Copolymerization of Ethylene and Methyl Methacrylate with Salicylaldiminate Nickel(Ⅱ) Complexes†

doi:10.7503/cjcu20170256

Abstract

Abstract:

Four salicylaldiminate-based nickel(Ⅱ) complexes: bis[N-(2,6-diisopropylphenyl)salicylaldiminate]-nickel(Ⅱ)(C1), bis[N-(2,6-diisopropylphenyl)-3-methylsalicylaldiminate]-nickel(Ⅱ)(C2), bis[N-(2,6-diisopropylphenyl)-3-isopropylsalicylaldiminate]-nickel(Ⅱ)(C3) and [N-(2,6-diisopropyl-phenyl)-3-isopropylsalicylaldiminate]-nickel(Ph)(PPh₃)(C4), in the presence of methylaluminoxane(MAO), were applied in copolymerization of ethylene and methyl methacrylate(MMA). The influences of polymerization parameters, such as molar ratio of Al/Ni, polymerization temperature and time, on the copolymerization were studied with complex C3 as a model catalyst. Based on these results, the effect of the structure of the nickel complexes on the copolymerization was explored under optimized polymerization conditions. Complex C2 exhibits higher catalytic activity of 13.1 kg/(mol Ni·h) than C1 and C3, while C3 gives the lowest comonomer MMA incorporation of 14.1% in the obtained copolymers. For complexes C3 and C4, with the same ligand but different structures, C3 displays better catalytic activity than C4, but their comonomer MMA incorporations are similar. The microstructures and thermo-properties of the obtained copolymers were characterized by means of FTIR, ¹H NMR,¹³C NMR, GPC and DSC.

Key words: Salicylaldiminate-based nickel(Ⅱ) complex, Polyolefin, Copolymerization of ethylene and methyl methacrylate, Catalytic activity

CLC Number:

O631
O614.81

TrendMD:

ZHANG Danfeng, ZHANG Yujun, YU Guocong, GAO Wenhao. Copolymerization of Ethylene and Methyl Methacrylate with Salicylaldiminate Nickel(Ⅱ) Complexes^†[J]. Chem. J. Chinese Universities, 2017, 38(11): 2082.

Figures/Tables 7

References 36

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Entry	Cat.	Molar ratio of Al/Ni	t/h	T/℃	Activity/ (kg·mol^-1Ni·h^-1)	10^-4M_n	PDI	MMA Incorp. (%, molar fraction)	T_m/℃
1	C3	0	2	45
2	C3	100	2	45	6.2	2.6	2.4		112.0
3	C3	150	2	45	8.7	2.0	6.4	14.1	112.0
4	C3	200	2	45	6.5	2.1	6.0		122.0
5	C3	150	2	25	4.0	1.6	5.1		118.1
6	C3	150	2	65	3.3	1.6	3.9		119.1
7	C3	150	1	45	7.2				124.6
8	C3	150	4	45	4.5	2.4	4.0		107.5
9^b	C3	150	2	45	4.1	2.3	6.7		109.4
10	C1	150	2	45	6.3	2.1	6.2	60.4	118.5
11	C2	150	2	45	13.1	3.1	10.9	51.5	93.0
12	C4	150	2	45	3.7	2.3	3.3	12.6	119.1

Entry	Cat.	Molar ratio of Al/Ni	t/h	T/℃	Activity/ (kg·mol^-1Ni·h^-1)	10^-4M_n	PDI	MMA Incorp. (%, molar fraction)	T_m/℃
1	C3	0	2	45
2	C3	100	2	45	6.2	2.6	2.4		112.0
3	C3	150	2	45	8.7	2.0	6.4	14.1	112.0
4	C3	200	2	45	6.5	2.1	6.0		122.0
5	C3	150	2	25	4.0	1.6	5.1		118.1
6	C3	150	2	65	3.3	1.6	3.9		119.1
7	C3	150	1	45	7.2				124.6
8	C3	150	4	45	4.5	2.4	4.0		107.5
9^b	C3	150	2	45	4.1	2.3	6.7		109.4
10	C1	150	2	45	6.3	2.1	6.2	60.4	118.5
11	C2	150	2	45	13.1	3.1	10.9	51.5	93.0
12	C4	150	2	45	3.7	2.3	3.3	12.6	119.1