六方氮化硼负载的Zn单原子催化剂吸附脱硫的理论研究

Theoretical Study on Aromatic Sulfide Adsorption on Zn Embedded h-BN Catalyst

柴油中芳香性硫化物的吸附脱除是降低硫含量、提高油品质量的重要工艺之一。采用密度泛函方法(B3LYP)计算了Zn在六方氮化硼(h-BN)完整表面及缺陷位V_(B)、V_(N)、V_(BN)的吸附,计算表明Zn在B缺陷位(V_(B))可形成热力学稳定的Zn/V_(B)单原子催化剂。考察了芳香性硫化物在h-BN及h-BN负载的Zn单原子催化剂上的吸附构型及吸附能。结果表明,芳香性硫化物在Zn/V_(B)的吸附与h-BN相比明显增强,电荷分析表明Zn增强了硫化物与h-BN表面的电荷转移。

The adsorptive desulfurization from diesel oil is one of the important processes to reduce sulfur content and improve oil quality.By using density functional theory,the adsorption of Zn on the complete surface of hexagonal boron nitride(h-BN)and defect sites V_(B),V_(N)and V_(BN)was calculated.The calculations showed that Zn on the B defect site(V_(B))could form a thermodynamically stable Zn/V_(B)single-atom catalyst.The adsorption configurations and adsorption energies of aromatic sulfides on h-BN and h-BN-supported Zn single-atom catalysts were investigated.The results showed that the adsorption of aromatic sulfides on Zn/V_(B)was significantly enhanced compared with h-BN,and the charge analysis indicated that Zn enhanced the charge transfer between sulfide and h-BN surface.