Detailed DFT calculations of C₂H₂ hydrogenation on Pd₆, Pd₆⁺ and Pd₆B clusters were performed to explore the effect of interstitial B on the mechanisms of C₂H₂ hydrogenation catalyzed by Pd₆. The results show that the Pd₆B cluster has the lowest diffusion barriers of H atoms and dissociated barriers of H₂; the interstitial B atom can simultaneously improve both the activity and selectivity of C₂H₂ hydrogenation to C₂H₄ on Pd₆ cluster by altering the major product and the optimal pathway. Moreover, the higher charge is conducive to enhancing the adsorption of C₂H₂ and C₂H₄, rather than the selectivity of C₂H₄ formation. Our work provides some insight into the activity selectivity charge relationship of Pd-based catalysts in C₂H₂ selective hydrogenation.

进行了Dd ₆，Pd ₆ ⁺和Pd ₆ B团簇上C ₂ H ₂加氢的详细DFT计算，以探讨间隙B对Pd ₆催化C ₂ H ₂加氢机理的影响。结果表明，Pd ₆ B团簇具有最低的H原子扩散势垒和H _2的离解势垒; 间隙中的B原子可同时提高C ₂ H ₂加氢生成Pd ₆上C ₂ H ₄的活性和选择性通过改变主要产品和最佳途径来实现集群。此外，较高的电荷有利于增强C ₂ H ₂和C ₂ H ₄的吸附，而不是C ₂ H ₄形成的选择性。我们的工作为C ₂ H ₂选择性加氢中基于Pd的催化剂的活性选择性电荷关系提供了一些见识。