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题名: From Exothermic to Endothermic Dehydrogenation - Interaction of Monoammoniate of Magnesium Amidoborane and Metal Hydrides
作者: Chua, Yong Shen1;  Li, Wen1, 2;  Wu, Guotao1;  Xiong, Zhitao1;  Chen, Ping1
关键词: hydrogen storage ;  amidoborane ;  endothermic ;  dehydrogenation
刊名: CHEMISTRY OF MATERIALS
发表日期: 2012-09-25
DOI: 10.1021/cm301662q
卷: 24, 期:18, 页:3574-3581
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Physical ;  Materials Science, Multidisciplinary
研究领域[WOS]: Chemistry ;  Materials Science
英文摘要: Metal amidoborane ammoniate such as Mg-(NH2BH3)(2)center dot NH3 and Ca(NH2BH3)(2)center dot nNH(3) with n = 1, 2, release NH3 predominantly and endothermically at low temperatures in an open-system. However, a strong exothermic reaction occurs when these ammoniates were dehydrogenated in a closed-system, where the adducted NH3 take part in the reaction. Our approach in tailoring the thermodynamic properties of Mg(NH2BH3)(2)center dot NH3, by replacing its adducted NH3 with amide was successful, yielding a composite consisting of bimetallic amidoborane and Mg(NH2)(2). Crystal structures of bimetallic amidoboranes, i.e., Na2Mg(NH2BH3)(4) and K2Mg(NH2BH3)(4) were identified and solved. Significant improvement in the dehydrogenation thermodynamic was observed in the composite system as compared to the pristine Mg(NH2BH3)(2)center dot NH3, i.e., the dehydrogenation enthalpies were altered from an exothermic to an endothermic one. In addition, the detection of bimetallic amidoboranes in the composites urges detailed investigation on pristine bimetallic amidoborane, to which later we found that Na2Mg(NH2BH3)(4) also dehydrogenated endothermically at the identical temperature range (ca. 150-170 degrees C) with that of composite systems. Similar activation barriers were observed in Na2Mg(NH2BH3)(4) and composite systems, suggesting that metal hydride mediation may be the internal barrier that dominates the kinetic barrier of the composite system. First-principles calculations also showed that the thermodynamic stability of metal amidoborane (MNH2BH3, MAB) increases with decreasing Pauling electronegativity of the metal. Based on the calculated results, a reactant stabilization approach was proposed, which suggests that forming a stable reactant is an effective way of reducing the exothermicity of the dehydrogenation of metal amidoborane.
关键词[WOS]: HYDROGEN STORAGE PROPERTIES ;  THERMAL-DECOMPOSITION ;  CRYSTAL-STRUCTURE ;  AMMONIA-BORANE ;  LITHIUM HYDRIDE ;  RELEASE ;  COMPLEXES ;  ALKALI ;  NA ;  AMIDOTRIHYDROBORATE
语种: 英语
WOS记录号: WOS:000309041000010
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/143143
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.Dalian Inst Chem Phys, Dalian 116023, Peoples R China
2.Natl Univ Singapore, Dept Phys, Singapore 117542, Singapore

Recommended Citation:
Chua, Yong Shen,Li, Wen,Wu, Guotao,et al. From Exothermic to Endothermic Dehydrogenation - Interaction of Monoammoniate of Magnesium Amidoborane and Metal Hydrides[J]. CHEMISTRY OF MATERIALS,2012,24(18):3574-3581.
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