论文标题
比较密度的功能理论研究，用于预测单原子催化剂的氧还原活性
Comparative density functional theory study for predicting oxygen reduction activity of single-atom catalyst
论文作者
论文摘要
已经很好地确定，氮协调的过渡金属TM-N $ _ {4} $ - C（TM $ = $ = $ fe and Co和Co）是负责较高的催化活性，用于降低电化学还原反应。但是，使用密度函数理论计算获得的结果因多一种而异，这可能导致争议。 Herein, we assess the accuracy of the theoretical approach using different class of exchange-correlation functionals, i.e., Perdew-Burke-Ernzerhof (PBE) and revised PBE (RPBE), those with the Grimme's semiempirical dispersion correction (PBE+D3 and RPBE+D3), and the Bayesian error estimate functional with the nonlocal correlation (BEEF-vdW) on the在石墨烯和OH终止的TM-N $ _ {4} $部分上氧还原反应的反应能量。我们发现，使用RPBE+D3的预测过电势与使用牛肉VDW的预测相当，并且是一致的。我们的发现表明，正确选择交换相关功能对于对该系统的催化活性的精确描述至关重要。
It has been well established that nitrogen coordinated transition metal, TM-N$_{4}$-C (TM$=$Fe and Co) moieties, are responsible for the higher catalytic activity for the electrochemical oxygen reduction reaction. However, the results obtained using density functional theory calculations vary from one to another, which can lead to controversy. Herein, we assess the accuracy of the theoretical approach using different class of exchange-correlation functionals, i.e., Perdew-Burke-Ernzerhof (PBE) and revised PBE (RPBE), those with the Grimme's semiempirical dispersion correction (PBE+D3 and RPBE+D3), and the Bayesian error estimate functional with the nonlocal correlation (BEEF-vdW) on the reaction energies of oxygen reduction reaction on TM-N$_{4}$ moieties in graphene and those with OH-termination. We found that the predicted overpotentials using RPBE+D3 are comparable and consistent with those using BEEF-vdW. Our finding indicates that a proper choice of the exchange-correlation functional is crucial to a precise description of the catalytic activity of this system.
