Confined organometallic Au1Nx single-site as an efficient bifunctional oxygen electrocatalyst. (April 2018)

• Record Type: Journal Article
• Authors: Liu, Lingyun; Su, Hui; Tang, Fumin; Zhao, Xu; Liu, Qinghua
• Is Part Of: Nano energy. Volume 46(2018)
• Page Start: 110
• Page End: 116
• Publication Date: 2018-04
• Subjects: Single-site catalysis -- Bifunctional electrocatalyst -- Oxygen reduction reaction -- Oxygen evolution reaction -- Organometallic complexes; Nanoscience -- Periodicals; Nanotechnology -- Periodicals; Nanostructured materials -- Periodicals; Power resources -- Technological innovations -- Periodicals; Nanoscience; Nanostructured materials; Nanotechnology; Power resources -- Technological innovations; Periodicals; 621.042
• DOI: 10.1016/j.nanoen.2018.01.044
• Languages: English
• ISSNs: 2211-2855

Abstract

Abstract: 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 Au1 N x 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 Au 1+ atoms are grafted onto carbon-nitride support by covalent Au–N bonds via an amine-induced-reduction strategy, forming atomic Au1 N x single-sites with potential oxygen-related catalytic activity. Hence, this developed Au1 N x single-site electrocatalyst could exhibit excellent electrocatalytic activity and durability with extraordinarily large mass activities of ~9000 AgAu −1 for ORR at the half-wave potential 0.76 V, and of ~1500 AgAu −1 for OER at overpotential 0.45 V, 20–26 times higher than those of benchmarking Pt/C and RuO2 electrocatalysts. Graphical abstract: We have designed a new type of atomic-level Au1 N x single-site confined on organic carbon-nitride as a promising bifunctional oxygen electrocatalyst. This developed atomic Au1 N x single-site electrocatalyst can achieve excellent electrocatalytic activity and durability with extraordinarily large mass activities of ~9000 AgAu −1 for ORR at the half-wave potential 0.76 V and of ~1500 AgAu −1 for OER at overpotential 0.45 V, 20–26 times those of benchmarking Pt/C and RuO2 electrocatalysts.fx1 Highlights: A new-type organometallic Au1 N x single-site is designed to realize highly efficient and durable bifunctional oxygen electrocatalytic performance. The atomic Au1 N x single-sites achieve extremely large mass activity of ~9000 and ~1500 A∙gAu −1 for oxygen reduction and evolution reaction, respectively, 20–26 times higher than those of benchmarking Pt/C and RuO2 electrocatalyst. A facile and ecofriendly "amine-induced reduction" strategy was developed to large-scale construct the atomically dispersed Au1 N x single sites. The combination of strong Au–N interaction and robust coupling effect between Au1 N x and carbon-nitride endows the atomic Au1 N x single-site with excellent redox catalytic activity and long-term durability for oxygen-involved catalysis.