Construction of N-doped carbon frames anchored with Co single atoms and Co nanoparticles as robust electrocatalyst for hydrogen evolution in the entire pH range

The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction (HER) in the entire pH range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames (NCFs) anchored with Co single atoms (SAs) and Co nanoparticles (NPs) catalyst by a doping-adsorption-pyrolysis strategy for elec-trocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhi-bits a superior HER performance in the entire pH range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N3 coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H2O molecule is easily activated and dissoci-ated on Co NPs, while the generated H* is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H2O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application. (c) 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

Automated summary

A highly dispersed N-doped carbon frames (NCFs) catalyst anchored with Co single atoms (SAs) and Co nanoparticles (NPs) was synthesized for efficient electrocatalytic hydrogen evolution, exhibiting excellent HER activity with small overpotential, low Tafel slope, high turnover frequency, and remarkable stability across the entire pH range. The synergy between Co SAs with Co-N3 coordination structure and Co NPs promotes H2O activation and dissociation for enhanced HER performance, providing a novel strategy for constructing high-efficiency HER electrocatalysts with atomic-level precision.