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In this study, we utilized an ultramicroporous metal-organic framework (MOF) named [Ni(pzdc)(ade)(HO)]·2.18HO (where Hpzdc represents pyrazole-3,5-dicarboxylic acid and ade represents adenine) for hydrogen (H) adsorption. Upon activation, [Ni(pzdc)(ade)] was obtained, and in situ carbon monoxide loading by transmission infrared spectroscopy revealed the generation of open Ni(II) sites. The MOF displayed a Brunauer-Emmett-Teller (BET) surface area of 160 m/g and a pore size of 0.67 nm. Hydrogen adsorption measurements conducted on this MOF at 77 K showed a steep increase in uptake (up to 1.93 mmol/g at 0.04 bar) at low pressure, reaching a H uptake saturation at 2.11 mmol/g at ∼0.15 bar. The affinity of this MOF for H was determined to be 9.7 ± 1.0 kJ/mol. In situ H loading experiments supported by molecular simulations confirmed that H does not bind to the open Ni(II) sites of [Ni(pzdc)(ade)], and the high affinity of the MOF for H is attributed to the interplay of pore size, shape, and functionality.
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| http://dx.doi.org/10.1021/acsami.3c12139 | DOI Listing |
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