脱氢
氢化物
无机化学
硼氢化
氢气储存
金属有机骨架
镁
氢键
材料科学
化学
物理化学
金属
氢
分子
催化作用
有机化学
吸附
作者
Andreas Schneemann,Liwen F. Wan,Andrew Lipton,Yi‐Sheng Liu,Jonathan L. Snider,Alexander A. Baker,Joshua D. Sugar,Catalin D. Spataru,Jinghua Guo,Tom Autrey,Mathias Jørgensen,Torben R. Jensen,Brandon C. Wood,Mark D. Allendorf,Vitalie Stavila
出处
期刊:ACS Nano
[American Chemical Society]
日期:2020-07-13
卷期号:14 (8): 10294-10304
被引量:49
标识
DOI:10.1021/acsnano.0c03764
摘要
The lower limit of metal hydride nanoconfinement is demonstrated through the coordination of a molecular hydride species to binding sites inside the pores of a metal-organic framework (MOF). Magnesium borohydride, which has a high hydrogen capacity, is incorporated into the pores of UiO-67bpy (Zr6O4(OH)4(bpydc)6 with bpydc2- = 2,2'-bipyridine-5,5'-dicarboxylate) by solvent impregnation. The MOF retained its long-range order, and transmission electron microscopy and elemental mapping confirmed the retention of the crystal morphology and revealed a homogeneous distribution of the hydride within the MOF host. Notably, the B-, N-, and Mg-edge XAS data confirm the coordination of Mg(II) to the N atoms of the chelating bipyridine groups. In situ11B MAS NMR studies helped elucidate the reaction mechanism and revealed that complete hydrogen release from Mg(BH4)2 occurs as low as 200 °C. Sieverts and thermogravimetric measurements indicate an increase in the rate of hydrogen release, with the onset of hydrogen desorption as low as 120 °C, which is approximately 150 °C lower than that of the bulk material. Furthermore, density functional theory calculations support the improved dehydrogenation properties and confirm the drastically lower activation energy for B-H bond dissociation.
科研通智能强力驱动
Strongly Powered by AbleSci AI