Open AccessDensity functional study of CO2 adsorption on Pu(100) surface
Author(s) -
Meng Da-Qiao,
Luo Wenhua,
Li Gan,
Chen Hu-chi
Publication year - 2009
Publication title -
wuli xuebao
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.199
H-Index - 47
ISSN - 1000-3290
DOI - 10.7498/aps.58.8224
Subject(s) - adsorption , density functional theory , molecule , materials science , atomic orbital , atom (system on chip) , density of states , chemistry , atomic physics , electron , computational chemistry , physics , condensed matter physics , organic chemistry , quantum mechanics , computer science , embedded system
The adsorption of CO2 on Pu100 surface has been studied with periodic slab model by revised Perdew-Burke-Ernzerh approximation within the framework of density functional theory. The optimized results of adsorption energies and geometrical structures show that the H-C4O4-type adsorption is optimum adsorption mode with adsorption energy of 1.48 eV. The atomic population and density of states analysis indicate that the interaction between Pu atom and CO2 molecule results mainly from strong electron transfer and weak overlap-hybridization between molecular orbital 2πμ of CO2 molecule and Pu5f, Pu6d and Pu7s orbitals of surface Pu atom. The calculated activation barrier and adsorption energy CO2→CO+O dissociative reaction are 0.66 and 2.65 eV, respectively, which indicates the dissociative adsorption of CO2 on Pu100 surface is favorable under the certain heat activation condition. The comparison of O2H2CO and CO2 adsorption on Pu100 surface indicates the adsorption strength follows the ordering: O2COCO2H2 and O2CO2COH2 at lower and higher temperature, respectively.