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Establishing the Relationship between Quantum Capacitance and Softness of N-Doped Graphene/Electrolyte Interfaces within the Density Functional Theory Grand Canonical Kohn-Sham Formalism.
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-01-10 , DOI: 10.1021/acs.jpca.9b10885 Alvaro Ochoa-Calle 1 , Alfredo Guevara-García 2 , Jorge Vazquez-Arenas 2 , Ignacio González 1 , Marcelo Galván 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-01-10 , DOI: 10.1021/acs.jpca.9b10885 Alvaro Ochoa-Calle 1 , Alfredo Guevara-García 2 , Jorge Vazquez-Arenas 2 , Ignacio González 1 , Marcelo Galván 1
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The joint density functional theory (JDFT) is applied in the context of the grand canonical Kohn-Sham theory to calculate the global and local softness of pristine and N-substituted graphene structures. A comparison is established between the different theoretical approaches to evaluate total capacitance, revealing that the JDFT approach presents the closest result of this property with experimental data. A model of series capacitors is used to determine the quantum and nonquantum contributions of total capacitance, which enables us to determine the limitations of the rigid band approximation for the studied systems. It is found that global chemical softness is proportional to the total capacitance measured in the experiments, when the geometry relaxation is neglected. In this context, it is possible to obtain quantum and total capacitance (and consequently softness) from an average number of electrons vs applied potential plots and the model of series capacitors. Likewise, the relation of capacitance and softness gives rise to a new definition of local capacitance within the JDFT formalism. The evaluation of global and local softness paves the way to analyze electrochemical surface reactivity as a function of applied potential for a solid-electrolyte interface.
中文翻译：
在密度泛函理论大正则科恩-沙姆形式主义中建立量子电容与N掺杂石墨烯/电解质界面的柔软度之间的关系。
联合密度泛函理论（JDFT）在大正则Kohn-Sham理论的背景下应用，以计算原始和N-取代的石墨烯结构的整体和局部柔软度。建立了用于评估总电容的不同理论方法之间的比较，表明JDFT方法用实验数据提供了该特性的最接近结果。使用串联电容器模型来确定总电容的量子和非量子贡献，这使我们能够确定所研究系统的刚性带近似值的局限性。当忽略几何松弛时，发现整体化学柔软度与实验中测得的总电容成正比。在这种情况下，可以从平均电子数与施加电势图以及串联电容器的模型中获得量子和总电容（以及软度）。同样，电容和柔软度的关系在JDFT形式主义中引起了局部电容的新定义。整体和局部柔软性的评估为分析电化学表面反应性作为固体电解质界面所施加电势的函数铺平了道路。
更新日期：2020-01-10
中文翻译：
在密度泛函理论大正则科恩-沙姆形式主义中建立量子电容与N掺杂石墨烯/电解质界面的柔软度之间的关系。
联合密度泛函理论（JDFT）在大正则Kohn-Sham理论的背景下应用，以计算原始和N-取代的石墨烯结构的整体和局部柔软度。建立了用于评估总电容的不同理论方法之间的比较，表明JDFT方法用实验数据提供了该特性的最接近结果。使用串联电容器模型来确定总电容的量子和非量子贡献，这使我们能够确定所研究系统的刚性带近似值的局限性。当忽略几何松弛时，发现整体化学柔软度与实验中测得的总电容成正比。在这种情况下，可以从平均电子数与施加电势图以及串联电容器的模型中获得量子和总电容（以及软度）。同样，电容和柔软度的关系在JDFT形式主义中引起了局部电容的新定义。整体和局部柔软性的评估为分析电化学表面反应性作为固体电解质界面所施加电势的函数铺平了道路。
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