The Innovation (Feb 2021)

Controllable Generation of Reactive Oxygen Species on Cyano-Group-Modified Carbon Nitride for Selective Epoxidation of Styrene

  • Hao Tan,
  • Peng Kong,
  • Riguang Zhang,
  • Mengting Gao,
  • Meixian Liu,
  • Xianmo Gu,
  • Weifeng Liu,
  • Zhanfeng Zheng

Journal volume & issue
Vol. 2, no. 1
p. 100089

Abstract

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Summary: The controlled generation of reactive oxygen species (ROS) to selectively epoxidize styrene is a grand challenge. Herein, cyano-group-modified carbon nitrides (CNCYx and CN-Ty) are prepared, and the catalysts show better performance in regulating ROS and producing styrene oxide than the cyano-free sample. The in situ diffuse reflectance infrared and density functional theory calculation results reveal that the cyano group acts as the adsorption and activation site of oxygen. X-ray photoelectron spectroscopy and NMR spectrum results confirm that the cyano group bonds with the intact heptazine ring. This unique structure could inhibit H2O2 and ⋅OH formation, resulting in high selectivity of styrene oxide. Furthermore, high catalytic activity is still achieved when the system scales up to 2.7 L with 100 g styrene under solar light irradiation. The strategy of cyano group modification gives a new insight into regulating spatial configuration for tuning the utilization of oxygen-active species and shows potential applications in industry.

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