High-performance single-atom Ni catalyst loaded graphyne for H2O2 green synthesis in aqueous media

A high-performance Single-Atom Ni Catalyst Loaded Graphyne was screened by utilizing density functional theory calculations. [Display omitted] The electrochemical synthesis of hydrogen peroxide (H2O2) provides a greener and more efficient method compared with classic catalysts containing toxic metals. Herein, we used first-principles density functional theory (DFT) calculations to investigate 174 different single-atom catalysts with graphyne substrates, and conducted a three-step screening strategy to identify the optimal noble metal-free single atom catalyst. It is found that a single Ni atom loaded on γ-graphyne with carbon vacancies (Ni@V-γ-GY) displayed remarkable thermodynamic stability, excellent selectivity, and high activity with an ultralow overpotential of 0.03 V. Furthermore, based on ab-initio molecular dynamic and DFT calculations under the H2O solvent, it was revealed that the catalytic performance for H2O2 synthesis in aqueous phase was much better than that in gas phase condition, shedding light on the hydrogen bond network being beneficial to accelerate the transfer of protons for H2O2 synthesis.