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题名: Transition and Alkali Metal Complex Ternary Amides for Ammonia Synthesis and Decomposition
作者: Cao, Hujun1;  Guo, Jianping2;  Chang, Fei2;  Pistidda, Claudio1;  Zhou, Wei3;  Zhang, Xilun2;  Santoru, Antonio1;  Wu, Hui3;  Schell, Norbert4;  Niewa, Rainer5;  Chen, Ping2;  Klassen, Thomas1;  Dornheim, Martin1
关键词: ammonia decomposition ;  ammonia synthesis ;  ternary transition metal amide ;  transition metal nitride
刊名: CHEMISTRY-A EUROPEAN JOURNAL
发表日期: 2017-07-21
DOI: 10.1002/chem.201702728
卷: 23, 期:41, 页:9766-9771
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: A new complex ternary amide, Rb-2[Mn(NH2)(4)], which simultaneously contains both transition and alkali metal catalytic sites, is developed. This is in line with the recently reported TM-LiH composite catalysts, which have been shown to effectively break the scaling relations and achieve ammonia synthesis under mild conditions. Rb-2[Mn(NH2)(4)] can be facilely synthesized by mechanochemical reaction at room temperature. It exhibits two temperature-dependent polymorphs, that is, a low-temperature orthorhombic and a high-temperature monoclinic structure. Rb-2[Mn(NH2)(4)] decomposes to N-2, H-2, NH3, Mn3N2, and RbNH2 under inert atmosphere; whereas it releases NH3 at a temperature as low as 80 degrees C under H-2 atmosphere. Those unique behaviors enable Rb-2[Mn(NH2)(4)], and its analogue K-2[Mn(NH2)(4)], to be excellent catalytic materials for ammonia decomposition and synthesis. Experimental results show both ammonia decomposition onset temperatures and conversion rates over Rb-2[Mn(NH2)(4)] and K-2[Mn(NH2)(4)] are similar to those of noble metal Ru-based catalysts. More importantly, these ternary amides exhibit superior capabilities in catalyzing NH3 synthesis, which are more than 3 orders of magnitude higher than that of Mn nitride and twice of that of Ru/MgO. The in situ SR-PXD measurement shows that manganese nitride, synergistic with Rb/KH or Rb/K(NH2)(x)H1-x, are likely the active sites. The chemistry of Rb-2/K-2[Mn(NH2)(x)] and Rb/K(NH2)(x)H1-x with H-2/N-2 and NH3 correlates closely with the catalytic performance.
关键词[WOS]: HYDROGEN STORAGE MATERIALS ;  AMMONOTHERMAL SYNTHESIS ;  CATALYSIS ;  NITROGEN ;  NITRIDE ;  IMIDES ;  LINH2 ;  RU
语种: 英语
WOS记录号: WOS:000405923800013
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/151909
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.Helmholtz Zentrum Geesthacht GmbH, Mat Technol, Inst Mat Res, Max Planck Str 1, D-21502 Geesthacht, Germany
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA
4.Helmholtz Zentrum Geesthacht, Inst Mat Sci, Notkestr 85, D-22607 Hamburg, Germany
5.Univ Stuttgart, Inst Inorgan Chem, Pfaffenwaldring 55, D-70569 Stuttgart, Germany

Recommended Citation:
Cao, Hujun,Guo, Jianping,Chang, Fei,et al. Transition and Alkali Metal Complex Ternary Amides for Ammonia Synthesis and Decomposition[J]. CHEMISTRY-A EUROPEAN JOURNAL,2017,23(41):9766-9771.
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