title: Solving signal instability to maintain the second-order advantage in the resolution and determination of multi-analytes in complex systems by modeling liquid chromatography-mass spectrometry data using alternating trilinear decomposition method assisted with piecewise direct standardization.
abstract: The application of calibration transfer methods has been successful in combination with near-infrared spectroscopy or other tools for prediction of chemical composition. One of the developed methods that can provide accurate performances is the piecewise direct standardization (PDS) method, which in this paper is firstly applied to transfer from one day to another the second-order calibration model based on alternating trilinear decomposition (ATLD) method built for the interference-free resolution and determination of multi-analytes in complex systems by liquid chromatography-mass spectrometry (LC-MS) in full scan mode. This is an example of LC-MS analysis in which interferences have been found, making necessary the use of second-order calibration because of its capacity for modeling this phenomenon, which implies analytes of interest can be resolved and quantified even in the presence of overlapped peaks and unknown interferences. Once the second-order calibration model based on ATLD method was built, the calibration transfer was conducted to compensate for the signal instability of LC-MS instrument over time. This allows one to reduce the volume of the heavy works for complete recalibration which is necessary for later accurate determinations. The root-mean-square error of prediction (RMSEP) and average recovery were used to evaluate the performances of the proposed strategy. Results showed that the number of calibration samples used on the real LC-MS data was reduced by using the PDS method from 11 to 3 while producing comparable RMSEP values and recovery values that were statistically the same (F-test, 95% confidence level) to those obtained with 11 calibration samples. This methodology is in accordance with the highly recommended green analytical chemistry principles, since it can reduce the experimental efforts and cost with regard to the use of a new calibration model built in modified conditions.
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Hui-Wen
authors.initials: HW
authors.lastname: Gu
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China. Electronic address: hlwu@hnu.edu.cn.
authors.forename: Hai-Long
authors.initials: HL
authors.lastname: Wu
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Xiao-Li
authors.initials: XL
authors.lastname: Yin
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Shan-Shan
authors.initials: SS
authors.lastname: Li
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Ya-Juan
authors.initials: YJ
authors.lastname: Liu
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Hui
authors.initials: H
authors.lastname: Xia
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Li-Xia
authors.initials: LX
authors.lastname: Xie
authors.affiliation: State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China.
authors.forename: Ru-Qin
authors.initials: RQ
authors.lastname: Yu
authors.affiliation: Institutes of Biomedical Science and Department of Chemistry, Fudan University, Shanghai 200032, China. Electronic address: pyyang@fudan.edu.cn.
authors.forename: Peng-Yuan
authors.initials: PY
authors.lastname: Yang
authors.affiliation: Institutes of Biomedical Science and Department of Chemistry, Fudan University, Shanghai 200032, China.
authors.forename: Hao-Jie
authors.initials: HJ
authors.lastname: Lu
mesh_terms: D000465:Algorithms; D002138:Calibration; D002623:Chemistry Techniques, Analytical / Q000592:standards*; D002853:Chromatography, Liquid; D013058:Mass Spectrometry; D008956:Models, Chemical
keywords: Alternating trilinear decomposition method; Liquid chromatography–mass spectrometry; Piecewise direct standardization; Second-order advantage; Signal instability; Sulfonylurea-type oral antidiabetic agents