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Thermodynamics of hydrogen adsorption in MOF-177 at low temperatures: measurements and modelling

机译：低温下MOF-177中氢吸附的热力学：测量和建模

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摘要

Hydrogen adsorption measurements and modelling for the Zn-based microporous metal-organic framework (MOF) Zn_4O(1,3,5-benzenetribenzoate)_2, MOF-177, were performed over the 50-77 K and 0-40 bar ranges. The maximum excess adsorption measured under these conditions varies over about 105-70 mg g~(-1). An analysis of the isotherms near saturation shows that hydrogen is ultimately adsorbed in an incompressible phase whose density is comparable to that of the bulk liquid. These liquid state properties observed under supercritical conditions reveal a remarkable effect of nanoscale confinement. The entire set of adsorption isotherms can be well described using a micropore filling model. The latter is used, in particular, to determine the absolute amounts adsorbed and the adsorption enthalpy. When expressed in terms of absolute adsorption, the isotherms show considerable hydrogen storage capacities, reaching up to 125 mg g~(-1) at 50 K and 25 bar. The adsorption enthalpies are calculated as a function of fractional filling and range from 3 to 5 kJ mol~(-1) in magnitude, in accordance with physisorption. These results are discussed with respect to a similar analysis performed on another Zn-based MOF, Zn_4O(1,4-benzenedicarboxylate)_3, IRMOF-1, presented recently. It is found that both materials adsorb hydrogen by similar mechanisms.
机译：在50-77 K和0-40 bar的压力范围内，进行了Zn基微孔金属有机骨架（MOF）Zn_4O（1,3,5-苯三苯甲酸酯）_2，MOF-177的氢吸附测量和建模。在这些条件下测得的最大过量吸附在约105-70 mg g〜（-1）之间变化。对接近饱和的等温线的分析表明，氢最终被吸附在不可压缩的相中，该相的密度与本体液体的密度相当。在超临界条件下观察到的这些液态性质揭示了纳米级限制的显着效果。可以使用微孔填充模型很好地描述整套吸附等温线。后者尤其用于确定绝对吸附量和吸附焓。当用绝对吸附表示时，等温线显示出相当大的储氢能力，在50 K和25 bar下达到125 mg g〜（-1）。根据物理吸附，计算出的吸附焓是分数填充的函数，其范围为3至5 kJ mol〜（-1）。关于最近对另一个基于Zn的MOF Zn_4O（1,4-苯二甲酸）_3 IRMOF-1进行的类似分析，讨论了这些结果。发现两种材料都通过相似的机理吸收氢。

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