Asymmetric coordinative modulation boosting the activity and thermal stability of Pt1/CeO2 for CO oxidation under harsh condition

Abstract

Supported metal catalysts play a central role in chemical industry, but it remains a formidable challenge to realize high activity while maintaining atomically dispersed status to maximize atom efficiency under harsh conditions. Herein, a novel strategy of constructing asymmetric coordination Pt active sites via coating N-doped carbon onto ceria supported Pt single atoms (Pt₁/CeO₂@CN) is proposed, through which superior low-temperature CO oxidation activity and satisfactory thermal stability are achieved simultaneously. Experimental and density functional theory results confirm that the unique asymmetric N₂-Pt₁-O₂ coordinative configuration on Pt₁/CeO₂@CN tailors the electronic properties of Pt 5d states, increasing the turnover frequency by 15 times for CO oxidation at 120 °C compared with that on Pt₁/CeO₂ and sustaining the atomically dispersed status of Pt at as high as 400 °C under H₂-containing atmosphere. This strategy suggests a promising avenue to fabricating highly active and stable supported metal catalysts for practical applications under harsh conditions.