Reactivity of layered manganese oxide toward water oxidation under alkaline conditions in presence and in absence of iron

This dataset includes the computational workflows of a density functional theory based study of the oxygen evolution reaction (OER) on a manganese oxide catalyst in presence and absence of iron dopant. The thermodynamic OER overpotential has been computed by using a surface slab model based on a layered birnessite bulk structure of MnO₂ considering supercells with two and four MnO₂ units and by varying the intercalation with KOH, the amount of Fe dopant and the dopant positions. In addition, the dependence of the oxidation state of the active site atoms (either Mn or Fe) on the directly bound OER intermediate species, has been investigated. The results suggest a decrease of up to 310 mV in the thermodynamic OER overpotential upon doping the considered model structures with Fe that is consistent with the experimentally measured total overpotential decrease of 190 mV.

本数据集涵盖了基于密度泛函理论对锰氧化物催化剂上氧还原反应（OER）在有无铁掺杂存在下的计算工作流程。通过采用基于MnO₂层状水铝矿块体结构的表面层模型，并考虑含有两个和四个MnO₂单元的超细胞，以及通过改变与KOH的间插层、Fe掺杂量及掺杂位置，计算了OER的热力学过电位。此外，还研究了活性位点原子（Mn或Fe）的氧化态与直接结合的OER中间物种之间的依赖关系。结果表明，在考虑的模型结构中掺杂Fe后，热力学OER过电位降低了高达310 mV，这与实验测量的总过电位降低190 mV相一致。