Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene

doi:10.1016/j.cjche.2019.07.018

中国化学工程学报 ›› 2020, Vol. 28 ›› Issue (7): 1805-1808.DOI: 10.1016/j.cjche.2019.07.018

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene

Shuguang Xiang, Jiye Wang

Institute of Process Systems Engineering, Qingdao University of Science&Technology, Qingdao 266042, China

收稿日期:2018-12-17 修回日期:2019-06-02 出版日期:2020-07-28 发布日期:2020-08-31
通讯作者: Shuguang Xiang, Jiye Wang
基金资助:
Finacial support from the National Natural Science Foundation of China (21676139) is greatly acknowledged.

Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene

Shuguang Xiang, Jiye Wang

Institute of Process Systems Engineering, Qingdao University of Science&Technology, Qingdao 266042, China

Received:2018-12-17 Revised:2019-06-02 Online:2020-07-28 Published:2020-08-31
Contact: Shuguang Xiang, Jiye Wang
Supported by:
Finacial support from the National Natural Science Foundation of China (21676139) is greatly acknowledged.

摘要/Abstract

摘要： Based on the quantum chemical descriptors and the activities for isoprene polymerization of 12 neodymium carboxylates obtained by authors' earlier work, statistical analysis of data was made and a QSAR model correlating the quantum chemical descriptors and the activity was built with the partial least square (PLS) approach. The model is: A = 51602 ε_HOMO + 6 σ + 12546, which indicates that the catalytic activity A is positively correlated with the HOMO energy ε_HOMO and the ligand polarizability σ, with the contribution of σ being larger, ε_HOMO smaller. The model's coefficient of determination r² = 0.96 and that of cross validation q² = 0.94, both being close to 1, which means that its quality is well and its predictive power is strong. Analysis of the modeling process and the resulted QSAR model, together with the interpretation of the model's mechanism, also shows that the model obtained from this study is valid and reliable. According to the QSAR model, the mechanism of catalyst activity can be interpreted as that neodymium carboxylates with higher HOMO energy and larger ligand polarizability are easier to react with the co-catalysts so as to produce more active and stable centers of catalyst, resulting in a higher activity.

关键词: Neodymium carboxylate, QSAR modeling, Isoprene coordination polymerization, Catalyst

Abstract: Based on the quantum chemical descriptors and the activities for isoprene polymerization of 12 neodymium carboxylates obtained by authors' earlier work, statistical analysis of data was made and a QSAR model correlating the quantum chemical descriptors and the activity was built with the partial least square (PLS) approach. The model is: A = 51602 ε_HOMO + 6 σ + 12546, which indicates that the catalytic activity A is positively correlated with the HOMO energy ε_HOMO and the ligand polarizability σ, with the contribution of σ being larger, ε_HOMO smaller. The model's coefficient of determination r² = 0.96 and that of cross validation q² = 0.94, both being close to 1, which means that its quality is well and its predictive power is strong. Analysis of the modeling process and the resulted QSAR model, together with the interpretation of the model's mechanism, also shows that the model obtained from this study is valid and reliable. According to the QSAR model, the mechanism of catalyst activity can be interpreted as that neodymium carboxylates with higher HOMO energy and larger ligand polarizability are easier to react with the co-catalysts so as to produce more active and stable centers of catalyst, resulting in a higher activity.

Key words: Neodymium carboxylate, QSAR modeling, Isoprene coordination polymerization, Catalyst

Shuguang Xiang, Jiye Wang. Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene[J]. 中国化学工程学报, 2020, 28(7): 1805-1808.

Shuguang Xiang, Jiye Wang. Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene[J]. Chinese Journal of Chemical Engineering, 2020, 28(7): 1805-1808.

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Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene

Quantum chemical descriptors based QSAR modeling of neodymium carboxylate catalysts for coordination polymerization of isoprene

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