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Title: A New Molybdenum Nitride Catalyst with Rhombohedral MoS2 Structure for Hydrogenation Applications

Nitrogen-rich transition-metal nitrides hold great promise to be the next-generation catalysts for clean and renewable energy applications. However, incorporation of nitrogen into the crystalline lattices of transition metals is thermodynamically unfavorable at atmospheric pressure; most of the known transition metal nitrides are nitrogen-deficient with molar ratios of N:metal less than a unity. In this work, we have formulated a high-pressure route for the synthesis of a nitrogen-rich molybdenum nitride through a solid-state ion-exchange reaction. The newly discovered nitride, 3R-MoN2, adopts a rhombohedral R3m structure, isotypic with MoS2. This new nitride exhibits catalytic activities that are three times more active than the traditional catalyst MoS2 for the hydrodesulfurization of dibenzothiophene and more than twice as high in the selectivity to hydrogenation. The nitride is also catalytically active in sour methanation of syngas with >80% CO and H2 conversion at 723 K. Lastly, our formulated route for the synthesis of 3R-MoN2 is at a moderate pressure of 3.5 GPa and, thus, is feasible for industrial-scale catalyst production.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7] ;  [8] ;  [8] ;  [4] ;  [9] ;  [2] ;  [8] ;  [10] ;  [6] ;  [5] ;  [11]
  1. Univ. of Nevada, Las Vegas, NV (United States). HiPSEC & Physics Dept.; Sichuan Univ., Chengdu (China). Inst. of Atomic & Molecular Physics; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Chinese Academy of Sciences (CAS), Taiyuan (China). Inst. of Coal Chemistry
  3. National Inst. of Clean- & Low-Carbon Energy (NICE), Beijing (China)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  5. Sichuan Univ., Chengdu (China). Inst. of Atomic & Molecular Physics
  6. Chinese Academy of Sciences (CAS), Taiyuan (China). Inst. of Coal Chemistry; Synfuels China, Beijing (China)
  7. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics
  8. Univ. of Nevada, Las Vegas, NV (United States). HiPSEC & Physics Dept.
  9. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  10. Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics
  11. Univ. of Nevada, Las Vegas, NV (United States). HiPSEC & Physics Dept.; Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Physics
Publication Date:
OSTI Identifier:
1261429
Grant/Contract Number:
AC05-00OR22725; FC52-06NA27684; 21473231; AC52- 6NA25396; XDA07020400
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 14; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation of China (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY