A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- 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 Org.:
- USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1332528
- Alternate Identifier(s):
- OSTI ID: 1261429
- Grant/Contract Number:
- NA0001982; AC05-00OR22725; FC52-06NA27684; AC52-06NA25396; XDA07020400
- Resource 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)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; molybdenum nitride; MoN2; high-pressure synthesis; catalyst; hydrodesulfurization; sour mathanation
Citation Formats
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, and Zhao, Yusheng. A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b01446.
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. A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications. United States. https://doi.org/10.1021/jacs.5b01446
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, and Zhao, Yusheng. Mon .
"A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications". United States. https://doi.org/10.1021/jacs.5b01446. https://www.osti.gov/servlets/purl/1332528.
@article{osti_1332528,
title = {A new molybdenum nitride catalyst with rhombohedral MoS2 structure for hydrogenation applications},
author = {Wang, Shanmin and Ge, Hui and Sun, Shouli and Zhang, Jianzhong and Liu, Fangming and Wen, Xiaodong and Yu, Xiaohui and Wang, Liping and Zhang, Yi and Xu, Hongwu and Neuefeind, Joerg C. and Qin, Zhangfeng and Chen, Changfeng and Jin, Changqin and Li, Yongwang and He, Duanwei and Zhao, Yusheng},
abstractNote = {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.},
doi = {10.1021/jacs.5b01446},
journal = {Journal of the American Chemical Society},
number = 14,
volume = 137,
place = {United States},
year = {Mon Mar 23 00:00:00 EDT 2015},
month = {Mon Mar 23 00:00:00 EDT 2015}
}
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