Probing Metal/High-Entropy Perovskite Heterointerface for Efficient and Sustainable CO2 Electroreduction

Abstract

Solid oxide electrolysis cells (SOECs) are increasingly recognized for their great potential in carbon dioxide reduction reaction (CO2RR). However, the sluggish kinetics of CO2RR impedes their widespread commercialization. Here, a novel in-situ formed metal/high-entropy perovskite heterointerface, NiFe@Sr2Fe0.4V0.4Mo0.4Ni0.4Ti0.6O6-δ (SFVMNT), is proposed to enhance CO2RR. The electronic conductivity of NiFe@SFVMNT is one order of magnitude higher than that of Sr2FeMoO6-δ perovskite. Theoretical analyses reveal that the strong metal/perovskite interaction significantly accelerate CO2RR kinetics. Moreover, the NiFe@SFVMNT with its high-entropy configuration and embedded exsolution structure ensures high stability during continuous CO2RR. As an application, the NiFe@SFVMNT-based SOECs demonstrates an impressive current density of 1.66 A cm-2 at 1.5 V and 800 °C, maintaining nearly consistent performance over 200 h, thereby surpassing most state-of-the-art cathode materials for CO2RR. Consequently, this metal/high-entropy perovskite interface emerges as a highly efficient and durable cathode of SOECs towards CO2RR.