High Temperature Iron Ethylene Polymerization Catalysts Bearing <italic style="font-style: italic">N,N,N'</italic>-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

Chantsalnyam Bariashir; Qiu-Yue Zhang; Bayasgalan Ulambayar; Gregory A. Solan; Tong-Ling Liang; Wen-Hua Sun

doi:10.1007/s10118-023-3037-9

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High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

RESEARCH ARTICLE | Updated：2024-01-12

- High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines
  Enhanced Publication
- Chinese Journal of Polymer Science Vol. 42, Issue 2, Pages: 188-201(2024)
- Affiliations：
  
  a.Institute of Chemistry and Chemical Technology, Mongolian Academy of Sciences, Ulaanbaatar 13330, Mongolia
  b.Key Laboratory of Engineering Plastics and Beijing National Laboratory for Molecular Science, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
  c.Department of Chemistry, University of Leicester, University Road, Leicester LE1 7RH, UK
  d.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China
- Author bio：
  
  gas8@leicester.ac.uk (G.A.S.)
  whsun@iccas.ac.cn (W.H.S.)
- Funds：
- DOI：10.1007/s10118-023-3037-9
  CLC：
- Received：05 July 2023，
  
  Revised：2023-7-26，
  
  Accepted：27 July 2023，
  
  Online First：12 September 2023，
  
  Published：01 February 2024
- Accepted：
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Bariashir, C.; Zhang, Q. Y.; Ulambayar, B.; Solan, G. A.; Liang, T. L.; Sun, W. H. High temperature iron ethylene polymerization catalysts bearing N,N,N'-2-(1-(2,4-dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines. Chinese J. Polym. Sci. 2024, 42, 188–201

Chantsalnyam Bariashir, Qiu-Yue Zhang, Bayasgalan Ulambayar, et al. High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines[J]. Chinese Journal of Polymer Science, 2024, 42(2): 188-201. DOI: 10.1007/s10118-023-3037-9.
Bariashir, C.; Zhang, Q. Y.; Ulambayar, B.; Solan, G. A.; Liang, T. L.; Sun, W. H. High temperature iron ethylene polymerization catalysts bearing N,N,N'-2-(1-(2,4-dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines. Chinese J. Polym. Sci. 2024, 42, 188–201 DOI： 10.1007/s10118-023-3037-9.

Chantsalnyam Bariashir, Qiu-Yue Zhang, Bayasgalan Ulambayar, et al. High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines[J]. Chinese Journal of Polymer Science, 2024, 42(2): 188-201. DOI: 10.1007/s10118-023-3037-9. DOI：

摘要

The combined effect of an electron withdrawing fluoride and a sterically bulk benzhydryl group at the

ortho

-sites of one

-aryl group in the title iron precatalyst

allows for very high polymerization activity at an operating temperature of 80 oC.

Abstract

The

-ferrous chloride complexes

[2-{CMeN(2

4-(CHPh)

-6-FC

)}-6-(CMeNAr)C

N]FeCl

(Ar

6-Me

Fe1

6-Et

Fe2

Fe3

6-Me

Fe4

and 2

6-Et

-4-MeC

Fe5

)

each possessing one

-2

4-dibenzhydryl-6-fluorophenyl group

were readily synthesized from their respective unsymmetrical bis(imino)pyridines

–

. Structural identification of

Fe2

highlighted the variation in the steric properties provided by the dissimilar

-aryl groups. Following pre-treatment with either MAO or MMAO

complexes

Fe1

–

Fe5

all displayed

at an operating temperature of 80 °C

high activities for ethylene polymerization with levels falling in the order:

Fe4

Fe1

Fe5

Fe2

Fe3

. Notably

Fe4

/MAO displayed the highest activity of 1.94×10

·mol

−1

·h

−1

of the study with only a modest loss in performance at 90 °C. Generally

the resulting polyethylenes were highly linear (

range: 122–132 °C)

narrowly disperse and of low molecular weight (

range: 6.73−46.04 kg·mol

−1

)

with the most sterically hindered

Fe3

forming the highest molecular weight polymer of the series. End-group analysis by

H- and

C-NMR spectroscopy revealed saturated alkyl (

-propyl and

-propyl) and unsaturated vinyl chain ends indicative of the role of both

-H elimination and chain transfer to aluminum as termination pathways. By comparison with previously reported iron precatalysts with similar tridentate ligand skeletons

it is evident that the introduction of a large benzhydryl group in combination with a fluorine as the

ortho

-substituents of one

-aryl group has the effect of enhancing thermal stability of the iron polymerization catalyst whilst maintaining appreciable polymer molecular weight.

关键词

Keywords

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High Temperature Iron Ethylene Polymerization Catalysts Bearing N,N,N'-2-(1-(2,4-Dibenzhydryl-6-fluorophenylimino)ethyl)-6-(1-(arylphenylimino)ethyl)pyridines

DOI：10.1007/s10118-023-3037-9

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