Cu Atom Regulated AuPtCu@T‐Cu <sub>x</sub> S Janus Heterostructure Electrocatalyst for High‐Performance Lithium‐Oxygen Batteries
Yingjian Nie, Jiafeng Li, Luyuan Zhang, Chunxia Li, Boya Zhang, Zhiwei Zhang, Longwei Yin
Abstract
Abstract The Janus heterostructure containing two disparate functional components can be well adopted as electrocatalyst for lithium‐oxygen batteries (LOBs), whose asymmetrical discharge/charge electrochemical process and low oxygen reduction and oxygen evolution reaction (ORR/OER) kinetics result in poor round‐trip efficiency. Herein, an efficient copper atom modulation strategy is developed to construct well‐designed Cu‐deficient T‐Cu x S nanoparticles (Cu 1.75 S treated at high temperature), paired with AuPtCu nanoalloy (AuPtCu@T‐Cu x S), serving as bifunctional cathode electrocatalysts to accelerate ORR/OER kinetics of LOBs. The abundant coordination unsaturated sites on the surface of T‐Cu x S can be viewed as the anchoring center of AuPt, and also can be efficient catalytic sites for the ORR/OER kinetics. The internal electric field modulates the electronic structure and d‐band center of the Cu and Pt atoms, optimizes the interaction between the AuPtCu@T‐Cu x S and the intermediate LiO 2 , regulating the growth mode of the Li 2 O 2 . As expected, LOBs based on AuPtCu@T‐Cu x S catalyst delivers a minimal overpotential (0.56 V) and long‐term cyclability (590 cycles, 500 mA g −1 ) at 1000 mAh g −1 , exceeding most state‐of‐the‐art Janus electrocatalysts. This work affords significant insights for atomic and electronic structure optimization of Janus heterostructures for LOBs.