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题名: Barium Hydride-Mediated Nitrogen Transfer and Hydrogenation for Ammonia Synthesis: A Case Study of Cobalt
作者: Gao, Wenbo1, 2;  Wang, Peikun1, 2;  Guo, Jianping1, 4;  Chang, Fei1, 2;  He, Teng1;  Wang, Qianru1, 2;  Wu, Guotao1;  Chen, Ping1, 3, 4
关键词: ammonia synthesis ;  barium hydride ;  cobalt ;  barium imide ;  promoter ;  heterogeneous catalysis
刊名: ACS CATALYSIS
发表日期: 2017-05-01
DOI: 10.1021/acscatal.7b00284
卷: 7, 页:3654-3661
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical
研究领域[WOS]: Chemistry
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.
关键词[WOS]: SUPPORTED RUTHENIUM CATALYST ;  IRON-COBALT ;  CARBON ;  PROMOTER ;  ADSORPTION ;  PRESSURE ;  SURFACES ;  KINETICS ;  NITRIDE
语种: 英语
WOS记录号: WOS:000401054300069
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/152288
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.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:
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.
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