Synthesis and advanced dehydrogenation properties of niobium-based ammine borohydride

Synthesis and advanced dehydrogenation properties of niobium-based ammine borohydride
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铌基氨胺硼氢化物的合成及先进脱氢性能

DOI:
10.1016/j.ijhydene.2013.05.044
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发表时间:
2013-07
期刊:
Int. J. Hydrogen Energy [IF=3.5]
影响因子:
--
通讯作者:
Yu, Xuebin
Yu, Xuebin
中科院分区:
其他
文献类型:
--
作者:
Li, Meng;Yuan, Feng;Gu, Qinfen;Yu, Xuebin

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以NbCl5·5nh3和MBH4(M = Li, Na)为原料,摩尔比为1:5,采用简单球磨法制备了铌基氨基硼氢化物。热重质谱分析(TGA-MS)和程序升温解吸(TPD)结果表明,NbCl5·5nh3 / 5libh4和NbCl5·5nh3 / 5nabh4混合物在加热至250℃时的脱氢过程为两步分解,纯氢析出率分别为8.1 wt.%和11.2 wt.%。等温TPD结果表明,在150℃和220℃条件下,60 min内,NbCl5·5nh3 / 5nabh4分别释放出6 wt.%和10.4 wt.%的纯氢。傅里叶变换红外光谱(FTIR)和同位素标记测量表明,铌基氨基硼氢化物的脱氢机制不仅基于BH和NH基团的组合反应,而且BH⋯HB和NH⋯HN的同极性相互作用也有助于h2生成。
In this paper, niobium-based ammine borohydride has been synthesized via a simple ball milling of NbCl5·5NH3and MBH4(M = Li, Na) with a molar ratio of 1:5. Thermogravimetric analysis–mass spectrometry (TGA–MS) and temperature-programmed-desorption (TPD) results revealed that the dehydrogenation of NbCl5·5NH3/5LiBH4and NbCl5·5NH3/5NaBH4mixtures showed a two-step decomposition process with a total of 8.1 wt.% and 11.2 wt.% pure hydrogen evolution upon heating to 250 °C, respectively. Isothermal TPD results showed that over 6 wt.% and 10.4 wt.% pure hydrogen were liberated from NbCl5·5NH3/5NaBH4within 60 min at 150 °C and 220 °C, respectively. Fourier transform infrared spectroscopy (FTIR) and isotope tagging measurements demonstrated that the dehydrogenation mechanism of niobium-based ammine borohydride is not only based on the combination reaction of BH and NH groups, but the BH⋯HB and NH⋯HN homo-polar interactions also contribute to the H2formation.
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