We present a comprehensive understanding of sing Ru atom supported on defective graphene for water splitting using density functional theory calculations and microkinetic analysis. The structural and electronic properties of Ru atom supported single vacancy graphene (SVG), double vacancy graphene (DVG) and Stone-Wales graphene (SWG) are systematically investigated. We find that the Ru atom can be trapped effectively by the defects on each defective graphene surfaces. The binding strength of the single Ru atom onto defective graphene surfaces follows the order: [email protected] > [email protected] > [email protected] After binding, the d-band centers in [email protected], [email protected] and [email protected] are about −1.67, −1.36, −1.02 eV, respectively. We find that the reaction barrier of H₂O splitting decreases with increase of Ru d-band center. The reaction activity of H₂O splitting are as follows: [email protected] < [email protected] < [email protected] The splitting of water molecule on [email protected] surface only need a small activation energy of 0.43 eV. In addition, in the temperature range of 300–600 K, the [email protected] presents better reaction activity for H₂O splitting. The reaction rate and turnover frequency are orders of magnitude larger than that on [email protected] and [email protected] Overall, our study provides insights on the significant role of a single metal atom on defective graphene.

我们使用密度泛函理论计算和微动力学分析，对负载在有缺陷的石墨烯上的单钌原子进行水分解提供了全面的了解。系统研究了Ru原子负载的单空位石墨烯（SVG），双空位石墨烯（DVG）和Stone-Wales石墨烯（SWG）的结构和电子性能。我们发现Ru原子可以被每个有缺陷的石墨烯表面上的缺陷有效地俘获。单个Ru原子在有缺陷的石墨烯表面上的结合强度遵循以下顺序：[受电子邮件保护]> [受电子邮件保护]> [受电子邮件保护]结合后，d波段位于[受电子邮件保护]，[受电子邮件保护]和[电子邮件保护]分别约为-1.67，-1.36和-1.02 eV。我们发现H ₂的反应势垒O分裂随着Ru d带中心的增加而减小。H ₂ O裂解的反应活性如下：[受电子邮件保护] <[受电子邮件保护] <[受电子邮件保护]在[受电子邮件保护]表面分裂水分子仅需要0.43 eV的小活化能。此外，在300–600 K的温度范围内，[受电子邮件保护]对H ₂ O裂解具有更好的反应活性。反应速率和转换频率比[受电子邮件保护]和[受电子邮件保护]的数量级大。总体而言，我们的研究提供了关于单个金属原子在有缺陷的石墨烯上的重要作用的见解。