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Mixed oxides supported low-nickel formulations for the direct amination of aliphatic alcohols with ammonia
Journal of Catalysis ( IF 6.5 ) Pub Date : 2017-11-06 , DOI: 10.1016/j.jcat.2017.08.015
A. Tomer , Z. Yan , A. Ponchel , M. Pera-Titus

The present study focuses on the selective synthesis of primary amines from aliphatic alcohols and ammonia using alumina-ceria supported nickel formulations based on very low nickel loading (≤2 wt%) and without any additive or external H2 supply. The effect of the catalyst preparation methods and modes of nickel impregnation were studied in detail and comprehensively characterized. The best formulation afforded 80% n-octanol conversion with 78% selectivity to n-octylamine at optimized reaction conditions, which were far better than control catalysts and benchmark Ni-alumina formulations relying on high Ni loadings. The enhanced activities of the alumina-ceria supported nickel catalysts was attributed to three combined effects: (1) a higher reducibility of surface nickel oxide species, (2) the genesis of very small and homogeneously distributed nickel nanoparticles (2–3 nm), and (3) a strong decline in the formation of nickel aluminates. Furthermore, unlike benchmark Ni catalysts, these formulations afforded a higher resistance to leaching.



中文翻译:

混合氧化物支持的低镍配方,用于氨与脂肪醇的直接胺化

本研究的重点是使用基于氧化铝负载的镍的镍配方,基于极低的镍负载量(≤2 wt%),从脂肪醇和氨中选择性合成伯胺,而无需任何添加剂或外部H 2供给。详细研究了催化剂的制备方法和镍浸渍方式的影响,并进行了全面的表征。最佳配方可提供80%的辛醇转化率,对n的选择性为78%-辛胺在最佳反应条件下的性能远远优于对照催化剂和依靠高Ni负载量的基准Ni-氧化铝配方。氧化铝-二氧化铈负载的镍催化剂的活性增强归因于三个综合作用:(1)表面氧化镍物种的还原性更高;(2)很小且均匀分布的镍纳米颗粒(2-3 nm)的产生; (3)铝酸镍的形成急剧下降。此外,与基准镍催化剂不同,这些配方具有更高的耐浸出性。

更新日期:2017-11-06
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