Understanding the synergistic catalysis effect on the dual-metal-N4 embedding single-walled carbon nanotubes from first principles

Abstract

Developing high-efficiency electrocatalysts for the oxygen evolution reaction (OER) remains a crucial bottleneck on the way to the water splitting for producing clean fuel (H2). Compared with single atom catalysis (SACs), dual-atom catalysts (DACs) have attracted great interest due to higher OER catalytic efficiency. In this work, the OER properties of dual-metal-N4 embedding armchair single-walled carbon nanotubes (D-MN4/CNTs) were systematic studied by density functional theory (DFT) simulations. Our results indicate that CoN4 embedding armchair CNTs exhibit higher OER activity than the corresponding planar structure, especially for CoN4 embedding in armchair CNT (4, 4) (CNT4). For MN4-CoN4 co-embedding CNTs, the TiN4-CoN4/CNTs have good OER synergistic effect with the lowest overpotential. Besides, the diameter of CNTs have a significant impact on the OER efficiency. The lowest reaction overpotential 0.47 V were obtained in TiN4-CoN4/CNT4 with a 5.69 Å tube diameter. Interestingly, compressive stress will further enhance the synergistic effect between two metal atoms in the OER reaction. The OER overpotential of CoN4-TiN4 embedding armchair CNT4 can reduce to 0.40 V under the −4 % uniaxial compression strain. These works were expected to better understand the synergistic mechanisms and design high-efficiency dual-atom OER electrocatalysts.