Coaxial Metal-Nitrogen–Carbon Single-Atom Catalysts Boost Acid Hydrogen Peroxide Production
Hongshang Hu#, Chang Zhang#, Wei Liu, Huiyao Qi, Haoyu Wang, Xinyu Wang, Lilong Zhang, Lei Liu, Lipiao Bao, Muneerah Alomar, Jian Zhang,* and Xing Lu*
Adv. Funct. Mater. 2024, 2419220
https://doi.org/10.1002/adfm.202419220
Abstract
Electrosynthesis of hydrogen peroxide (H2O2) by two-electron oxygen reduction reaction (2e− ORR) under acidic conditions is promising. However, constructing a highly efficient acid-resistant 2e− ORR electrocatalyst is critical but challenging. Herein, a coaxial cobalt single-atom catalyst on carbon nanotubes (CoSA-N-C/CNTs) is designed and synthesized by an ingenious separation chemical vapor deposition (SCVD) strategy, which achieves higher ORR activity, dominated 2e− selectivity, and superior stability in acid, compared to the counterpart nanoparticle catalyst prepared by traditional mixture pyrolysis. The as-assembled electrode using CoSA-N-C/CNTs catalyst demonstrates a high H2O2 yield in excess of 2000 mmol gcat−1 h−1 with a Faraday efficiency of >90% over 100 h without decay in a flow cell, as superior to the most reported acidic H2O2 production catalysts. Experimental characterization and theoretical calculations reveal that such excellent 2e− ORR performance of CoSA-N-C/CNTs originate from the combined advantages of strongly coupled coaxial core–shell structure and highly dispersed single-atom property. Most importantly, a series of other coaxial transition metal single-atom catalysts (MSA-N-C/CNTs, M = Fe, Cu, or Ni) are prepared through this SCVD strategy, and they all show enhanced ORR performance, demonstrating universality.
