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Atomically Dispersed Iridium on Polyimide Support for Acidic Oxygen Evolution.

Longsheng ZhangJing BaiShouhan ZhangYunxia LiuJinyu YeWei FanElke DebroyeTianxi Liu
Published in: ACS nano (2024)
Designing a high-performing iridium (Ir) single-atom catalyst is desired for acidic water electrolysis, which shows enormous potential given its high catalytic activity toward acidic oxygen evolution reaction (OER) with minimum usage of precious Ir metal. However, it still remains a substantial challenge to stabilize the Ir single atoms during the OER operation without sacrificing the activity. Here, we report a high-performing OER catalyst by immobilizing Ir single atoms on a polyimide support, which exhibits a high mass activity on a carbon paper electrode while simultaneously achieving outstanding stability with negligible decay for 360 h. The resulting electrode (denoted as Ir 1 -PI@CP) reaches a 49.7-fold improvement in mass activity compared to the counterpart electrode prepared without polyimide support. Both our experimental and theoretical results suggest that, owing to the strong metal-support interactions, the polyimide support can enhance the Ir 5d states of Ir single atoms in Ir 1 -PI@CP, which can tailor the adsorption energies of intermediates and decrease the thermodynamic barrier at the rate-determining step of the OER, but also facilitate the proton-electron-transfer process and improve the reaction kinetics. This work offers an alternative avenue for developing single-atom catalysts with superior activity and durability toward various catalytic systems and beyond.
Keyphrases
  • electron transfer
  • ionic liquid
  • molecular dynamics
  • carbon nanotubes
  • metal organic framework
  • risk assessment
  • gold nanoparticles
  • density functional theory
  • climate change
  • carbon dioxide
  • aqueous solution