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First report of Schiff-base nickel nanoparticle-catalyzed oligomerization and polymerization of norbornene
Journal of Catalysis ( IF 6.5 ) Pub Date : 2021-11-16 , DOI: 10.1016/j.jcat.2021.11.008
Wilhelm H. le Roux 1 , Megan Matthews 1 , Albena Lederer 1, 2 , Albert J. van Reenen 1 , Rehana Malgas-Enus 1
Affiliation  

Ten novel Schiff-base functionalized nickel nano-systems were synthesized to investigate the capping ability of the ligands as well as the stability of the resulting nanoparticles. All four ligands employed were found to be capable and comparable stabilizers to produce monodispersed nanoparticles. These nanoparticles were further evaluated as catalysts in the polymerization of norbornene, using MAO or MMAO as a co-catalyst. All ten nanomaterials were active polymerization catalysts, resulting in the first ever reported nanoparticle-assisted polymerization processes. It was shown that the nano-catalyst can facilitate either oligomerization or polymerization depending on the co-catalyst employed. Other than vinyl polynorbornene, hydroxy functionalized oligomer stabilized nanocomposite products were also obtained. The oligomers could be cleaved from the nanoparticle surface, depending on its intended application. The vinyl polymers obtained gave high molecular weights and low polydispersity indices, whereas the hydroxy oligomers gave low molecular weight oligomers that were monodispersed. It was shown that the metal to ligand concentration, i.e. the extent of the nanoparticle surface stabilization, has little influence on the catalytic activity but rather influenced the polymer selectivity. A higher ligand to metal ratio resulted in higher molecular weight polymers with lower polydispersity indices compared to the lower metal to ligand ratio analogues. The effect of the type of ligand employed, is also investigated.



中文翻译:

席夫碱镍纳米粒子催化降冰片烯低聚聚合的首次报道

合成了十种新型席夫碱功能化镍纳米系统,以研究配体的封端能力以及所得纳米颗粒的稳定性。发现所用的所有四种配体都是能够和相当的稳定剂,以产生单分散的纳米粒子。这些纳米颗粒被进一步评估为降冰片烯聚合中的催化剂,使用 MAO 或 MMAO 作为助催化剂。所有十种纳米材料都是活性聚合催化​​剂,导致首次报道的纳米粒子辅助聚合过程。结果表明,根据所使用的助催化剂,纳米催化剂可以促进低聚或聚合。除了乙烯基聚降冰片烯之外,还获得了羟基官能化的低聚物稳定的纳米复合产品。根据其预期应用,低聚物可以从纳米颗粒表面裂解。获得的乙烯基聚合物具有高分子量和低多分散指数,而羟基低聚物产生单分散的低分子量低聚物。结果表明,金属与配体的浓度,即纳米颗粒表面稳定的程度,对催化活性几乎没有影响,而是影响了聚合物的选择性。与较低金属与配体比率的类似物相比,较高的配体与金属比率导致具有较低多分散指数的较高分子量聚合物。还研究了所用配体类型的影响。获得的乙烯基聚合物具有高分子量和低多分散指数,而羟基低聚物产生单分散的低分子量低聚物。结果表明,金属与配体的浓度,即纳米颗粒表面稳定的程度,对催化活性几乎没有影响,而是影响了聚合物的选择性。与较低金属与配体比率的类似物相比,较高的配体与金属比率导致具有较低多分散指数的较高分子量聚合物。还研究了所用配体类型的影响。获得的乙烯基聚合物具有高分子量和低多分散指数,而羟基低聚物产生单分散的低分子量低聚物。结果表明,金属与配体的浓度,即纳米颗粒表面稳定的程度,对催化活性几乎没有影响,而是影响了聚合物的选择性。与较低金属与配体比率的类似物相比,较高的配体与金属比率导致具有较低多分散指数的较高分子量聚合物。还研究了所用配体类型的影响。对催化活性影响不大,但对聚合物选择性有影响。与较低金属与配体比率的类似物相比,较高的配体与金属比率导致具有较低多分散指数的较高分子量聚合物。还研究了所用配体类型的影响。对催化活性影响不大,但对聚合物选择性有影响。与较低金属与配体比率的类似物相比,较高的配体与金属比率导致具有较低多分散指数的较高分子量聚合物。还研究了所用配体类型的影响。

更新日期:2021-11-17
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