氢分子在超深度加氢脱硫催化剂上吸附与解离

 本文应用量子力学计算方法研究了氢分子在超深度脱硫催化剂上吸附解离的化学过程，考察了特定催化剂簇结构模型的不同位置上H2解离的催化活性，发现活性与反应位之间有一定关系，催化剂边位的活性较高；H2在几种不同加氢脱硫催化剂上的反应热及能垒计算结果显示了几种不同催化剂体系对H2吸附解离反应的催化活性不同；对助剂在H2解离活化反应中的间接、直接作用也进行了比较。

QUANTUM-MECHANICAL CALCULATION OF CHEMISORPTION AND ACTIVATION OF HYDROGEN ON ULTRA-DEEP HYDRODESULFURATION CATALYSTS

Molecular simulation based on density function theory was performed to investigate the chemisorption sites and activation process of H2 on several HDS catalyst systems,such as Mo-S,Co-Mo-S,Ni-Mo-S,Ni-W-S,W-S and Co-W-S.It was found that different reaction sites on catalyst possessed different catalytic activity among which those edge reaction sites possessed higher activity.Reaction heat and barrier energy of H2 activation on these catalyst systems mentioned above were calculated to study their activity for HDS catalysts and to compare the direct and indirect effects of promoters in process of H2 activation.The results showed that advantageous reaction sites of H2 activation on Ni-Mo-S and Ni-W-S catalysts tended to be the edge sites,while on Mo-S or Co-Mo-S catalyst,these advantageous reaction sites tended to be on(001) surfaces,and the indirect effects of promoters in process of H2 activation were more obvious than the direct effects.