Enhanced phenanthrene hydrogenation saturation performance of Ni-Co/NiAlOX catalysts and its catalytic mechanism
Enhanced phenanthrene hydrogenation saturation performance of Ni-Co/NiAlOX catalysts and its catalytic mechanism
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DOI：
10.1016/j.fuproc.2023.107902
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发表时间：
2023
影响因子：
7.5
通讯作者：
Yu Chen;Zemin Zhao;Zeren Li;Jie-ying Jing;Wenying Li
中科院分区：
文献类型：
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作者：
Yu Chen;Zemin Zhao;Zeren Li;Jie-ying Jing;Wenying Li
菲的加氢饱和是获得高能量密度燃料的有效方法。要实现上述反应，设计高效稳定的加氢饱和催化剂是必不可少的。本文采用不同温度还原的方法合成了一系列Ni-Co/NiAlOx催化剂。活性评价结果表明，在5 6 0℃下还原的催化剂(Cat-5 6 0)在30 0℃、5℃压力下运行6h后，菲转化率为8.0mmol.g-1，活性组份·h−1，全氢菲选择性为98%。进一步研究发现，Cat-560具有较高的比活性(4.3mmol.kg−1·S−1)和TOF(41.10×10−3S−1)，比活性是520℃下还原催化剂的3倍，这与其特殊的几何结构和电子结构有关。表征结果表明，Ni-Co/NiAlOX催化剂中的Ni2+主要分布在镍铝尖晶石八面体位置，有利于镍的还原和较小镍粒子的形成。此外，还探索了Cat-560催化剂的负电荷密度为−0.12e，该密度适合菲和对称八氢菲的吸附和活化。
Hydrogenation saturation of phenanthrene was an effective method to acquire high energy density fuels. It is essential to design highly active and stable hydrogenation saturated catalyst to realize the above reaction. Herein, series of Ni-Co/NiAlOx catalysts were synthesized by reducing at different temperatures. Activity evaluation showed that the catalysts reduced at 560 °C (Cat-560) possessed a phenanthrene conversion amount of 8.0 mmol·g-1active component·h−1and 98% perhydrophenanthrene selectivity after running 6 h under 300 °C, 5 MPa. Furthermore, it was found that Cat-560 presented superior specific activity (4.3 mmol·kg−1·s−1) andTOF(41.1 × 10−3s−1) for symmetric octahydrophenanthrene hydrogenation (the rate determining reaction), and its specific activity was 3 times as high as that of the catalysts reduced at 520 °C The excellent hydrogenation performance of Cat-560 could be attributed to its special geometric and electronic structure. Characterization indicated that the Ni2+in Ni-Co/NiAlOXcatalyst was mainly located in the nickel aluminum spinel octahedral sites, which was beneficial to the reduction of Ni and the formation of smaller Ni particles. Moreover, it was explored that the Nidcharge density of Cat-560 catalyst was −0.12 e, which was suitable for the adsorption and activation of phenanthrene and symmetric octahydrophenanthrene.