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Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt
Gao, Wenbo1,2; Wang, Peikun1,2; Guo, Jianping1,4; Chang, Fei1,2; He, Teng1; Wang, Qianru1,2; Wu, Guotao1; Chen, Ping1,3,4
KeywordAmmonia Synthesis Barium Hydride Cobalt Barium Imide Promoter Heterogeneous Catalysis
Source PublicationACS CATALYSIS
2017-05-01
DOI10.1021/acscatal.7b00284
Volume7Pages:3654-3661
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordSUPPORTED RUTHENIUM CATALYST ; IRON-COBALT ; CARBON ; PROMOTER ; ADSORPTION ; PRESSURE ; SURFACES ; KINETICS ; NITRIDE
AbstractIndustrial ammonia synthesis catalyzed by Fe- and Ru-based catalysts is an energy-consuming process. The development of low-temperature active catalyst has been pursued for a century. Herein, we report that barium hydride (BaH2) can synergize with Co, leading to a much better low-temperature activity, i.e., the BaH2-Co/carbon nanotube (CNT) catalyst exhibits ammonia synthesis activity right above 150 degrees C; at 300 degrees C, it is 2 orders of magnitude higher than that of the BaO-Co/CNTs and more than 2.5-times higher than Cs promoted Ru/MgO. Kinetic analyses reveal that the dissociative adsorption of N-2 on the Co-BaH2 catalyst may not be the rate-determining step, as evidenced by the much smaller reaction order of N-2 (0.43) and the lower apparent activation energy (58 kJ mol(-1)) compared with those of the unpromoted and BaO-promoted Co-based catalysts. BaH2, with a negative hydride ion, may act as a strong reducing agent, removing activated N from the Co surface and forming a BaNH species. The hydrogenation of the BaNH species to NH3 and BaH2 can be facilely carried out at 150 degrees C. The relayed catalysis by Co and BaH2 sites creates an synthesis under milder conditions.
Language英语
WOS IDWOS:000401054300069
Citation statistics
Cited Times:16[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/152288
Collection中国科学院大连化学物理研究所
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
4.Collaborat Innovat Ctr Chem Energy Mat, Dalian 116023, Peoples R China
Recommended Citation
GB/T 7714
Gao, Wenbo,Wang, Peikun,Guo, Jianping,et al. Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt[J]. ACS CATALYSIS,2017,7:3654-3661.
APA Gao, Wenbo.,Wang, Peikun.,Guo, Jianping.,Chang, Fei.,He, Teng.,...&Chen, Ping.(2017).Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt.ACS CATALYSIS,7,3654-3661.
MLA Gao, Wenbo,et al."Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt".ACS CATALYSIS 7(2017):3654-3661.
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