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Isophthalonitrile (IPN) hydrogenation over K modified Ni-Co supported catalysts: catalyst characterization and performance evaluation

机译:K改性Ni-Co负载催化剂上的间苯二甲腈(IPN)加氢:催化剂表征和性能评估

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The hydrogenation of isophthalonitrile (IPN) to meta-xylylenediamine (m-XDA) is usually catalyzed by the Raney or supported Ni based catalysts in the presence of basic additive. Although the supported catalysts are safer than the Raney Ni catalysts, they have lower selectivity to m-XDA. This work revealed that the acid sites of NiCo/Al2O3 were responsible for the condensation reactions between amines and imines, which were the dominant side reactions. Besides the original acid sites on gamma-Al2O3, the loading of Ni-Co introduced new acid sites, which had a greater contribution to the condensation reactions. The K modification significantly enhanced the selectivity to m-XDA by reducing the two kinds of acid sites. Due to the formation mechanism of new acid sites and the K modification mechanism on these sites, both the K loading and K impregnation sequence affected the catalytic performance. When 3.0 wt% K was introduced to NiCo/Al2O3 by co-impregnation (3KNiCo/Al2O3), the catalyst acidity decreased by 82%, and the selectivity to m-XDA increased from 45.5% to 99.9%. The superiority of the optimized catalyst 3KNiCo/Al2O3 was also confirmed when no basic additive was used.
机译:间苯二甲腈(IPN)氢化为间苯二甲二胺(m-XDA)通常是在碱性添加剂存在下,由阮内或负载型镍基催化剂催化的。尽管负载的催化剂比阮内镍催化剂更安全,但它们对间-XDA的选择性较低。这项工作表明,NiCo / Al2O3的酸性位点是胺和亚胺之间的缩合反应的主要反应。除了γ-Al2O3上的原始酸位,Ni-Co的负载还引入了新的酸位,这对缩合反应有更大的贡献。 K修饰通过减少两种酸位显着提高了对m-XDA的选择性。由于新的酸位的形成机理和这些位上的K修饰机理,K的负载量和K的浸渍顺序都影响了催化性能。当通过共浸渍(3KNiCo / Al2O3)将3.0wt%的K引入NiCo / Al2O3中时,催化剂酸度降低了82%,对m-XDA的选择性从45.5%增加到99.9%。当不使用碱性添加剂时,也证实了优化催化剂3KNiCo / Al2O3的优越性。

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