Realizing a high OER activity in new single-atom catalysts formed by introducing TMN x ( x = 3 and 4) units into carbon nanotubes using high-throughput calculations.

Exploring highly efficient electrocatalysts for the oxygen evolution reaction (OER) is of great significance for hydrogen production through water splitting. By means of high-throughput density functional theory (DFT) calculations, we investigated the OER catalytic activity of a series of one-dimensional carbon nanotube (CNT)-based systems containing TMN 4 or TMN 3 functional units. Through the screening of 3d/4d/5d transition metals (TMs) from Group IVB to Group VIII, eight newly obtained TMN x @CNT ( x = 3 and 4) systems were found to exhibit excellent OER activity, with very low overpotentials in the range 0.29-0.51 V, where the Co, Rh, Ir, Ti, Fe, and Ru atoms could be used as active sites. It was found that under the framework of TMN 3 @CNTs, the pre-adsorption of some species from water dissociation on the relevant TM sites (TM = Ti, Fe, and Ru) could lead to a high OER catalytic activity, which was different from the general situation where OER reactions directly occur on the clean surfaces of the remaining systems with Co/Rh/Ir metal centers. Moreover, the catalytic mechanisms were analyzed in detail. This work can be conducive to obtaining low-cost and high-performance OER single-atom electrocatalysts based on excellent CNT nanomaterials.