A Bulky Pd(II) α-Diimine Catalyst Supported on Sulfated Zirconia for the Polymerization of Ethylene and Copolymerization of Ethylene and Methyl Acrylate,Organometallics

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A Bulky Pd(II) α-Diimine Catalyst Supported on Sulfated Zirconia for the Polymerization of Ethylene and Copolymerization of Ethylene and Methyl Acrylate
Organometallics ( IF 2.5 ) Pub Date : 2018-02-22 00:00:00 , DOI: 10.1021/acs.organomet.8b00016
Damien B. Culver ₁ , Hosein Tafazolian ₁ , Matthew P. Conley ₁

Affiliation

The reaction of (N∧N)PdMe₂ (N∧N is Ar–N═CMeMeC═N–Ar; Ar = 2,6-bis(diphenylmethyl)-4-methylbenzene) and sulfated zirconia (SZO) in diethyl ether forms organometallic Pd-sites that polymerize ethylene and copolymerize ethylene and methyl acrylate. The Pd-sites bind CO and were studied by infrared and solid-state NMR spectroscopies. Analysis of the reaction mixture shows that more methane than expected evolves during the grafting reaction, suggesting that some Pd-sites do not contain a Pd-Me group. Consistent with this observation, deuterium labeling experiments show that ∼9% of palladium sites are active in polymerization reactions. (N∧N)PdMe₂/SZO polymerizes ethylene with activity as high as 1342 kg_PE/(mol_active Pd*h) and incorporated up to 0.46% methyl acrylate in copolymerization reactions.

中文翻译：

硫化锆负载的大体积Pd（II）α-二胺催化剂用于乙烯的聚合以及乙烯和丙烯酸甲酯的共聚

（N∧N）PdMe ₂（N∧N为Ar–N═CMeMeC═N–Ar； Ar = 2,6-双（二苯基甲基）-4-甲基苯）与二氧化硫形式的硫酸化氧化锆（SZO）的反应聚合乙烯并使乙烯和丙烯酸甲酯共聚的有机金属Pd位。Pd位与CO结合，并通过红外和固态NMR光谱研究。对反应混合物的分析表明，在接枝反应过程中会产生比预期更多的甲烷，这表明某些Pd位不包含Pd-Me基团。与该观察结果一致，氘标记实验表明约9％的钯位点在聚合反应中具有活性。（N∧N）PdMe ₂ / SZO聚合乙烯，活性高达1342 kg _PE /（mol_活性Pd * h），并在共聚反应中加入最多0.46％的丙烯酸甲酯。

更新日期：2018-02-23

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