High-Throughput Screening Strategy for Electrocatalysts for Selective Catalytic Oxidation of Formaldehyde to Formic Acid

Electrocatalytic oxidation of formaldehyde (FOR) is an effective way to prevent the damage caused by formaldehyde and produce high-value products. A screening strategy of a single-layer MnO₂-supported transition metal catalyst for the selective oxidation of formaldehyde to formic acid was designed by high-throughput density functional calculation. N-MnO₂@Cu and MnO₂@Cu are predicted to be potential FOR electrocatalysts with potential-limiting steps (PDS) of 0.008 and -0.009 eV, respectively. Electronic structure analysis of single-atom catalysts (SACs) shows that single-layer MnO₂ can regulate the spin density of loaded transition metal and thus regulate the adsorption of HCHO (E_ad), and E_ad is volcanically distributed with the magnetic moment descriptor -|m_M - m_H|. In addition, the formula quantifies E_ad and |m_M - m_H| to construct a volcano-type descriptor α describing the PDS [ΔG(*CHO)]. Other electronic and structural properties of SACs and α are used as input features for the GBR method to construct machine learning models predicting the PDS (R² = 0.97). This study hopes to provide some insights into FOR electrocatalysts.