and ¹⁴N₂ were examined for each time. The standard deviations of the peak height ratios and peak area ones were 2.2% and 1.9%, respectively, for 20 spectra acquired with peak height of 1 million counts of ¹⁴N₂. The uncertainties are about two times higher than those predicted from the noise of a CCD. Improvement of the pixel resolution can enhance the precision of the nitrogen isotope ratios by Raman spectroscopy.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 9-10","pages":"269-277"},"PeriodicalIF":0.0,"publicationDate":"2022-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200020","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47615411","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}

{"title":"Toward a greener approach to detect inorganic arsenic using the Gutzeit method and X-ray fluorescence spectroscopy","authors":"Helen Lin,&nbsp;Haochen Dai,&nbsp;Lili He","doi":"10.1002/ansa.202200014","DOIUrl":"10.1002/ansa.202200014","url":null,"abstract":"<p>Inorganic arsenic is a carcinogen repeatedly found in water and foods threatening global human health. Prior work applied the Gutzeit method and X-ray fluorescence spectroscopy to quantify inorganic arsenic based on a harmful chemical, i.e., mercury bromide, to capture the arsine gas. In this project, we explored silver nitrate as an alternative to mercury bromide for the capture and detection of inorganic arsenic. To compare the performance of mercury bromide and silver nitrate, two standard curves were established in the range from 0 to 33.3 µg/L after optimization of reaction conditions such as the quantity of reagents and reaction time. Our result shows silver nitrate-based standard curve had a lower limit of detection and limit of quantification at 1.02 µg/L and 3.40 µg/L, respectively, as compared to the one built upon mercury bromide that has limit of detection of 4.86 µg/L and limit of quantification of 16.2 µg/L. The relative higher sensitivity when using silver nitrate was contributed by the less interfering elements for X-ray fluorescence analysis and thus lower background signals. A commercial apple juice was studied for matrix inference, and the results show 85%–99% recoveries and 7.4%–24.5% relative standard deviation. In conclusion, we demonstrated silver nitrate is a better choice in terms of safety restrictions and detection capability at lower inorganic arsenic concentrations.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 9-10","pages":"262-268"},"PeriodicalIF":0.0,"publicationDate":"2022-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200014","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41888396","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}

{"title":"Cross-validated permutation feature importance considering correlation between features","authors":"Hiromasa Kaneko","doi":"10.1002/ansa.202200018","DOIUrl":"10.1002/ansa.202200018","url":null,"abstract":"<p>In molecular design, material design, process design, and process control, it is important not only to construct a model with high predictive ability between explanatory features x and objective features y using a dataset but also to interpret the constructed model. An index of feature importance in x is permutation feature importance (PFI), which can be combined with any regressors and classifiers. However, the PFI becomes unstable when the number of samples is low because it is necessary to divide a dataset into training and validation data when calculating it. Additionally, when there are strongly correlated features in x, the PFI of these features is estimated to be low. Hence, a cross-validated PFI (CVPFI) method is proposed. CVPFI can be calculated stably, even with a small number of samples, because model construction and feature evaluation are repeated based on cross-validation. Furthermore, by considering the absolute correlation coefficients between the features, the feature importance can be evaluated appropriately even when there are strongly correlated features in x. Case studies using numerical simulation data and actual compound data showed that the feature importance can be evaluated appropriately using CVPFI compared to PFI. This is possible when the number of samples is low, when linear and nonlinear relationships are mixed between x and y when there are strong correlations between features in x, and when quantised and biased features exist in x. Python codes for CVPFI are available at https://github.com/hkaneko1985/dcekit.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 9-10","pages":"278-287"},"PeriodicalIF":0.0,"publicationDate":"2022-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47450935","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}

{"title":"Front Cover: Resonance Raman analysis of intracellular vitamin B12 analogs in methanogenic archaea","authors":"","doi":"10.1002/ansa.202200900","DOIUrl":"https://doi.org/10.1002/ansa.202200900","url":null,"abstract":"<p>The cover image is based on the Research Article <i>Resonance Raman analysis of intracellular vitamin B₁₂ analogs in methanogenic archaea</i> by Nanako Kanno et al., https://doi.org/10.1002/ansa.202100042.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 5-6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200900","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"137712597","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}

{"title":"Helping reviewers assess statistical analysis: A case study from analytic methods","authors":"Ron S. Kenett,&nbsp;Bernard G. Francq","doi":"10.1002/ansa.202000159","DOIUrl":"10.1002/ansa.202000159","url":null,"abstract":"<p>Analytic methods development, like many other disciplines, relies on experimentation and data analysis. Determining the contribution of a paper or report on a study incorporating data analysis is typically left to the reviewer's experience and good sense, without reliance on structured guidelines. This is amplified by the growing role of machine learning driven analysis, where results are based on computer intensive algorithm applications. The evaluation of a predictive model where cross validation was used to fit its parameters adds challenges to the evaluation of regression models, where the estimates can be easily reproduced. This lack of structure to support reviews increases uncertainty and variability in reviews. In this paper, aspects of statistical assessment are considered. We provide checklists for reviewers of applied statistics work with a focus on analytic method development. The checklist covers six aspects relevant to a review of statistical analysis, namely: (1) study design, (2) algorithmic and inferential methods in frequentism analysis, (3) Bayesian methods in Bayesian analysis (if relevant), (4) selective inference aspects, (5) severe testing properties and (6) presentation of findings. We provide a brief overview of these elements providing references for a more elaborate treatment. The robustness analysis of an analytical method is used to illustrate how an improvement can be achieved in response to questions in the checklist. The paper is aimed at both engineers and seasoned researchers.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 5-6","pages":"212-222"},"PeriodicalIF":0.0,"publicationDate":"2022-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202000159","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43247494","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}

{"title":"Adaptive soft sensor based on transfer learning and ensemble learning for multiple process states","authors":"Nobuhito Yamada,&nbsp;Hiromasa Kaneko","doi":"10.1002/ansa.202200013","DOIUrl":"10.1002/ansa.202200013","url":null,"abstract":"<p>The objective of this study is to develop an adaptive software sensor technique that can predict objective process variables for a target grade in a plant while also considering information related to various other grades. We use a dataset of the target grade as the target domain and those of the other grades as source domains to perform transfer learning. Multiple models or sub-models are constructed by setting a source domain for each grade and changing the number of samples used as the source domain. Furthermore, to prevent the negative transfer, the use of a source domain is automatically judged. In this study, we constructed sub-models using the locally weighted partial least squares approach as an adaptive soft sensor technique. The values of an objective variable were predicted with ensemble learning using sub-models. The effectiveness of the proposed method was verified using a dataset measured in an actual incineration plant, and the proposed method was able to accurately predict the product quality even when the plant was operated in five grades and when a new grade was produced.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 5-6","pages":"205-211"},"PeriodicalIF":0.0,"publicationDate":"2022-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200013","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48047879","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}

{"title":"A validated liquid chromatography-tandem mass spectroscopy method for the quantification of tolinapant in human plasma","authors":"Vanessa Martins,&nbsp;Nicola Wilsher,&nbsp;Song Lin,&nbsp;Aram Oganesian","doi":"10.1002/ansa.202200009","DOIUrl":"10.1002/ansa.202200009","url":null,"abstract":"<p>Tolinapant (ASTX660), a pan-selective inhibitor of apoptosis protein antagonist with dual cIAP/XIAP activity, was identified as a clinical candidate in preclinical efficacy, pharmacokinetic and safety studies. In order to assess tolinapant in first-in-human Phase I/II clinical trials, a validated bioanalytical method was required to determine plasma pharmacokinetics. Tolinapant and d₄-tolinapant were extracted from human plasma using liquid-liquid extraction. Separation chromatography was performed on a Acquity BEH C18 1.7 µM, 50 mm × 2.1 mm i.d. column, using a mobile phase of 0.1% formic acid in water and 0.1% formic acid in acetonitrile. Mass spectrometry detection was performed by positive turbo ion spray ionisation, in multiple reaction monitoring mode. The method was validated according to the US Food and Drug Administration (FDA) guidelines. The method has a quantifiable linear range of 1–500 ng/mL (<i>r</i>² = 0.999). The intra- and inter-day coefficients of variation were &lt; 11.4%. Dilution QC samples agreed with prepared concentrations, with a precision of 1.5% and accuracy of 101%. Tolinapant mean recoveries ranged from 85.1–94.4 % with negligible matrix effects. A highly sensitive and selective LC-MS/MS bioanalytical method was developed and validated. The method was successfully applied in Phase 1/2 clinical trials to determine the human pharmacokinetic profile of tolinapant.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 5-6","pages":"198-204"},"PeriodicalIF":0.0,"publicationDate":"2022-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202200009","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41385035","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}

{"title":"Artificial amniotic fluid for nuclear magnetic resonance spectroscopy studies","authors":"Doshina Naila,&nbsp;Siddharth Sadanand,&nbsp;Dafna Sussman","doi":"10.1002/ansa.202100055","DOIUrl":"10.1002/ansa.202100055","url":null,"abstract":"<p>Amniocentesis is the process of retrieving the nutrient-rich amniotic fluid (AF) that encompasses the growing fetus in order to diagnose fetal diseases and developmental disorders. Currently, it is only performed on pregnant persons at risk and is invasive with the potential for infection and in some cases, miscarriage. A non-invasive alternative is needed and could be developed using magnetic resonance spectroscopy (MRS). To develop such MRS sequences, ample testing and training are needed and could be most efficiently conducted on a phantom. We propose a protocol for creating such a synthetic AF phantom for MRS testing and optimization. The proposed AF is validated using nuclear magnetic resonance (NMR) proving it produces spectra comparable to those in the literature. The results from this study can aid in developing a non-invasive fetal diagnostic tool to replace amniocentesis.</p>","PeriodicalId":93411,"journal":{"name":"Analytical science advances","volume":"3 5-6","pages":"174-187"},"PeriodicalIF":0.0,"publicationDate":"2022-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ansa.202100055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44912938","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}