Journal
ACS NANO
Volume 8, Issue 1, Pages 761-770Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn405420t
Keywords
nanoporous materials; quantum sieving; hydrogen isotopes; gas adsorption; isotope separation; metal-organic frameworks
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Funding
- International Max Planck Research School for Advanced Materials (IMPRS-AM)
- German Research Foundation DFG
- European Research Council [ERC-StG C3ENV, GA256962]
- Marie-Curie IAPP QUASINANO [GA251149]
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Separating gaseous mixtures that consist of very similar size is one of the critical issues in modern separation technology. Especially, the separation of the isotopes hydrogen and deuterium requires special efforts, even though these isotopes show a very large mass ratio. Conventionally, H/D separation can be realized through cryogenic distillation of the molecular species or the Girdler-sulfide process, which are among the most energy-intensive separation techniques in the chemical industry. However, costs can be significantly reduced by using highly mass-selective nanoporous sorbents. Here, we describe a hydrogen isotope separation strategy exploiting the strongly attractive open metal sites present in nanoporous metal organic frameworks of the CPO-27 family (also referred to as MOF-74). A theoretical analysis predicts an outstanding hydrogen isotopologue separation at open metal sites due to isotopal effects, which has been directly observed through cryogenic thermal desorption spectroscopy. For H-2/D-2 separation of an equimolar mixture at 60 K, the selectivity of 12 is the highest value ever measured, and this methodology shows extremely high separation efficiencies even above 77 K. Our theoretical results imply also a high selectivity for HD/H-2 separation at similar temperatures, and together with catalytically active sites, we propose a mechanism to produce D-2 from HD/H-2 mixtures with natural or enriched deuterium content.
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