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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Plastomeric-like polyethylenes achievable using thermally robust N,N '-nickel catalysts appended with electron withdrawing difluorobenzhydryl and nitro groups
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Plastomeric-like polyethylenes achievable using thermally robust N,N '-nickel catalysts appended with electron withdrawing difluorobenzhydryl and nitro groups

机译：使用热鲁棒N，N'-Nickel催化剂可实现的塑性化的聚乙烯，用电子取出二氟苯肼和硝基基团

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摘要

A new set of five unsymmetrical N, N'-diiminoacenaphthenes, 1-[2,6-{(4-FC6H4)(2)CH}2-4-NO2C6H4N]-2-(ArN) C2C10H6 (Ar = 2,6-Me2C6H3 L1, 2,6-Et2C6H3 L2, 2,6-iPr(2)C(6)H(3) L3, 2,4,6-Me3C6H2 L4, 2,6-Et-2-4-MeC6H2 L5), have been synthesized and used to prepare their corresponding nickel(II) halide complexes, LNiBr2 (Ni1-Ni5) and LNiCl2 (Ni6-Ni10). The molecular structures of Ni-3(OH2) and Ni4 reveal distorted square pyramidal and tetrahedral geometries, respectively, while the 1H NMR spectra of all the nickel(II) (S = 1) complexes show broad paramagnetically shifted peaks. Upon activation with either methylaluminoxane (MAO) or ethylaluminum sesquichloride (Et3Al2Cl2, EASC), Ni1-Ni10 displayed very high activities for ethylene polymerization with the optimal performance being observed using 2,6-dimethylcontaining Ni1 in combination with EASC (1.66 x 107 g PE mol(-1) (Ni) h-1 at 50 degrees C) which produced high molecular weight plastomeric polyethylene (Mw = 3.93 x 10(5) g mol(-1), Tm = 70.6 degrees C) with narrow dispersity (Mw/Mn = 2.97). Moreover, Ni1/EASC showed good thermal stability by operating effectively at an industrially relevant 80 degrees C with a level of activity (6.01 x 106 g of PE mol(-1) (Ni) h(-1)) that exceeds previously disclosed N, N'-nickel catalysts under comparable reaction conditions. This improved thermal stability and activity has been ascribed to the combined effects imparted by the para-nitro and fluoride-substituted benzhydryl ortho-substituents.
机译：一种新的五种非对称N，N'-DiIminoacenaphthenes，1- [2,6 - {（4-Fc6H4）（2）CH} 2-4-NO 2 C6H4N] -2-（ARN）C2C10H6（AR = 2,6 -ME2C6H3 L1,2,6-ET 2 C6H3 L2,2,6-IPR（2）C（6）H（3）L3，2,4,6-Me3C6H2 L4，2,6-ET-2-4-MEC6H2 L5 ）已经合成并用于制备它们相应的镍（II）卤化物配合物，LNIB1（Ni1-Ni5）和Lnic12（Ni6-Ni10）。 Ni-3（OH2）和Ni4的分子结构分别揭示了扭曲的方形锥体和四面体几何形状，而所有镍（II）（S = 1）配合物的1H NMR光谱显示出宽的顺式偏移峰。在用甲基铝氧烷（MAO）或乙基铝均辛醚（ET3Al 2Cl2，EASC）中，Ni1-Ni10显示出非常高的乙烯聚合活性，并使用2,6-二甲基Ni1与EASC组合使用2,6-二甲基Ni1（1.66×107g pe Mol（-1）（Ni）H-1在50℃），其产生高分子量塑性聚乙烯（MW = 3.93×10（5 )g mol（-1），Tm = 70.6℃），具有窄分散性（MW / mn = 2.97）。此外，Ni1 / Easc通过在工业相关的80℃下有效地运行，具有超过先前公开的N的行业相关的80℃（6.01×106g（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（ni）h（-1））的良好的热稳定性。 ，N'-镍催化剂在相当的反应条件下。这种改善的热稳定性和活性已经归因于由对硝基和氟化物取代的苯甲酸酯叔取代基赋予的组合效果。

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