Guided Heterostructure Growth of CoFe LDH on Ti3C2Tx MXene for Durably High Oxygen Evolution Activity

Abstract Heterostructures of layered double hydroxides (LDHs) and MXenes have shown great promise for oxygen evolution reaction (OER) catalysts, owing to their complementary physical properties. Coupling LDHs with MXenes can potentially enhance their conductivity, stability, and OER activity. In this work, a scalable and straightforward in situ guided growth of CoFeLDH on Ti 3 C 2 T x is introduced, where the surface chemistry of Ti 3 C 2 T x dominates the resulting heterostructures, allowing tunable crystal domain sizes of LDHs. Combined simulation results of Monte Carlo and density functional theory (DFT) validate this guided growth mechanism. Through this way, the optimized heterostructures allow the highest OER activity of the overpotential = 301 mV and Tafel slope = 43 mV dec −1 at 10 mA cm −2 , and a considerably durable stability of 0.1% decay over 200 h use, remarkably outperforming all reported LDHs‐MXenes materials. DFT calculations indicate that the charge transfer in heterostructures can decrease the rate‐limiting energy barrier for OER, facilitating OER activity. The combined experimental and theoretical efforts identify the participation role of MXene in heterostructures for OER reactions, providing insights into designing advanced heterostructures for robust OER electrocatalysis.