SCI和EI收录∣中国化工学会会刊

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   

  1. 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   

  1. 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: 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 εHOMO + 6 σ + 12546, which indicates that the catalytic activity A is positively correlated with the HOMO energy εHOMO and the ligand polarizability σ, with the contribution of σ being larger, εHOMO 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 εHOMO + 6 σ + 12546, which indicates that the catalytic activity A is positively correlated with the HOMO energy εHOMO and the ligand polarizability σ, with the contribution of σ being larger, εHOMO 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