The extraction of uranium (U) and its alternative resources, such as thorium (Th) and plutonium (Pu), from seawater is essential to address the scarcity of terrestrial U resources. The development of a separation material with high adsorption properties is the key to solving this problem.

This study aims to reveal the adsorption behavior of actinides (U, Th, and Pu) on the surface of a two-dimensional metal material, antimonene.

The Hubbard U values, U_eff, were determined for the on-site Coulomb interactions of 5f electrons of U and Pu atoms using the linear response method. Furthermore, the adsorption energy, adsorption configuration, electronic structures, charge transfer, and highest occupied molecular orbital wavefunction of a U, Th, or Pu atom adsorbed on the surface of monolayer antimonene were analyzed using the DFT+U approximation. The variation of the adsorption rate with temperature was further calculated by the equilibrium adsorption rate equation.

The calculated U_eff values of U and Pu atoms are 2.24 eV and 2.84 eV, respectively. The Pu atom is energetically unfavorable to be adsorbed on antimonene (with a negative adsorption energy for each adsorption site), whereas the U and Th atoms exhibit strong chemical adsorption on its surface. Antimonene also offers abundant surficial stable adsorption sites for the U and Th adatoms. The most energetically stable sites for the U and Th adatoms are the B (Bridge)-H (Hollow) site and H (Hollow) site, with adsorption energies of 4.40 eV and 3.62 eV, respectively. The impurity states are generated in the band gap of antimonene upon the adsorption of the U or Th atom, and the strong p-d coupling between the U or Th adatom and antimonene in the impurity states contributes to the strong adsorption of the adatoms. The desorption temperatures of U and Th on the surface of antimonene reach 837 K and 660 K, respectively.

The results indicate that antimonene is an excellent two-dimensional adsorbent material for U and Th and has potential for several applications such as in the extraction of actinides from seawater.