A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications

Wang, Shanmin; Ge, Hui; Sun, Shouli; Zhang, Jianzhong; Liu, Fangming; Wen, Xiaodong; Yu, Xiaohui; Wang, Liping; Zhang, Yi; Xu, Hongwu; Neuefeind, Joerg C.; Qin, Zhangfeng; Chen, Changfeng; Jin, Changqin; Li, Yongwang; He, Duanwei; Zhao, Yusheng

doi:10.1021/jacs.5b01446

Title: A new molybdenum nitride catalyst with rhombohedral MoS₂ structure for hydrogenation applications

Journal Article · Mon Mar 23 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b01446· OSTI ID:1332528

Wang, Shanmin ^[1]; Ge, Hui ^[2]; Sun, Shouli ^[3]; Zhang, Jianzhong ^[4]; Liu, Fangming ^[5]; Wen, Xiaodong ^[6]; Yu, Xiaohui ^[7]; Wang, Liping ^[8]; Zhang, Yi ^[8]; Xu, Hongwu ^[4]; Neuefeind, Joerg C. ^[9]; Qin, Zhangfeng ^[2]; Chen, Changfeng ^[8]; Jin, Changqin ^[10]; Li, Yongwang ^[6]; He, Duanwei ^[5]; Zhao, Yusheng ^[11]

Univ. of Nevada, Las Vegas, NV (United States); Sichuan Univ., Chengdu (China); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Chinese Academy of Sciences (CAS), Shanxi (China)
National Institute of Clean- & Low-Carbon Energy (NICE), Beijing (China)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sichuan Univ., Chengdu (China)
Chinese Academy of Sciences (CAS), Shanxi (China); Synfuels China, Beijing (China)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Univ. of Nevada, Las Vegas, NV (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Chinese Academy of Sciences (CAS), Beijing (China)
Univ. of Nevada, Las Vegas, NV (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences (CAS), Beijing (China)

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. Further, 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.

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Research Organization:: Univ. of Nevada, Las Vegas, NV (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: NA0001982; AC05-00OR22725; FC52-06NA27684; AC52-06NA25396; XDA07020400

OSTI ID:: 1332528

Alternate ID(s):: OSTI ID: 1261429

Journal Information:: Journal of the American Chemical Society, Vol. 137, Issue 14; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 169 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
molybdenum nitride
MoN2
high-pressure synthesis
catalyst
hydrodesulfurization
sour mathanation

Title: A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications

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Title: A new molybdenum nitride catalyst with rhombohedral MoS₂ structure for hydrogenation applications