摘要：Using density functional theory (DFT) with numerical atomic functions including dispersion corrections, we establish a series of energy changes and Gibbs free energies of in situ and ex situ substitution by ammonia on Ni-Mo-S nanocluster, which includes Ni-Mo-Edge, Ni-S-Edge and Corner-Site. The results show that the in situ substitution on all active sites on Ni-Mo-S is hard to happen. The –SH group and hydrogen atom on coordinately unsaturated sites (CUS) of Ni-S-Edge can form H2S under a moderate condition, whereas the sulfur atoms on Ni-Mo-Edge are rather difficult to form H2S. The ex situ substitution of sulfur atoms on both Ni-S-Edge and Ni-Mo-Edge is energetically favored; however, the substitution may only occur on Ni-S-Edge under low partial pressure of ammonia based on the steady state of Ni-Mo-S active phase. The orbital properties show the eigenvalue has increased after substitution, which indicates the decreasing of binding electron capacity. Furthermore, the HDS performance would drop remarkably attributed to steric hindrance and lacking of activated hydrogen after substitution.
© 2019 Elsevier B.V.

ISSN号：0920-5861

卷、期、页：v 353,p17-25

发表日期：2020-08-15

影响因子：5.825000

期刊分区（SCI为中科院分区）：二区

收录情况：SCI（科学引文索引印刷版）,EI（工程索引）,SCIE（科学引文索引网络版）

发表期刊名称：Catalysis Today

通讯作者：刘晓东,周景明,魏阳阳,张鹏飞

第一作者：周亚松,魏强

论文类型：期刊论文

论文概要：刘晓东,周景明,周亚松,魏强,魏阳阳,张鹏飞，Substitution of Sulfur Atoms on Ni-Mo-S by Ammonia – A DFT Study，Catalysis Today，2020，v 353,p17-25

论文题目：Substitution of Sulfur Atoms on Ni-Mo-S by Ammonia – A DFT Study