Direct copolymerization of ethylene with protic comonomers enabled by multinuclear Ni catalysts

Gang Ji, Zhou Chen, Xiao-Yan Wang, Xiao-Shan Ning, Chong-Jie Xu, Xing-Min Zhang, Wen-Jie Tao, Jun-Fang Li, Yanshan Gao, Qi Shen, Xiu-Li Sun (), Hao-Yang Wang, Jun-Bo Zhao, Bo Zhang, Yin-Long Guo (), Yanan Zhao, Jiajie Sun, Yi Luo () and Yong Tang ()
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Gang Ji: Chinese Academy of Sciences
Zhou Chen: Chinese Academy of Sciences
Xiao-Yan Wang: Chinese Academy of Sciences
Xiao-Shan Ning: Chinese Academy of Sciences
Chong-Jie Xu: Chinese Academy of Sciences
Xing-Min Zhang: Soochow University
Wen-Jie Tao: Chinese Academy of Sciences
Jun-Fang Li: Chinese Academy of Sciences
Yanshan Gao: Chinese Academy of Sciences
Qi Shen: Soochow University
Xiu-Li Sun: Chinese Academy of Sciences
Hao-Yang Wang: Chinese Academy of Sciences
Jun-Bo Zhao: Chinese Academy of Sciences
Bo Zhang: Chinese Academy of Sciences
Yin-Long Guo: Chinese Academy of Sciences
Yanan Zhao: Dalian University of Technology
Jiajie Sun: Dalian University of Technology
Yi Luo: Dalian University of Technology
Yong Tang: Chinese Academy of Sciences

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Ethylene/polar monomer coordination copolymerization offers an attractive way of making functionalized polyolefins. However, ethylene copolymerization with industrially relevant short chain length alkenoic acid remain a big challenge. Here we report the efficient direct copolymerization of ethylene with vinyl acetic acid by tetranuclear nickel complexes. The protic monomer can be extended to acrylic acid, allylacetic acid, ω-alkenoic acid, allyl alcohol, and homoallyl alcohol. Based on X-ray analysis of precatalysts, control experiments, solvent-assisted electrospray ionization-mass spectrometry detection of key catalytic intermediates, and density functional theory studies, we propose a possible mechanistic scenario that involves a distinctive vinyl acetic acid enchainment enabled by Ni···Ni synergistic effects. Inspired by the mechanistic insights, binuclear nickel catalysts are designed and proved much more efficient for the copolymerization of ethylene with vinyl acetic acid or acrylic acid, achieving the highest turnover frequencies so far for both ethylene and polar monomers simultaneously.

Date: 2021
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DOI: 10.1038/s41467-021-26470-x

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