氢分子在超深度加氢脱硫催化剂上吸附与解离的量子力学研究  

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

作　　者：李皓光[1] 赵晓光[1] 周涵[1] 聂红[1] 

机构地区：[1]中国石化石油化工科学研究院,北京100083

出　　处：《石油学报（石油加工）》2007年第1期51-57,共7页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家重点基础研究发展规划973项目(G2000048003)资助

摘　　要：应用密度函数计算方法研究了氢分子在超深度加氢脱硫催化剂体系(Mo-S,Co-Mo-S,Ni-Mo-S,Ni-W-S,W-S,Co-W-S)上吸附解离的化学过程,考察了在特定催化剂活性相结构模型的不同位置上H2解离的催化活性。结果表明,催化剂不同反应位上的催化活性不同,边位的催化活性较高。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它们对H2吸附解离反应的催化活性不同,在Ni-Mo-S和Ni-W-S催化剂上,边位的氢解活性高,而Mo-S、Co-Mo-S催化剂上(001)层面S原子的氢解活性高;比较了助剂在H2解离活化反应中的间接、直接作用,发现其间接作用大于直接作用。Molecular simulation based on density the chemisorption sites and activation process of function theory was performed to investigate H2 on several HDS catalyst systems, such as Mo-S, Co Mo-S, Ni-Mo-S, Ni WS, 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.

关 键 词：超深度加氢脱硫 催化剂 吸附 解离 密度函数 分子模拟 

分 类 号：TE624.9[石油与天然气工程—油气加工工程]