(FENXI HUAXUE) Chinese Journal of Analytical Chemistry. Boosting

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42 (FENXI HUAXUE) 11 2014 11 Chinese Journal of Analytical Chemistry 1679~ 1686 10.11895 / j.issn.0253-3820.140465 Bagging Boosting * * 100102 Near infrared spectroscopy NIR NIR Bagging Bagging-PLS Boosting Boosting-PLS Partial Least Squares PLS Synergy interval partial least squares sipls Competitive adaptive reweighted sampling CARS Bagging-PLS Boosting-PLS 10 PLS sipls 820 ~ 1029.5 nm 1030~ 1239.5 nm 820 ~ 959.5 960 ~ 1099.5 nm CARS 5 10 RMSECV Bagging-PLS Boosting-PLS RMSEP 0.02~ 0.04 g /L 4% ~ 5% Baggning-PLS Boosting-PLS NIR Bagging Boosting 1 Near infrared spectroscopy NIR 1 2 MSPC 3 4 PCA-MBRSD NIR Lonicera japonica Partial least squares PLS PLS 5 NIR Bagging-PLS Boosting-PLS NIR Bagging Boosting Bagging Boosting PLS 6 NIR 2 2.1 7 HPLC 216 PLS Kennard-Stone K-S 144 72 2014-05-29 2014-07-24 No.81303218 No.20130013120006 * E-mail yjqiao@ 263.net wzs@ bucm.edu.cn

1680 42 Bagging-PLS Boosting-PLS K-S 400 ~ 2500 nm HPLC 1 2.2 Bagging Boosting 1 HPLC Bagging Bootstrap aggregating Table 1 Two batches statistics of HPLC reference value chlorogenic acid in ethanol precipitation process of Lonicera japonica Batch Minimum Maxium Average SD RSD % Bagging 1 1.57 3.01 2.28 0.37 0.2 2 1.48 2.92 2.24 0.373 0.2 HPLC g /L Notes Concentration unit of HPLC reference value g /L. Boosting Boosting Bagging Boosting Boosting T ω t i = 1 /M i = 1 2 M 1 M t = 1 2 T ⅰ~ ⅵ ⅰ t M ⅱ t M PLS h t ⅲ h t L t l = ^y t i - y i /max ^y t - y i i = 1 2 M 2 ^y t i t ⅳ t 珔 L t = M L t i ω t i 3 i = 1 ⅴ β t = 珔 L t / 1 - 珔 L t 4 0 ~ 1 ⅵ t +1 ωi = ω t i β 1- 珔 L t i 5 T 8 9 2.3 Bagging-PLS Boosting-PLS NIR Bagging-PLS Boosting-PLS NIR 10~ Bagging 12 13 Bagging 14 Boosting 15 NIR Bagging Boosting 16 Bagging-PLS Boosting-PLS 2.4 Matlab 7.10 MatlabWorks Inc. U.S. PLS PLS_Toolbox Eigenvector Research Inc. U.S. XDS Rapid Liquid Analyzer FOSS Unscrambler9.7 CAMO CARS http / /code.google.com /p /carspls / r RMSEP

11 Bagging Boosting 1681 500 1000 3 3.1 NIR 1 1 2000 ~ 2500 nm PLS r p R 2 cal R 2 val 2 3 2 3 PLS r p 0.92 ~ 0.97 PLS PLS K-S Bagging-PLS Boosting-PLS Bagging-PLS Boosting-PLS 500 Bagging-PLS Boosting-PLS 10 2 3 1000 r p RMSEP r p RMSEP Bagging-PLS Boosting-PLS NIR 4 1 Fig.1 A B NIR NIR spectra of ethanol precipitation process of Lonicera japonica A is the first batch and B is the second batch 2 PLS Table 2 Results of PLS models of ethanol precipitation process of Lonicera japonica in the first batch Pretreatment method Later factors Calibration set R 2 cal RMSEC Validation set R 2 cal RMSEC Raw 4 0.9667 0.0682 0.9643 0.0705 0.9342 Baseline 2 0.9364 0.0942 0.9196 0.1069 0.9547 SNV 4 0.9783 0.0550 0.9767 0.0569 0.9421 SNV+Baseline 4 0.9714 0.0611 0.9733 0.0631 0.9446 Baseline+SNV+Noise 3 0.9931 0.0311 0.9926 0.0231 0.9523 S-G 3 0.9661 0.0687 0.9637 0.0711 0.9341 S-G+Noise 2 0.9899 0.0375 0.9895 0.0382 0.9441 SNV+Noise 4 0.9848 0.0466 0.9837 0.0483 0.9432 ST 4 0.9582 0.0763 0.9554 0.0788 0.9647 SNV+ST 4 0.9563 0.0780 0.9523 0.0816 0.9717 Baseline+ST 2 0.9296 0.0991 0.9259 0.1016 0.9663 MSC 2 0.9439 0.0885 0.9138 0.1099 0.9543 Raw S-G Savitaky-Golay ST Kubelka-Munk SNV MSC Noise Raw Original spectrum S-G Savitaky-Golay ST Spectroscopic transformation absorbance to Kubelka-Munk transformation SNV Standard normal variate MSC Multiplicative scatter correction Noise Added noise RMSEC Root mean square error of calibration RMSECV Root mean square error of cross-validation. r p

1682 42 3 PLS Table 3 Results of PLS models of ethanol precipitation process of Lonicera japonica in the first batch Pretreatment method Later factors Calibration set R 2 cal RMSEC Validation set R 2 cal RMSEC Raw 4 0.9693 0.0659 0.9663 0.0691 0.9234 Baseline 4 0.9749 0.0608 0.9718 0.0632 0.9415 SNV 3 0.9691 0.0662 0.9671 0.0683 0.9394 S-G 4 0.9691 0.0662 0.9660 0.0694 0.9236 SNV+Baseline 4 0.9750 0.0595 0.9732 0.0617 0.9347 Baseline+SNV+Noise 3 0.9963 0.0224 0.9962 0.0232 0.9495 SNV+Noise 3 0.9746 0.0600 0.9730 0.0619 0.9392 ST 4 0.9552 0.0797 0.9468 0.0869 0.9316 SNV+ST 4 0.9583 0.0769 0.9546 0.0803 0.9419 MSC 2 0.9439 0.0885 0.9138 0.1099 0.9543 Raw S-G Savitaky-Golay ST Kubelka-Munk SNV MSC Noise Raw Original spectrum S-G Savitaky-Golay ST Spectroscopic transformation absorbance to Kubelka-Munk transformation SNV Standard normal variate MSC Multiplicative scatter correction Noise Added noise. r p 2 Fig.2 NIR r p A B r p values for NIR models of ethanol precipitation process of Lonicera japonica A is the first batch B is the second batch 3 Fig.3 NIR RMSEP A B RMSEP values for NIR models of ethanol precipitation process of Lonicera japonica A is the first batch B is the second batch Bagging-PLS Boosting-PLS r p 0.93 ~ 0.95 RMSEP 0.12 500 3.2 3.2.1 sipls Synergy interval partial least squares sipls sipls Norgaard ipls 17 PLS 2 3 4

11 Bagging Boosting 1683 4 NIR Table 4 Prediction results of NIR models for two batches of ethanol precipitation process of Lonicera japonica Algorithm Bagging-PLS Boosting-PLS Batches of samples 1 2 1 2 Interation number r p r p mean RMSEP RMSEP mean 500 0.943 2 0.117 9 1000 0.942 8 0.118 5 500 0.938 9 0.118 2 1000 0.940 8 0.116 4 500 0.943 1 0.118 4 1000 0.942 8 0.118 8 500 0.938 3 0.118 0 1000 0.938 7 0.117 8 Root mean square error of cross-validation RMSECV NIR RMSECV RMSECV = n i = 1 槡 y NIRi -y Refi 2 n y NIRi PLS y Refi HPLC sipls 4 5 r NIR RMSECV 1 0 4 sipls Fig.4 Ethanol precipitation of Lonicera japonica in the first batch using synergy interval PLS sipls to select variables 5 sipls Fig.5 Ethanol precipitation of Lonicera japonica in the friest batch using synergy iterval PLS sipls to select variables

1684 42 3 4 820 ~ 1029.5 nm 1030 ~ 1239.5 nm 15 4 5 820 ~ 959.5 nm 960 ~ 1099.5 nm NIR 8 6 7 r p 2% ~ 4% RMSEP 0.02 ~ 0.04 g /L sipls 6 Fig.6 sipls NIR models results of ethanol precipitation of Lonicera japonica in the first batch after variables selection using sipls 7 Fig.7 sipls NIR models results of ethanol precipitation of Lonicera japonica in the second batch after variables selection using sipls 3.2.2 CARS CARS competitive adaptive reweighted sampling 18 19 RMSEP root mean square error of prediction 1000 5 10 290 261 5 Table 5 The models for two batches of ethanol precipitation of Lonicera japonica CARS-Bagging-PLS RMSEP r p CARS-Boosting-PLS Algorithms Batches Variable selection RMSEP mean r p mean 5 CARS Without selected 0.1189 0.9425 1 CARS 0.0723 0.9805 Bagging-PLS Without selected 0.1183 0.9391 2 CARS 0.0713 0.9817 r p Without selected 0.1191 0.9423 1 4 ~ 5 CARS 0.0727 0.9803 Boosting-PLS Without selected 0.1173 0.9391 2 CARS 0.0708 0.9821 0.98 CARS Competitive adaptive reweighted sampling RMSEP Root mean square error of prediction.

11 Bagging Boosting 1685 5 CARS r p RMSEP Bagging Boosting CARS r p RMSEP 4 Bagging-PLS Boosting-PLS PLS NIR Bagging-PLS Boosting-PLS Bagging- PLS Boosting-PLS NIR NIR References 1 LIU Shu-Hua ZHANG Xue-Gong ZHOU Qun SUN Su-Qin. Spectroscopy and Spectral Analysis 2006 26 4 629-632. 2006 26 4 629-632 2 WU Zhi-Sheng TAO Ou CHENG Wei YU Lu SHI Xin-Yuan QIAO Yan-Jiang. Chinese J. Anal. Chem. 2011 39 5 628-634. 2011 39 5 628-634 3 XU Bing SHI Xin-Yuan QIAO Yan-Jiang DU Min SUI Cheng-Lin LIU Qian. China Journal of Traditional Chinese Medicine and Pharmacy 2012 4 784-788. 2012 4 784-788 4 XU Bing LUO Gan LIN Zhao-Zhou AI Lu SHI Xin-Yuan QIAO Yan-Jiang. Chemical Journal of Chinese Universities 2013 34 10 2284-2289. 2013 34 10 2284-2289 5 Wu Z S Xu B Du M Sui C L Shi X Y Qiao Y J. Journal of Pharmaceutical and Biomedical Analysis 2012 62 1-6 6 CHENG Long WANG Gui-Zeng. Journal of Tsinghua University Science and Technology 2008 48 s2 1780-1784. 2008 48 s2 1780-1784 7 Wu Z S Du M Sui C L Shi X Y Qiao Y J. Analytical Methods 2012 4 4 1084-1088 8 Drucker H. Proceedings of the Fourteenth International Conference on Machine Learning 1997 9 Shao X Bian X Cai W. Analy. Chim. Acta 2010 666 1-2 32-37 10 ZHU Hong-Bin. Computer Applications and Software 2010 27 1 234-236. 2010 27 1 234-236 11 HE Ming LI Guo-Zheng YUAN Jie WU Geng-Feng. Journal of Shanghai University Natural Science Edition 2006 4 415. 2006 4 415 12 WANG Li ZHU Xue-Feng. Control Engineering of China 2009 16 1 59-61 79. 2009 16 1 59-61 79 13 Breiman L. Machine Learning. 1996 24 2 123-140 14 Zhang H Ishikawa M. International Congress Series 2007 1301 184-187 15 YU Ling WU Tie-Jun. Pattern Recognition and Artificial Intelligence 2004 17 1 52-59. 2004 17 1 52-59 16 CHU Xiao-Li XU Yu-Peng LU Wan-Zhen. Chinese J. Anal. Chem. 2008 36 5 702-709. 2008 36 5 702-709 17 Norgaard L Saudland A Wagner J Nielsen J P Munck L Engelsen S B. Applied Spectroscopy 2000 54 3 413-419

1686 42 18 Li H Liang Y Xu Q Cao D S. Anal. Chim. Acta 2009 648 1 77-84 19 LIN Zhao-Zhou SHI Xin-Yuan QIAO Yan-Jiang. World Science and Technology /Modernization of Traditional Chinese Medicine and MateriaMedica 2012 14 4 1760-1766. - 2012 14 4 1760-1766 A Study on Model Performance for Ethanol Precipitation Process of Lonicera japonica by NIR Based on Bagging-PLS and Boosting-PLS algorithm CHEN Zhao 1 2 WU Zhi-Sheng * 2 SHI Xin-Yuan 2 XU Bing 2 ZHAO Na 2 QIAO Yan-Jiang * 2 1 Fujian University of Traditional Chinese Medicine Fuzhou 350122 China 2 Research Center of TCM Information Engineering Beijing University of Chinese Medicine Beijing 100102 China Abstract To provide the methodology for rapid quality evaluation of Lonicera japonica we have established the stable quantitative model of near infrared spectroscopy NIR. The performance of Bagging partial least squares Bagging-PLS model and Boosting partial least squares Boosting-PLS model was compared with that partial least squares PLS model based on the NIR data of ethanol precipitation process of Lonicera japonica. On this basis the performance of these two models after variables selection was also studied by the methods of sipls synergy interval partial least squares and CARS competitive adaptive reweighted sampling. The experimental results showed that the prediction performance of Bagging-PLS and Boosting-PLS models was superior to PLS model with the latent factor of 10. The band of 820-1029. 5 nm and 1030-1239.5 nm for the first batch was selected by the method of sipls. In addition the band of 820-1029.5 nm and 1030-1239.5 nm was selected for the second batch sample in the same method.furthermore the method of CARS was taken to select variables for the two batches samples with 5-fold cross-validation and 10-fold cross-validation.and the lowest RMSECV root mean square error of cross-validation values were used to take subset.compared to the model performance without the method of CARS the RMSEP value of the Bagging- PLS model and Boosting-PLS model for the concentration of chlorogenic acid reduced by 0.02-0.04 g /L and r p correlation coefficient of prediction value increased by 4%-5%. Generally Bagging-PLS and Boosting-PLS could be regarded as rapid prediction methodsfor NIR quantitative models of ethanol precipitation process of Lonicera japonica. Keywords Process analysis technology Lonicera japonica Ethanol precipitation Bagging-partial least squares model Boosting-partial least squares moldel Received 29 May 2014 accepted 24 July 2014 This work was supported by the National Natural Science Foundation of China No. 81303218 and the Special Research Foundation for the Doctoral Program of Higher Education No. 20130013120006