Cr/Ti掺杂石墨烯活化CO2分解的理论研究

为筛选更高效的CO2分解还原的催化材料，采用密度泛函理论中的B3LYP方法结合6-31G(d)基组，研究了Cr、Ti掺杂石墨烯对CO2分子的吸附与催化分解的机理.研究结果表明：CO2分子在Cr元素和Ti元素掺杂石墨烯表面的吸附为放热过程，吸附能分别为28.3kcal/mol和7.7kcal/mol，两种元素掺杂石墨烯催化CO2分子中C-O断裂的活化能分别为15.5kcal/mol和7.8kcal/mol,反应过程遵循插入-消除原理，计算结果为CO2还原的催化剂设计提供理论指导.

Theoretical study of the dissociation of CO2 catalyzed by Cr/Ti-doped graphene

In order to screen the highly efficient catalyst for the reduction of CO2 molecule, the B3LYP method in combination with the 6-31G(d) basis set was used to calculate the adsorption of CO2 molecule on surfaces of the Cr-doped graphene and Ti-doped graphene. Meanwhile, the CO2 dissociation mechanism catalyzed by the Cr-doped graphene and Ti-doped graphene was also considered with the same calculation method. Results show that the process is exothermal for the CO2 adsorption on the doped-graphene surface. The adsorption energies are 28.3kcal/mol and 7.7kcal/mol for the CO2 adsorption on the Cr-doped graphene and Ti-doped graphene surface, respectively. The dissociation of CO2 catalyzed by the Cr/Ti-doped graphene follows the insertion-elimination mechanism. The calculated activation energies of the C-O bond dissociation are 15.5 kcal/mol and 7.8kcal/mol for the Cr and Ti-doped graphene, respectively. Our calculation results would be a guideline for the design of catalyst for the CO2 reduction.