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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >High-pressure/low-temperature neutron scattering of gas inclusion compounds: Progress and prospects
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High-pressure/low-temperature neutron scattering of gas inclusion compounds: Progress and prospects

机译：气体夹杂物的高压/低温中子散射：进展与展望

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Alternative energy resources such as hydrogen and methane gases are becoming increasingly important for the future economy. A major challenge for using hydrogen is to develop suitable materials to store it under a variety of conditions, which requires systematic studies of the structures, stability, and kinetics of various hydrogen-storing compounds. Neutron scattering is particularly useful for these studies. We have developed high-pressure/low-temperature gas/fluid cells in conjunction with neutron diffraction and inelastic neutron scattering instruments allowing in situ and real-time examination of gas uptake/release processes. We studied the formation of methane and hydrogen clathrates, a group of inclusion compounds consisting of frameworks of hydrogen-bonded H2O molecules with gas molecules trapped inside the cages. Our results reveal that clathrate can store up to four hydrogen molecules in each of its large cages with an intermolecular H2–H2 distance of only 2.93 Å. This distance is much shorter than that in the solid/metallic hydrogen (3.78 Å), suggesting a strong densification effect of the clathrate framework on the enclosed hydrogen molecules. The framework-pressurizing effect is striking and may exist in other inclusion compounds such as metal-organic frameworks (MOFs). Owing to the enormous variety and flexibility of their frameworks, inclusion compounds may offer superior properties for storage of hydrogen and/or hydrogen-rich molecules, relative to other types of compounds. We have investigated the hydrogen storage properties of two MOFs, Cu3[Co(CN)6]2 and Cu3(BTC)2 (BTC = benzenetricarboxylate), and our preliminary results demonstrate that the developed neutron-scattering techniques are equally well suited for studying MOFs and other inclusion compounds.
机译：诸如氢气和甲烷气体之类的替代能源对未来的经济越来越重要。使用氢的主要挑战是开发适合的材料以在各种条件下存储氢，这需要对各种储氢化合物的结构，稳定性和动力学进行系统研究。中子散射对于这些研究特别有用。我们开发了高压/低温气体/流体池，结合中子衍射和非弹性中子散射仪器，可就地和实时检查气体的吸收/释放过程。我们研究了甲烷和氢包合物的形成，甲烷和氢包合物是一组由氢键合的H2O分子的框架与捕获在笼子中的气体分子组成的包裹体。我们的结果表明，包合物可以在每个大笼子中最多存储四个氢分子，分子间的H2-H2距离仅为2.93 93。该距离比固体/金属氢（3.78 3.7）中的距离短得多，表明笼形骨架对封闭的氢分子具有很强的致密化作用。骨架加压效果惊人，并且可能存在于其他夹杂物中，例如金属有机骨架（MOF）。由于其构架的多样性和灵活性，相对于其他类型的化合物，夹杂化合物可为氢和/或富氢分子的存储提供优越的性能。我们已经研究了两种MOF（Cu3 [Co（CN）6] 2和Cu3（BTC）2（BTC =苯三羧酸酯））的储氢特性，我们的初步结果表明，开发的中子散射技术同样非常适合于研究MOF和其他包含物。

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