Search for: All records

Electrochemical two-electron water oxidation reaction (2e-WOR) has drawn significant attention as a promising process to achieve the continuous on-site production of hydrogen peroxide (H₂O₂). However, compared to the cathodic H₂O₂generation, the anodic 2e-WOR is more challenging to establish catalysts due to the severe oxidizing environment. In this study, we combine density functional theory (DFT) calculations with experiments to discover a stable and efficient perovskite catalyst for the anodic 2e-WOR. Our theoretical screening efforts identify LaAlO₃perovskite as a stable, active, and selective candidate for catalyzing 2e-WOR. Our experimental results verify that LaAlO₃achieves an overpotential of 510 mV at 10 mA cm⁻²in 4 M K₂CO₃/KHCO₃, lower than those of many reported metal oxide catalysts. In addition, LaAlO₃maintains a stable H₂O₂Faradaic efficiency with only a 3% decrease after 3 h at 2.7 V vs. RHE. This computation-experiment synergistic approach introduces another effective direction to discover promising catalysts for the harsh anodic 2e-WOR towards H₂O₂.

The emergence of ferromagnetism in materials where the bulk phase does not show any magnetic order demonstrates that atomically precise films can stabilize distinct ground states and expands the phase space for the discovery of materials. Here, the emergence of long-range magnetic order is reported in ultrathin (111) LaNiO₃(LNO) films, where bulk LNO is paramagnetic, and the origins of this phase are explained. Transport and structural studies of LNO(111) films indicate that NiO₆octahedral distortions stabilize a magnetic insulating phase at the film/substrate interface and result in a thickness-dependent metal–insulator transition att = 8 unit cells. Away from this interface, distortions relax and bulk-like conduction is regained. Synchrotron x-ray diffraction and dynamical x-ray diffraction simulations confirm a corresponding out-of-plane unit-cell expansion at the interface of all films. X-ray absorption spectroscopy reveals that distortion stabilizes an increased concentration of Ni²⁺ions. Evidence of long-range magnetic order is found in anomalous Hall effect and magnetoresistance measurements, likely due to ferromagnetic superexchange interactions among Ni²⁺–Ni³⁺ions. Together, these results indicate that long-range magnetic ordering and metallicity in LNO(111) films emerges from a balance among the spin, charge, lattice, and orbital degrees of freedom.