The development of novel synthesis technologies is essential to expand the use of bifunctional electrocatalysts for energy-efficient hydrogen production. Based on this,Professor Fu Gengtao of Nanjing Normal University, researcher Sun Kang of Chinese Academy of Forestry (co-corresponding author) and othersA series of carbon-based rare earth (RE) oxides (GD2O3, SM2O3, EU2O3 and CEO2) were constructed using a rare earth metal-organic framework, and the ORR performance of the PD site was adjusted through the PD-Rexoy interface interaction.
Represented by PD-GD2O3C, it is found that the strong coupling between PD and GD2O3 induces the formation of a PD-O-GD bridge, which triggers the charge redistribution of PD and GD2O3. The screened PD-GD2O3 C has a high starting potential (0.).986 vrhe), half-wave potential (0877 VRHE) and good stability with excellent ORR performance. Similar ORR results were obtained for the PD-SM2O3C, PD-EU2O3C, and PD-CEO2C catalysts.
Theoretical analysis shows that the coupling between PD and GD2O3 promotes electron transfer through the PD-O-GD bridge, thereby inducing the occupation of the antibond orbital of PD-*OH and thus optimizing the adsorption of *OH in the ORR rate-determining step. The pH-dependent microdynamics model showed that PD-GD2O3 was close to the theoretical optimal activity of ORR and better than PT under the same conditions. Due to its advantages in ORR, PD-GD2O3C has shown excellent performance as an air cathode material in zinc-air batteries, which indicates that it has good practicability.
importing antibonding-orbital occupancy through pd-o-gd bridge promotes electrocatalytic oxygen reduction. angew. chem. int. ed.,, doi: 10.1002/anie.202314565.