The adsorption thermodynamics of H2O and CO2 on PuO2(1 1 1) surface: A comparative study based on DFT+U-D3

Synthesis and multi-scale properties of PuO2 nanoparticles: recent advances and open questions

“…19,173 Simulations performed by Zhang et al indicated that interactions between the PuO 2 (111) surface and H 2 O are higher than those observed with CO 2 under similar (P,T) conditions. 174 Both molecular and dissociative adsorption of water molecules have been demonstrated on the PuO 2 surface using simulations. Particularly, it has been demonstrated that water can be present as adsorbed hydroxyl groups on the ( 110) and (100) surfaces, even at elevated temperatures and pressures.…”

“…19,173 Simulations performed by Zhang et al indicated that interactions between the PuO 2 (111) surface and H 2 O are higher than those observed with CO 2 under similar ( P , T ) conditions. 174…”

Adsorption, dissociation and diffusion behavior of H2O on the PuO2(111) surface from DFT + U-D3: the role of hydrogen bonding

“…24 An effective U (U eff = U − J; i.e., the difference between the Coulomb U and exchange J parameters, hereaer referred to as U) value of 4 eV is selected for the 5f electrons of Pu and U, according to our previous calculations 25,26 and other computational experience. 10,12,14,18,20,[27][28][29] We use the widely accepted collinear 1-k antiferromagnetic (AFM) states along the (111) orientations for the magnetic orders. 30,31 The Brillouin zone was sampled with a 3 × 3 × 1 k-points mesh for the surface models generated by the Monkhorst-Pack method.…”

Theoretical study on the hydrogen distribution and diffusion at the PuO2/α-Pu2O3 interface

“…28 An effective U (U eff = U − J; i.e., the difference between the Coulomb U and exchange J parameters, hereaer referred to as U) value of 4 eV is selected for the 5f electrons of Pu and U, according to our previous calculations 29,30 and other computational experience. 21,22,[31][32][33][34][35][36] According to experimental and theoretical calculations (DFT + U), the ground states of Pu 2 O 3 and PuO 2 are set to antiferromagnetic states (AFM). 28,37 Correction of van der Waals forces between H, H 2 , and plutonium oxide matrix using DFT-D3 method.…”