中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt

文献类型:期刊论文

作者Gao, Wenbo2,3; Wang, Peikun2,3; Guo, Jianping1,2; Chang, Fei2,3; He, Teng2; Wang, Qianru2,3; Wu, Guotao2; Chen, Ping1,2,4
刊名ACS CATALYSIS
出版日期2017-05-01
卷号7页码:3654-3661
关键词Ammonia Synthesis Barium Hydride Cobalt Barium Imide Promoter Heterogeneous Catalysis
DOI10.1021/acscatal.7b00284
英文摘要Industrial 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.
语种英语
WOS记录号WOS:000401054300069
源URL[http://cas-ir.dicp.ac.cn/handle/321008/152288]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
作者单位1.Collaborat Innovat Ctr Chem Energy Mat, Dalian 116023, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式
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.

入库方式: OAI收割

来源:大连化学物理研究所

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