Abstract
The separation of tritium (3H) from radioactive wastewater is a persistent challenging problem in the nuclear industry from an environmental perspective. This study provides new insight into the tritium separation by investigating hydrogen isotope-selective exchange reaction on hydrogen-bonded fluorine (F····H····O) site. In this study, fluorinated mesoporous silica, F-MCM-41_NCs were prepared as a novel tritium sorbent that showed a significantly enhanced tritium isotope separation factor (α) compared to the pristine MCM-41 (α = 1.2). The optimal α of 3.3 is achieved using 0.5F-MCM-41_NC prepared with 0.5 g of NH4F per gram of MCM-41. This optimal α is attributed to an excellent compromise between the amount and the stability of (NH4)2SiF6 on the pore channel with the integrity of the MCM-41 framework. Experimental, theoretical, and analytical characterization results consistently support chemical affinity quantum sieving effect at F····H····O hydrogen-bonding sites via the hydrogen isotope-selective exchange reaction as the dominant tritiumseparation mechanism.
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