Anisotropic Surface Modulation of Pt Catalysts for Highly Reversible Li–O₂ Batteries: High Index Facet as a Critical Descriptor

The surface structure of solid catalysts has been regarded as a critical descriptor for determining the catalytic activities in various applications. However, structure-dependent catalytic activities have been rarely understood for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) within Li-O2 batteries. Here, we succeeded in the preparation of a Pt catalyst with an anisotropic structure and demonstrated its high catalytic activity in non-aqueous Li-O2 batteries. The cathode incorporating Pt exposed with high-index {411} facets showed greatly enhanced ORR and OER performance in comparison to commercial Pt/C cathode. The anisotropic Pt catalyst improved ORR activity with a large capacity of 12,985 mAh gcarbon-1, high rate performance, and stable cyclic retention up to 70 cycles with the capacity limited to 1,000 mAh gcarbon-1 of capacity. Furthermore, the anisotropic Pt catalyst exhibited high round-trip efficiency of ~87% with a low OER potential (3.1 V) at a current density of 200 m...