【摘要】 银基催化剂和铜基催化剂是常用的草酸二甲酯(DMO)部分加氢制乙醇酸甲酯(MG)催化剂。本文运用密度泛函理论(DFT)计算研究了Ag(111)和Cu(111)表面上该过程的反应机制。通过结构优化,得到了最稳定的吸附构型。计算并比较了可能基元反应的活化能和反应热,得到了最可能的反应中间物种和最合理的反应路径;分析了反应路径中各基元反应发生的难易程度,解释了实验中Ag基催化剂和Cu基催化剂的催化行为。更多还原

【Abstract】 Density functional theory(DFT) was used to investigate the reaction mechanism of hydrogenation of dimethyl oxalate(DMO) to methyl glycolate(MG) on Ag-and Cu-based catalysts. The most stable adsorption configurations of all species were identified by optimizing initial configurations. By calculating and comparing the activation energies and reaction heats of possible elementary reactions, the most probable intermediates and dominant reaction pathways were determined. After analyzing the progress of every elementary reaction in this pathway, the catalytic behaviors of Ag-and Cu-based catalysts in previous literatures can be well elucidated.更多还原