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First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials
journal contribution
posted on 2018-03-27, 00:00 authored by Austin P. Ladshaw, Alexander S. Ivanov, Sadananda Das, Vyacheslav S. Bryantsev, Costas Tsouris, Sotira YiacoumiNuclear power is
a relatively carbon-free energy source that has
the capacity to be utilized today in an effort to stem the tides of
global warming. The growing demand for nuclear energy, however, could
put significant strain on our uranium ore resources, and the mining
activities utilized to extract that ore can leave behind long-term
environmental damage. A potential solution to enhance the supply of
uranium fuel is to recover uranium from seawater using amidoximated
adsorbent fibers. This technology has been studied for decades but
is currently plagued by the material’s relatively poor selectivity
of uranium over its main competitor vanadium. In this work, we investigate
the binding schemes between uranium, vanadium, and the amidoxime functional
groups on the adsorbent surface. Using quantum chemical methods, binding
strengths are approximated for a set of complexation reactions between
uranium and vanadium with amidoxime functionalities. Those approximations
are then coupled with a comprehensive aqueous adsorption model developed
in this work to simulate the adsorption of uranium and vanadium under
laboratory conditions. Experimental adsorption studies with uranium
and vanadium over a wide pH range are performed, and the data collected
are compared against simulation results to validate the model. It
was found that coupling ab initio calculations with process level
adsorption modeling provides accurate predictions of the adsorption
capacity and selectivity of the sorbent materials. Furthermore, this
work demonstrates that this multiscale modeling paradigm could be
utilized to aid in the selection of superior ligands or ligand compositions
for the selective capture of metal ions. Therefore, this first-principles
integrated modeling approach opens the door to the in silico design
of next-generation adsorbents with potentially superior efficiency
and selectivity for uranium over vanadium in seawater.
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multiscale modeling paradigmpH rangeadsorbent surfaceuranium fueladsorption capacitynext-generation adsorbentssimulation resultsFirst-Principles Integrated Adsorption Modelinguranium ore resourcesPolyamidoxime Sorbent Materials Nuclear powercompetitor vanadiumcarbon-free energy sourceprocess level adsorption modelinglaboratory conditionsadsorption modelamidoxime functionalitiesbinding strengthsmining activitiesab initio calculationscomplexation reactionssorbent materialsamidoximated adsorbent fibersquantum chemical methodsExperimental adsorption studiesbinding schemesmetal ionsmodeling approachligand compositionssilico designSelective Capture
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