Confined organometallic Au1Nx single-site as an efficient bifunctional oxygen electrocatalyst

The development of organometallic complexes with abundant stable single-atom active sites is highly desirable for cost-effective and commercial electrocatalysis towards renewable energy conversion and storage. Here, we report an atomic-level design and construction of a new type of organometallic Au1Nx single-site confined on organic carbon-nitride support as a promising bifunctional electrocatalyst for efficient and durable oxygen reduction (ORR) and evolution reaction (OER) performance. The combination of atomic characterizations and theoretical calculations confirm that the atomically dispersed Au1+ atoms are grafted onto carbon-nitride support by covalent Au-N bonds via an amine-induced-reduction strategy, forming atomic Au1Nx single-sites with potential oxygen-related catalytic activity. Hence, this developed Au1Nx single-site electrocatalyst could exhibit excellent electrocatalytic activity and durability with extraordinarily large mass activities of similar to 9000 A center dot g(Au)(-1) for ORR at the half-wave potential 0.76 V, and of similar to 1500A center dot g(Au)(-1) for OER at overpotential 0.45 V, 20-26 times higher than those of benchmarking Pt/C and RuO2 electrocatalysts.