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Transition and Alkali Metal Complex Ternary Amides for Ammonia Synthesis and Decomposition
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
2017-07-21
DOI10.1002/chem.201702728
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
关键词[WOS]HYDROGEN STORAGE MATERIALS ; AMMONOTHERMAL SYNTHESIS ; CATALYSIS ; NITROGEN ; NITRIDE ; IMIDES ; LINH2 ; RU
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.
语种英语
WOS记录号WOS:000405923800013
引用统计
被引频次:2[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/151909
专题中国科学院大连化学物理研究所
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
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GB/T 7714
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.
APA Cao, Hujun.,Guo, Jianping.,Chang, Fei.,Pistidda, Claudio.,Zhou, Wei.,...&Dornheim, Martin.(2017).Transition and Alkali Metal Complex Ternary Amides for Ammonia Synthesis and Decomposition.CHEMISTRY-A EUROPEAN JOURNAL,23(41),9766-9771.
MLA Cao, Hujun,et al."Transition and Alkali Metal Complex Ternary Amides for Ammonia Synthesis and Decomposition".CHEMISTRY-A EUROPEAN JOURNAL 23.41(2017):9766-9771.
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