Zhang Ruihua, Daglar Hilal, Tang Chun, Li Penghao, Feng Liang, Han Han, Wu Guangcheng, Limketkai Benjie N, Wu Yong, Yang Shuliang, Chen Aspen X-Y, Stern Charlotte L, Malliakas Christos D, Snurr Randall Q, Stoddart J Fraser
Department of Chemistry, The University of Hong Kong, Hong Kong, China.
Department of Chemistry, Northwestern University, Evanston, IL, USA.
Nat Chem. 2024 Dec;16(12):1982-1988. doi: 10.1038/s41557-024-01622-w. Epub 2024 Sep 3.
The storage of hydrogen is key to its applications. Developing adsorbent materials with high volumetric and gravimetric storage capacities, both of which are essential for the efficient use of hydrogen as a fuel, is challenging. Here we report a controlled catenation strategy in hydrogen-bonded organic frameworks (RP-H100 and RP-H101) that depends on multiple hydrogen bonds to guide catenation in a point-contact manner, resulting in high volumetric and gravimetric surface areas, robustness and ideal pore diameters (~1.2-1.9 nm) for hydrogen storage. This approach involves assembling nine imidazole-annulated triptycene hexaacids into a secondary hexagonal superstructure containing three open channels through which seven of the hexagons interpenetrate to form a seven-fold catenated superstructure. RP-H101 exhibits high deliverable volumetric (53.7 g l) and gravimetric (9.3 wt%) capacities for hydrogen under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar). This work illustrates the virtues of supramolecular crystals as promising candidates for hydrogen storage.
氢的储存是其应用的关键。开发具有高体积储氢容量和高重量储氢容量的吸附材料具有挑战性，这两者对于将氢作为燃料的高效利用都至关重要。在此，我们报道了一种在氢键有机框架（RP-H100和RP-H101）中的可控连锁策略，该策略依赖多个氢键以点接触方式引导连锁，从而产生高体积和高重量比表面积、稳定性以及适合储氢的理想孔径（约1.2 - 1.9纳米）。这种方法涉及将九个咪唑稠合的三蝶烯六酸组装成一个包含三个开放通道的二级六方超结构，其中七个六边形相互贯穿形成一个七重连锁超结构。在变温变压条件下（77 K/100 bar → 160 K/5 bar），RP-H101展现出高的可释放体积储氢容量（53.7 g l）和重量储氢容量（9.3 wt%）。这项工作说明了超分子晶体作为有前景的储氢候选材料的优点。
