2分子在UO2 (111)表面的吸附和解離，分析了不同構(gòu)型下的靜態(tài)和動(dòng)態(tài)吸附機(jī)理，吸附位點(diǎn)包括頂位、空位、橋位。在靜態(tài)計(jì)算中，探究了吸附過程中多種吸附參數(shù)的變化，如吸附構(gòu)型、吸附能、電荷轉(zhuǎn)移等。利用第一性原理分子動(dòng)力學(xué)（AIMD），探究了特定構(gòu)型下CO2分子的解離過程及差分電荷密度變化。結(jié)果表明，CO分子的吸附可分為2種類型：（1）自發(fā)吸附，包括化學(xué)和物理吸附；（2）非自發(fā)吸附。CO2分子的吸附僅表現(xiàn)為自發(fā)吸附的化學(xué)吸附及非自發(fā)吸附，無物理吸附。CO和CO2分子的最優(yōu)吸附構(gòu)型均為短橋位垂直（B-short-Ver）吸附。此外，0 K下CO2分子在UO2 (111)表面的B-short-Ver和長(zhǎng)橋位垂直吸附構(gòu)型吸附后會(huì)自發(fā)解離。AIMD模擬結(jié)果表明，這2種構(gòu)型在300 K下均發(fā)生解離。;The adsorption and dissociation of CO and CO2 molecules on UO2 (111) slab were investigated by the first-principles calculations based on density functional theory with the addition of Hubbard term for calculation correction. Different static and dynamic adsorption mechanisms under different configurations were analyzed, and the adsorption sites included top, hollow, and bridge sites. In the static calculations, the variation of adsorption parameters, such as adsorption configuration, adsorption energy, and charge transfer, during adsorption process was investigated. ab-initio molecular dynamics (AIMD) was employed to study the dissociation process of CO2 molecules and the changes in charge density difference. Results show that the adsorption of CO molecules can be categorized into two types: (1) stable adsorption, including chemical and physical adsorptions; (2) unstable adsorption. The adsorption types of CO2 on UO2 (111) slab only include the chemical adsorption of stable adsorption and unstable adsorption. No physical adsorption exists. The optimal configuration for the adsorption of both CO and CO2 molecules is short-bridge vertical (B-short-Ver) adsorption. Additionally, at 0 K, the CO2 molecules at the configurations related to B-short-Ver adsorption and long-bridge vertical adsorption on UO2 (111) slab spontaneously dissociate after adsorption. AIMD simulation results show that both configurations dissociate at 300 K."/>