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Author ORCID ID is 0000000153297408
  1. Managing water is critical for industrial applications including CO2 capture, catalysis, bio-oil separations and energy storage. Various classes of materials have been designed for these applications, achieving specific water adsorption capacities at a given relative humidity (RH). Three water adsorption-desorption mechanisms are common to inorganic materials: (1) chemisorption, which may lead to the modification of the first coordination sphere; (2) simple adsorption, which is reversible in nature; or (3) capillary condensation, which is irreversible in nature. Regardless of sorption mechanism, all materials known today increase water adsorption capacity with increasing RH; none exhibit repeated adsorption of water at low humiditymore » and release at high humidity. We present here a material that breaks from this convention: a new class of nitrogen containing carbon rods along with nonstoichiometric FeXSY that adsorb water at low humidity, and spontaneously expel half of the adsorbed water when the RH exceeds a 50–80% threshold. Monolayers of water form on the surfaces of the carbon rods, with the amount of water adsorbed directly linked to the aspect ratio of the rods and the available surface area. This unprecedented water expulsion is a reversible physical process. Once a complete monolayer is formed, adjacent rods in the bundles begin to adhere together via formation of a bridging monolayer, reducing the surface area available for water to adhere to. We believe the unique surface chemistry of these carbon rods can be used on other functionalized materials. Such behaviour offers a paradigm shift in water purification and separation: water could be repeatedly adsorbed from a low humidity vapour stream and then expelled into a pure water vapour stream, or humidity-responsive membranes could change their water permeance or selectivity as a function of RH.« less
  2. Nuclear energy is considered among the most viable alternatives to our current fossil fuel based energy economy.1 The mass-deployment of nuclear energy as an emissions-free source requires the reprocessing of used nuclear fuel to mitigate the waste.2 One of the major concerns with reprocessing used nuclear fuel is the release of volatile radionuclides such as Xe and Kr. The most mature process for removing these radionuclides is energy- and capital-intensive cryogenic distillation. Alternatively, porous materials such as metal-organic frameworks (MOFs) have demonstrated the ability to selectively adsorb Xe and Kr at ambient conditions.3-8 High-throughput computational screening of large databases ofmore » porous materials has identified a calcium-based nanoporous MOF, SBMOF-1, as the most selective for Xe over Kr.9,10 Here, we affirm this prediction and report that SBMOF-1 exhibits by far the highest Xe adsorption capacity and a remarkable Xe/Kr selectivity under relevant nuclear reprocessing conditions. The exceptional selectivity of SBMOF-1 is attributed to its pore size tailored to Xe and its dense wall of atoms that constructs a binding site with a high affinity for Xe, as evident by single crystal X-ray diffraction and molecular simulation.« less
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