Enhancing phenanthrene hydrogenation via controllable phosphate deposition over Ni2P/Al2O3 catalysts
Enhancing phenanthrene hydrogenation via controllable phosphate deposition over Ni2P/Al2O3 catalysts
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DOI：
10.1016/j.ces.2023.119251
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发表时间：
2023-09
影响因子：
4.7
通讯作者：
Jie-ying Jing;Zhongyuan Guo;Zeren Li;Yu Chen;Hao Li;Wen-Ying Li
中科院分区：
文献类型：
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作者：
Jie-ying Jing;Zhongyuan Guo;Zeren Li;Yu Chen;Hao Li;Wen-Ying Li
采用次亚磷酸分解法制备了具有磷酸盐沉积的Ni2P/ al2o3催化剂。Ni-2.5P/ al2o3催化剂由于其球形结构和表面沉积的磷酸盐的特殊电子性质，对菲（PHE）加氢具有显著的活性和稳定性，具有44.64 × 10-3s−1的高周转频率。广泛的表征表明，控制P/Ni摩尔比可以改变磷的迁移途径，影响生成的磷酸盐沉积量，进而影响Ni2P暴露的活性位点。密度泛函理论计算表明，沉积的磷酸盐可以诱导电子从Ni向磷酸盐转移，一定数量的磷酸盐沉积可以使Ni处于适当的缺电子状态，从而提高PHE的吸附，使PHE容易完全加氢。
Ni2P/Al2O3catalysts with phosphate deposition were synthesized by a hypophosphite decomposition method. Benefiting from its spherical structure and special electronic properties derived from the deposited phosphate on the catalyst surface, the Ni-2.5P/Al2O3catalyst offered remarkable activity and stability towards phenanthrene (PHE) hydrogenation, featuring a high turnover frequency of 44.64 × 10-3s−1. Extensive characterizations revealed that the control of P/Ni molar ratio could change the phosphorus migration pathway and affect the amount of the generated phosphate deposition and then the exposed active sites of Ni2P. Density functional theory computations indicated that the deposited phosphate could induce electron transfer from Ni to phosphate, and a certain amount of phosphate deposition can endow Ni with an appropriate electron-deficient state, which can improve the PHE adsorption and result in a facile complete PHE hydrogenation.