Tailoring the Electronic Structure of Transition Metals by the V₂C MXene Support: Excellent Oxygen Reduction...

The enhancement of oxygen reduction reaction (ORR) activity can significantly boost the performance of fuel cells. MXene-supported transition metals with strong metal-support interactions (SMSI) are an effective strategy to increase the catalytic activity and durability while decreasing the usage of noble metals. Herein, a series of composites of transition-metal atoms (Ni, Pd, Pt, Cu, Ag, and Au) deposited on V₂C MXene are designed as potential catalysts for ORR using density functional theory. The calculation results demonstrate that all the transition metals prefer to form a monolayer on V₂C (TM_ML/V₂C) with high thermodynamic stability because of SMSI, in which the Pd, Pt, Ag, and Au monolayers exhibit high chemical stability during the ORR process. Pt_ML/V₂C exhibits the highest activity toward ORR with the overpotential down to 0.38 V and the largest energy barrier of 0.48 eV. The excellent catalytic performance originates from the modification of the electronic structure by the V₂C support because of SMSI. Our studies elucidate the SMSI between transition-metal atoms and V₂C MXene from the atomic level and thus rationally design the ORR catalyst at the cathode of fuel cells to enhance the activity while possessing high stability and less Pt usage.