Photoinduced synergistic catalysis on Zn single-atom-loaded hierarchical porous carbon for highly efficient CO2 cycloaddition conversion

Abstract

The use of solar energy to drive efficient CO₂ cycloaddition conversion under mild reaction conditions is highly desired but remains a significant challenge. In this communication, a Zn single-atom-loaded N-doped carbon (Zn SA-NC) is facilely synthesized via direct pyrolysis of N-rich energetic MOFs. Because of a multiple light reflection effect, the obtained Zn SA-NC with a hierarchical porous structure shows an ultrahigh light-harvesting efficiency of >97% in a broadband range (250–2500 nm). The photogenerated electrons and photothermal effects can synergistically catalyze CO₂ cycloaddition reaction with Zn–N₄ as the main active sites. When faced with various epoxides, Zn SA-NC shows high catalytic activity with almost complete CO₂ cycloaddition conversion yields. It is assumed that this study has provided some unprecedented findings for the future design and application of single-atom catalysts in photoinduced CO₂ cycloaddition catalysis or other catalytic reactions.