Ha Junsu, Jung Minji, Park Jaewoo, Oh Hyunchul, Moon Hoi Ri
Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea.
ACS Appl Mater Interfaces. 2022 Jul 13;14(27):30946-30951. doi: 10.1021/acsami.2c07829. Epub 2022 Jun 23.
Hydrogen isotope separation with nanoporous materials is a very challenging yet promising approach. To overcome the limitation of the conventional isotope separation strategy, quantum sieving-based separation using nanoporous materials has been investigated recently. In this study, to see the thermodynamic deuterium separation phenomena attributed to the chemical affinity quantum sieving effect, we examine Hofmann-type metal-organic frameworks (MOFs), Co(pyz)[M(CN)] (pyz = pyrazine, M = Pd, Pt, and Ni), which have microporosity (4.0 × 3.9 Å) and an extraordinarily high density of open metal sites (∼9 mmol/cm). Owing to the preferential adsorption of D over H at strongly binding open metal sites, the Hofmann-type MOF, Co(pyz)[Pd(CN)] exhibited a high selectivity () of 21.7 as well as a large D uptake of 10 mmol/g at 25 K. This is the first study of Hofmann-type MOFs to report high selectivity and capacity, both of which are important parameters for the practical application of porous materials toward isotope separation.
利用纳米多孔材料进行氢同位素分离是一种极具挑战性但前景广阔的方法。为克服传统同位素分离策略的局限性，近年来人们对基于量子筛分的纳米多孔材料分离方法进行了研究。在本研究中，为了观察归因于化学亲和力量子筛分效应的热力学氘分离现象，我们研究了霍夫曼型金属有机框架（MOF），即Co(pyz)[M(CN)]（pyz = 吡嗪，M = Pd、Pt和Ni），其具有微孔结构（4.0 × 3.9 Å）和极高密度的开放金属位点（约9 mmol/cm）。由于在强结合的开放金属位点上D比H具有优先吸附性，霍夫曼型MOF，即Co(pyz)[Pd(CN)]在25 K时表现出21.7的高选择性以及10 mmol/g的大氘吸附量。这是首次对霍夫曼型MOF报道其高选择性和容量，这两个参数对于多孔材料在同位素分离实际应用中都很重要。
