U(VI)
and Eu(III), as representative elements of the hexavalent
actinide and trivalent lanthanides (always as a chemical analogue
for trivalent actinide), respectively, have attracted more and more
attentions due to the widespread use of nuclear energy. Much effort
has been focused on developing versatile materials for their uptake
from aqueous solution. For the first time, we report here UiO-66 and
its mono- (UiO-66-COOH) and di-carboxyl (UiO-66-2COOH) functional
derivatives as robust adsorbents for efficient U(VI) and Eu(III) removal.
It is found that the introduction of carboxyl groups greatly reduces
the surface charge of UiO-66, thus guaranteeing excellent adsorption
capacity at low pH. At pH = 3, for example, the adsorption capacity
of UiO-66-2COOH for U(VI) and Eu(III) is more than 100 and 60 mg/g,
respectively, while almost no adsorption occurs for pristine UiO-66.
At pH = 4, both UiO-66-COOH and UiO-66-2COOH show high performance
on U(VI) and Eu(III) removal. UiO-66-COOH has adsorption capacities
of 80 and 43 mg/g for U(VI) and Eu(III), respectively, while the values
for UiO-66-2COOH reach 150 and 80 mg/g, respectively. Also, all these
materials achieve adsorption equilibrium within 100 min. More importantly,
combining the needs of practical applications and the characteristics
of high stability, high porosity, and excellent adsorption performance
of UiO-66-2COOH, dynamic adsorption column experiments were successfully
conducted; ∼99% U(VI)/Eu(III) can be efficiently adsorbed,
and >90% adsorbed U(VI)/Eu(III) can be re-collected with dilute
nitric
acid solution, even after four adsorption–desorption cycles.
The findings of this work demonstrate the application potential of
metal–organic framework materials to remove radionuclides from
environmental samples or nuclear waste liquids.