Article
Chemistry, Analytical
Somaye Vali Zade, Klaus Neymeyr, Hamid Abdollahi, Mathias Sawall
Summary: Multivariate curve resolution (MCR) techniques are powerful for spectral data analysis but suffer from non-unique solutions and a continuum of possible pure component profiles. Additional constraints can improve the reliability of quantitative results and decrease ambiguity. Imposing unimodality constraints effectively limits the feasible solutions of MCR methods.
MICROCHEMICAL JOURNAL
(2021)
Article
Automation & Control Systems
Roma Tauler
Summary: The extension of MCR-ALS to analyze multiway data with multilinear constraints is described in the paper, allowing for implementation of constraints for different components in different modes and introducing different levels of complexity of multilinear models, including mixed models. This approach is tested on multiway data sets of varying complexity and has shown to be adequate and advantageous compared to current methods.
JOURNAL OF CHEMOMETRICS
(2021)
Article
Chemistry, Analytical
Maira D. Carabajal, Rocio Pellegrino Vidal, Juan A. Arancibia, Alejandro C. Olivieri
Summary: The abnormal features in the retrieved profile, such as abnormal lumps or negative dips, when using MCR-ALS to process second-order chromatographic-spectral data with baseline contributions, are caused by remaining rotational ambiguity. A new background interpolation constraint is proposed to avoid these abnormal features. The new constraint is supported by both simulated and experimental data, with the latter showing consistent analyte concentration estimations as previously reported.
ANALYTICA CHIMICA ACTA
(2023)
Article
Chemistry, Analytical
Silvia Mas Garcia, Jean-Michel Roger, Ruzica Ferbus, Denis Lourdin, Corinne Rondeau-Mouro
Summary: Magnetic resonance microimaging (MR mu I) is an excellent technique for studying water transfers in millimetric bio-based materials. In this study, the combination of MR mu I and multivariate curve resolution-alternating least squares (MCR-ALS) is proposed to monitor the water ingress into a potato starch extruded blend containing 20% glycerol. This approach provides spectral signatures and distribution maps of the components involved in the water uptake process, allowing for the resolution of two waterfronts at different times.
Article
Automation & Control Systems
Peter S. Kenny, Chiaki Crews, Tom Fearn, Robert D. Speller
Summary: Energy dispersive X-ray diffraction (EDXRD) and maximum likelihood principal component analysis multivariate curve resolution-alternating least squares (MLPCA-MCR-ALS) with correlation constraint were used to quantify the composition of packaged pharmaceutical formulations. MLPCA was used as a data pretreatment step to MCR-ALS, improving the resolution accuracy for the data set. The study successfully resolved the compositions of packaged pharmaceutical formulations by modeling the EDXRD profiles of both unpackaged and packaged samples simultaneously.
JOURNAL OF CHEMOMETRICS
(2021)
Article
Biochemical Research Methods
Xiaqiong Fan, Pan Ma, Minghui Hou, Yiping Ni, Zhi Fang, Hongmei Lu, Zhimin Zhang
Summary: Gas chromatography-mass spectrometry (GC-MS) is a major platform for analyzing volatile compounds in complex samples. DeepResolution, a method proposed in this study, utilizes deep learning to extract compound information from GC-MS data, showing superior compound identification capability and better quantitative performances. The method is automatic and adaptive, allowing for efficient resolution of overlapped components.
JOURNAL OF CHROMATOGRAPHY A
(2021)
Article
Chemistry, Analytical
Xiaqiong Fan, Zhenbo Xu, Hailiang Zhang, Dabiao Liu, Qiong Yang, Qiaotao Tao, Ming Wen, Xiao Kang, Zhimin Zhang, Hongmei Lu
Summary: DeepResolution2 is a novel approach for solving the co-eluting problem in GC-MS data. It utilizes deep neural networks to segment the profile, estimate the number of components, and predict elution regions, thereby assisting the multivariate curve resolution process. Compared to DeepResolution, DeepResolution2 is more efficient and stable, requiring only seven models to analyze the entire untargeted GC-MS data.
Article
Chemistry, Analytical
Somaye Vali Zade, Hamid Abdollahi
Summary: Pattern recognition models establish the relationship between variables and object classes. Different algorithms are needed to account for variations in measured variables, object patterns, and relationship models. MCR-ALS method, which incorporates physical and chemical information, simplifies result interpretation. The efficiency of MCR-DA and PLS-DA methods were evaluated and compared for discriminating olive oil samples.
MICROCHEMICAL JOURNAL
(2023)
Article
Mechanics
Y. Zheng, G. Z. Wang, K. Wang, F. Z. Xuan, S. T. Tu
Summary: Considering the crack-tip constraint effect, a correlation between T0 and a unified constraint parameter Ad* has been investigated in this study. A linear T0-Ad* correlation equation has been established and validated by experimental data, showing good capability to predict the MC T0 for any cracked structures across a wide range of conditions.
ENGINEERING FRACTURE MECHANICS
(2021)
Article
Chemistry, Analytical
Alejandro C. Olivieri
Summary: The present tutorial aims to demonstrate the importance of applying constraints when processing second-order analytical data with MCR-ALS, and show how these constraints can reduce or eliminate the impact of rotational ambiguity. Additionally, it provides details on a newly developed method for estimating uncertainty in predicted analyte concentrations.
MICROCHEMICAL JOURNAL
(2022)
Article
Chemistry, Analytical
Silvia Mas Garcia, Maxime Ryckewaert, Florent Abdelghafour, Maxime Metz, Daniel Moura, Carole Feilhes, Fanny Prezman, Ryad Bendoula
Summary: This study proposes a method for detecting grapevine diseases using hyperspectral imaging, combining MCR-ALS and FDA for reliable data analysis. The MCR-ALS/FDA discrimination model achieved a high level of correct pixel discrimination rates, with only a few misclassified images. The strategy shows potential for detecting flavescence doree and other phytopathologies.
Article
Chemistry, Analytical
Alejandro C. Olivieri
Summary: Rotational ambiguity is a phenomenon in protocols using MCR-ALS that can lead to uncertainty in analyte concentration estimation, especially when unexpected constituents are present in unknown samples. Analytical chemists developing second-order multivariate calibration methods using MCR-ALS need to acknowledge and assess the impact of this potential source of uncertainty on estimated analyte concentrations. It is crucial to estimate and report rotational ambiguity uncertainties, regardless of their magnitude, in order to ensure the accuracy of analyte predictions.
ANALYTICA CHIMICA ACTA
(2021)
Article
Food Science & Technology
Antoine Laborde, Francesc Puig-Castellvi, Delphine Jouan-Rimbaud Bouveresse, Luc Eveleigh, Christophe Cordella, Benoit Jaillais
Summary: This study successfully detected peanut flour adulteration in chocolate powder using NIR hyperspectral imaging and chemometrics, with adulterated pixel detection rates ranging from 0% to 17% in mixed samples.
Article
Chemistry, Physical
A. M. Kutsyk, O. O. Ilchenko, V. V. Nikonova, V. V. Obukhovsky
Summary: The mixing dynamics of liquid diethyl ether and chloroform were studied using time-resolved Fourier-transform infrared absorption spectroscopy in ATR mode. The data were analyzed using 2D COS and MCR, showing the existence of different species in unbound and bound states. The concentration profiles obtained through MCR decomposition were in good agreement with theoretical profiles based on a theory of nonlinear diffusion.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Automation & Control Systems
Marcie B. Wiggins, Mengyu Liu, Chang Liu, Karl S. Booksh
Summary: By employing Raman imaging spectroscopy and MCR-ALS, researchers were able to distinguish the polymorphs of basic copper chlorides in Chinese architectural paintings, identifying mixtures of atacamite and botallackite as well as the mineral azurite in different samples. This suggests a potential shift towards synthetic basic copper chloride pigments in Chinese architectural paints based on spectroscopic analysis.
JOURNAL OF CHEMOMETRICS
(2021)
Article
Pharmacology & Pharmacy
Benoit Igne, Caitlin N. Baldasano, Christian Airiau
Summary: Light-induced fluorescence has shown remarkable accuracy as a process analytical tool for monitoring low-dose pharmaceutical formulations, with modeling errors of 1.1% and lower observed. However, robustness improvements and method validation are still needed for wider manufacturing deployment.
JOURNAL OF PHARMACEUTICAL INNOVATION
(2021)
Review
Chemistry, Analytical
Anna de Juan, Roma Tauler
Summary: Multivariate Curve Resolution (MCR) is an algorithm designed to address the mixture analysis problem by expressing the original data through a bilinear model of pure component contributions. Since its inception in 1971, MCR methods have evolved to adapt to diverse scientific scenarios, incorporating new modeling tasks and mathematical properties. The continuous adaptation and application of MCR to new measurements and domains make it a mature yet lively methodology with potential for further advancement.
ANALYTICA CHIMICA ACTA
(2021)
Article
Automation & Control Systems
Miriam Perez-Cova, Carmen Bedia, Dwight R. Stoll, Roma Tauler, Joaquim Jaumot
Summary: Mass spectrometry is a preferred method in analytical field due to its sensitivity and selectivity in retrieving structural information for compound identification. The complexity of mass spectrometry datasets has led to the development of various computational approaches for pre-processing. The MSroi software aims to provide a comprehensive solution for compression and pre-processing of mass spectrometry datasets, allowing analysis of various types of datasets obtained through different acquisition approaches.
CHEMOMETRICS AND INTELLIGENT LABORATORY SYSTEMS
(2021)
Article
Chemistry, Analytical
Alessandro Nardecchia, Anna de Juan, Vincent Motto-Ros, Michael Gaft, Ludovic Duponchel
Summary: Laser-induced breakdown spectroscopy (LIBS) imaging is an innovative technique that utilizes powerful pulse lasers and chemometric analysis to capture atomic, ionic, and molecular emission signals in samples, but the complex data processing requires compression and fusion to achieve fast and reliable signal unmixing.
ANALYTICA CHIMICA ACTA
(2022)
Article
Biotechnology & Applied Microbiology
Suyang Wu, Stephanie A. Ketcham, Claudia C. Corredor, Douglas Both, James K. Drennen, Carl A. Anderson
Summary: Cell death is a common failure mode in mammalian cell culture, and apoptosis is the main death process observed. Detecting apoptosis in a timely manner is crucial for preventive control and product quality. This study presents a quantification model using capacitance spectroscopy to measure the percentage of apoptotic cells in an at-line setup, which offers a rapid, simple, and less labor-intensive alternative to traditional methods.
BIOTECHNOLOGY AND BIOENGINEERING
(2022)
Review
Biotechnology & Applied Microbiology
Adam J. Rish, James K. Drennen, Carl A. Anderson
Summary: Extensive knowledge of CHO cell metabolism is crucial for enhancing manufacturing productivity. The metabolism of CHO cells typically involves three stages: exponential growth, stationary, and death. Understanding these metabolic changes can lead to improvements in culture quality through identifying sources of toxicity and potential pathways for genetic engineering.
BIOTECHNOLOGY PROGRESS
(2022)
Article
Pharmacology & Pharmacy
Natasha L. Velez, James K. Drennen, Carl A. Anderson
Summary: This article reviews the applications of near infrared spectroscopy (NIR) for powder blend monitoring in the continuous manufacturing of solid oral dosage forms. It focuses on the challenges faced by NIR methods in monitoring blend uniformity, as well as the opportunities for optimization and recent advances in effective sample size measurement, probe location, and method robustness.
INTERNATIONAL JOURNAL OF PHARMACEUTICS
(2022)
Article
Biochemistry & Molecular Biology
Miriam Perez-Cova, Stefan Platikanov, Dwight R. Stoll, Roma Tauler, Joaquim Jaumot
Summary: Our study evaluates the performance of three multivariate ANOVA-based methods in metabolomics research, comparing their differences and adaptability, and validating their effectiveness through experimental data sets generated by liquid chromatography coupled to mass spectrometry.
Article
Chemistry, Analytical
Miriam Perez-Cova, Stefan Platikanov, Roma Tauler, Joaquim Jaumot
Summary: This work compares three chemometrics-based approaches for quantification purposes using two-dimensional liquid chromatography (LCxLC-MS). The study focuses on quantifying amino acids in commercial drug mixtures. The main novelty of this work is the demonstration of the applicability of these approaches to LCxLC-MS datasets. The results show that similar quantification results can be achieved with all three approaches, but the most accurate quantification is obtained when using the MCR-ALS method with an area correlation constraint.
Article
Chemistry, Analytical
Miriam Perez-Cova, Roma Tauler, Joaquim Jaumot
Summary: Rice crops are susceptible to arsenic exposure due to their growing conditions. This study used LC-MS to investigate the effects of arsenic on the lipidome and metabolome of rice in the early stages of growth. The results identified potential markers of arsenic exposure and showed significant metabolic alterations.
Article
Chemistry, Medicinal
Lauren Fontana, Carl Anderson, Robin Bogner, Michael Pikal
Summary: Raman scattering is a promising routine tool for detecting secondary and smaller tertiary structural changes in both solutions and solids before aggregation. A new method utilizing principal component analysis (PCA) of Raman spectra successfully detected pH-induced changes in protein structure linked to aggregate formation. The long-term goal is to explore Raman characterization as a routine monitoring tool for protein stability in both solution and solid states.
JOURNAL OF PHARMACEUTICAL SCIENCES
(2023)
Article
Chemistry, Analytical
Adrian Gomez-Sanchez, Raffaele Vitale, Olivier Devos, Anna de Juan, Cyril Ruckebusch
Summary: The unmixing of multiexponential decay signals into monoexponential components is a challenging task due to strong correlation and complete window overlap. Slicing methodologies, such as PowerSlicing, decompose the original data matrix into a three-way data array to provide unique solutions. However, when few sampling points are available, a degradation in accuracy and precision of the recovered profiles can be observed. In this work, a new methodology called Kernelizing is proposed to tensorize data matrices of multiexponential decays more efficiently, resulting in more accurate trilinear model estimates.
ANALYTICA CHIMICA ACTA
(2023)
Article
Automation & Control Systems
Albert Menendez-Pedriza, Laia Navarro-Martin, Joaquim Jaumot
Summary: This study evaluated the efficacy of MCR-ALS in analyzing mid-level fused data and combined it with JIVE for the evaluation of multi-omic data in ecotoxicology. The results showed that the combination of JIVE and MCR-ALS provided a more accurate interpretation of toxicological data.
CHEMOMETRICS AND INTELLIGENT LABORATORY SYSTEMS
(2023)
Article
Pharmacology & Pharmacy
Natasha L. Velez-Silva, James K. Drennen III, Carl A. Anderson
Summary: This study focuses on assessing the impact of powder physical variation on near-infrared (NIR) spectroscopy and develops an in-line characterization method for powder stream density in a simulated continuous system. The results demonstrate that powder density is a significant source of spectral variability due to flow rate. This study is important for facilitating continuous process scale-up and ensuring the robustness of analytical models.
INTERNATIONAL JOURNAL OF PHARMACEUTICS
(2023)
Article
Automation & Control Systems
Adam J. Rish, Natasha L. Velez-Silva, Samuel Henson, Md. Nahid Hasan, James K. Drennen, Carl A. Anderson
Summary: The use of calibration-free or minimal calibration chemometric modeling approaches has gained attention in the pharmaceutical industry as process analytical technologies expand. This study proposes a new diagnostic called NAS-T, which compares the shape of net analyte signals (NAS) between pure components and sample mixtures, to identify outliers in near-infrared spectral samples. The results support the adoption of pure component models for PAT applications in the pharmaceutical industry.
CHEMOMETRICS AND INTELLIGENT LABORATORY SYSTEMS
(2023)
Article
Chemistry, Analytical
Qian Wu, Li Tian, Xiangyu Shan, Huiling Li, Chao Li, Juan Lu
Summary: A novel ECL sensor was developed by modifying Fe3CuO4-Ru(bpy)3+ and GO-CdS@ZnS on the electrode for the detection of permethrin. The sensor exhibited high sensitivity and a wide detection range.
Article
Chemistry, Analytical
Tingting Gong, Lei Liao, Bingying Jiang, Ruo Yuan, Yun Xiang
Summary: In this study, a fluorescent biosensing system for high sensitivity detection of MT was established using a new Ag+-stabilized DNA triplex probe (Ag+-SDTP) combined with catalytic hairpin assembly (CHA) and CRISPR/Cas12a signal enhancements. The sensing method is able to selectively detect MT from other non-specific molecules and can achieve low level detection of MT in diluted human serums, demonstrating its potential for monitoring disease-specific MT biomarker at trace levels.
Article
Chemistry, Analytical
Estrella Sanz Rodriguez, Kyra Wood, Paul R. Haddad, Brett Paull
Summary: This study presents a simple, rapid, and reliable method for determining boron in aqueous solutions using suppressed ion chromatography coupled to electrospray ionisation-triple quadrupole mass spectrometry. The method achieved a low limit of detection and demonstrated excellent analytical performance.
Article
Chemistry, Analytical
Aline Cournut, Paul Moustiez, Yannick Coffinier, Christine Enjalbal, Claudia Bich
Summary: Alzheimer's disease is a major cause of senile dementia and is characterized by the aggregation of neurofibrillary tangles and amyloid plaques in the brain. The A beta 1-42 peptide is considered the primary cause of neurotoxicity due to its insolubility and subsequent aggregation. A beta 1-42 and A beta 1-40 have been identified as relevant biomarkers for AD diagnosis, and SurfaceAssisted Laser Desorption/Ionization Mass Spectrometry (SALDI-MS) was used to monitor the A beta 1-42/A beta 1-40 ratio without prior sample treatment.
Article
Chemistry, Analytical
Dotse Selali Chormey, Buse Tugba Zaman, Tulay Borahan Kustanto, Sezin Erarpat Bodur, Suleyman Bodur, Elif Ozturk Er, Sezgin Bakirdere
Summary: This review provides an overview of the harmful effects of endocrine disrupting chemicals (EDCs) on human health and introduces the methods for analyzing EDCs. Recent research has focused on using green chemicals, such as deep eutectic solvents (DESs), for microextraction to ensure environmental safety.
Article
Chemistry, Analytical
Yan Zhang, Renfeng Xu, Jingjing Wu, Zhenghong Zhang, Yuhuang Wang, Hongqin Yang, Sheng Zhang
Summary: This study visualized the pore-like structures in prostate cancer cell membranes after treatment with the anticancer drug paclitaxel, demonstrating its mechanism of action related to oxidative damage.
Article
Chemistry, Analytical
Chihong Ma, Qin Zhou, Jinjin Shi, Hua Gao, Di Huang, Huimin Xue, Han Wang, Zhenzhong Zhang, Sen Yang, Junli Zhang, Kaixiang Zhang
Summary: We developed a CRISPR-empowered electrochemical biosensor, named PER-E-CRISPR, for amplification-free and sensitive detection of miR-21. The biosensor combines the advantages of CRISPR/Cas13a and primer exchange reaction (PER) for target amplification. Under optimized conditions, the PER-E-CRISPR assay exhibits a linear range from 10-13 to 10-7 M and a limit of detection of 30.2 fM. The biosensor shows excellent performance in actual plasma, indicating promising prospects for miRNA detection in molecular diagnosis.
Article
Chemistry, Analytical
Gang Liang, Jie Zhao, Yufei Gao, Tao Xie, Jianhui Zhen, Ligang Pan, Wenwen Gong
Summary: Molecular docking (MD) analysis is widely used for studying the interaction between aptamers and small molecules. This study established steady-state aptamers of tertiary structures (SATS) using specific aptamers of tetracycline antibiotics as docking models. Molecular docking results revealed multiple binding sites in the SATS of aptamers, with significant variations in binding free energy (BFE) and docking score (DS). The study also proposed a method for MD analysis based on SATS, providing insights into binding mode and predicting binding sites.
Article
Chemistry, Analytical
Yixuan Xu, Changchang Teng, Huiping Dang, Dalong Yin, Lifeng Yan
Summary: Stable organic radical molecules with high NIR fluorescence quantum efficiency have been synthesized and encapsulated into nanoparticles, which show great potential for both photodynamic therapy (PDT) and photothermal therapy (PTT) of tumors.
Article
Chemistry, Analytical
Yu Su, Dandan Yang, Yanjie Wang, Jie Ding, Lan Ding, Daqian Song
Summary: In this study, a highly selective molecularly imprinted polymer Cu-MIPs@CS was designed and synthesized for bisphenol A (BPA). Cu-MIPs@CS showed significantly enhanced imprinting factor and selective factor towards BPA compared to MIPs@CS. It also exhibited superior discrimination ability between BPA and its structural analogue. Additionally, Cu-MIPs@CS were successfully applied as a solid phase extraction adsorbent for the determination of BPA in drinking water samples.
Article
Chemistry, Analytical
Yi Qiao, Qiongdan Zhang, Yukun He, Tianguang Cheng, Jing Tu
Summary: Single cell heterogeneity plays an important role in many biological phenomena, and distinguishing cells with specific mutations is beneficial for clinical diagnosis and drug screening. This study introduces a gel plate platform that can distinguish cell types based on their phenotypes, with low equipment requirement. The gel platform has potential in point-of-care circumstances and single-cell stimulation responses that prioritize efficiency and simplicity.
Article
Chemistry, Analytical
Chengke Wang, Shuyang Sun, Ping Wang, Huawei Zhao, Wenling Li
Summary: The food safety of aquatic products is a global concern. Nanotechnology-based analyses have advantages in the detection of bacteria, metal ions, and small molecule contaminants. This review summarizes the recent advances in biosensing strategies for aquatic products and highlights the application of nanomaterials, lateral flow-based biosensors, surface-enhanced Raman scattering, microfluidic chips, and molecular imprinting technologies.
Article
Chemistry, Analytical
Liping Zhu, Zeng Tang, Xuemei Zhang, Li Zhu, Tian Meng, Linying Yu, Ting Xiao, Shasha Lu, Xiaoli Xiong, Xiurong Yang
Summary: A sensitive off-on electrochemiluminescence DNA sensor was developed using Exo III-assisted cascade amplification system. The sensor achieved high selectivity and ultra-high sensitivity in detecting target DNA by utilizing ECL and SPR effects. This study provides a new perspective for designing highly sensitive and programmable ECL biosensors.
Article
Chemistry, Analytical
Tong Li, Mengxu Sun, Suping Xia, Ting Huang, Rong-Tian Li, Chunrong Li, Zong Dai, Jin-Xiang Chen, Jun Chen, Nuan Jia
Summary: Here, we developed a binary system based on DNA tetrahedron and fluorogenic RNA aptamers for highly specific and label-free mRNA imaging in living cells. This system achieved high specificity label-free detection of nucleic acids with a detection limit of 1.34 nM. The method has potential applications in early disease diagnosis and new drug development.
Article
Chemistry, Analytical
Yao Zhao, Shu Zhang, Wang Yao, Yuxuan Zhu, Jing Qian, Juan Yang, Nianjun Yang
Summary: A new hierarchical nanostructured composite with high conductivity and catalytic activity is synthesized. The sensor exhibits significant catalytic effect and high sensitivity for monitoring the environmental endocrine disruptor bisphenol A (BPA).