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Title: A theoretical study on reaction mechanisms and kinetics of thiophene hydrodesulfurization over MoS 2 catalysts

In the present study, thiophene hydrodesulphurization (HDS) over the Mo-edge, the S-edge, and the Mo-S connection edge of MoS 2 catalyst with 50% sulfur coverage was studied using first-principles based microkinetic modeling. Two parallel HDS routes, i.e., direct desulfurization (DDS) and hydrogenation (HYD) were taken into account. It has been found that the major reaction route of thiophene HDS on the Mo- and the Mo-S edges is temperature dependent. In the low temperature range of 500–600 K, the HYD route is dominant, leading to the C 4H 8 formation. As the temperature increases, the DDS route becomes competitive with the HYD route. At the temperature above 650 K, the DDS route will be the dominant HDS reaction route on the Mo- and the Mo-S edges. The DDS route leading to the formation of C 4H 6 is the major thiophene HDS reaction route on the S-edge in the entire temperature range of 500–750 K. The microkinetic modeling results show the overall HDS activity on the S-edge is lower than it on the Mo- and the Mo-S edges. The Mo-S edge also provides a preferential reaction pathway, which facilitates 2-hydrothiophene migration from the Mo-edge to the S-edge, followed by remaining elementarymore » steps with lower activation barriers in the DDS route.« less
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [2] ;  [3]
  1. Beijing Univ. of Chemical Technology, Beijing (China)
  2. Beijing Univ. of Chemical Technology, Beijing (China); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-130462
Journal ID: ISSN 0920-5861; PII: S0920586118300646; TRN: US1801495
Grant/Contract Number:
91534201; 21476012; 21571012; 21407007; AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Name: Catalysis Today; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thiophene; Hydrodesulphurization; MoS2; DFT; Microkinetic modeling
OSTI Identifier:
1420437