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Performance and kinetics of silicon-bridged diphosphines/CrCl3(C4H8O)3/modified methylaluminoxane catalyzed ethylene tri-/tetramerization in a continuous stirred tank reactor

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Abstract

In this study, PNSiP, a silicon-bridged diphosphines ligand, was coupled with CrCl3(THF)3 and modified methylaluminoxane (MMAO) to form a catalytic system. The continuous ethylene tri-/tetramerization catalytic performance of the PNSiP/CrCl3(THF)3/MMAO system was evaluated with a self-designed continuous stirred tank reactor (CSTR). The products have more than 88.00% selectivity for 1-hexene and 1-octene. Cyclic-C6 by-products (methyl-cyclopentane and methylene-cyclopentane) have a selectivity of less than 1.00%. The optimal process parameters for continuous ethylene tri-/tetramerization in CSTR were 60 °C reaction temperature, 5.0 MPa ethylene pressure, 1.2 mL/min catalyst feed flow rate, and 200 r/min impeller speed. The catalytic activity of the system can reach 7.26 × 105 g(products) g(Cr)−1 h−1. The mass fraction of polyethylene is less than 0.15% after 30 h. Finally, a kinetic model was established to describe the effects of chromium concentration and ethylene pressure on the continuous reaction of PNSiP/CrCl3(THF)3/MMAO catalyzed ethylene tri-/tetramerization in CSTR under the optimum conditions. This paper provides data basis and preliminary preparation for the continuous industrial production of linear α-olefins.

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Acknowledgements

This research was sponsored by the financial support from the National Natural Science Foundation of China (NSFC) (Grant Nos. 22071178, 22050410271), the Natural Science Foundation of Hebei Province of China (Grant No. B2019109045), China Petroleum Science and technology program (Grant No. 2020B-2512) and PetroChina Innovation Foundation (Grant No. 2020D-5007-0405).

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Author notes

  1. Xun Wang and Yating Wang have contributed equally to this work.

Authors and Affiliations

  1. College of Chemical Engineering and Material Science, Tianjin University of Science and Technology, Tianjin, 300457, China

    Xun Wang, Yating Wang, Jing Ma, Qihuan He, Huaiqi Shao, Yongrui Li, Jingyi Zhang, Qian Zhang, Qian Liu & Tao Jiang

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  1. Xun Wang
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  2. Yating Wang
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  3. Jing Ma
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Correspondence to Tao Jiang.

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Wang, X., Wang, Y., Ma, J. et al. Performance and kinetics of silicon-bridged diphosphines/CrCl3(C4H8O)3/modified methylaluminoxane catalyzed ethylene tri-/tetramerization in a continuous stirred tank reactor. Reac Kinet Mech Cat 135, 2441–2455 (2022). https://doi.org/10.1007/s11144-022-02255-1

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