Constructing Solid–Gas-Interfacial Fenton Reaction over Alkalinized‑C3N4 Photocatalyst To Achieve Apparent Quantum Yield of 49% at 420 nm

• Published in: Journal of the American Chemical Society Vol. 138; no. 40; pp. 13289 - 13297
• Main Authors: Li, Yunxiang, Ouyang, Shuxin, Xu, Hua, Wang, Xin, Bi, Yingpu, Zhang, Yuanfang, Ye, Jinhua
• Format: Journal Article
• Language: English
• Published: American Chemical Society 12.10.2016
• Subjects: air pollution; carbon nitride; electron paramagnetic resonance spectroscopy; electrons; energy; hydrogen peroxide; iron; oxidation; photocatalysis; photocatalysts; photolysis; pollutants; remediation; solar energy; volatile organic compounds
• ISSN: 0002-7863; 1520-5126; 1520-5126
• DOI: 10.1021/jacs.6b07272

Efficient generation of active oxygen-related radicals plays an essential role in boosting advanced oxidation process. To promote photocatalytic oxidation for gaseous pollutant over g-C3N4, a solid–gas interfacial Fenton reaction is coupled into alkalinized g-C3N4-based photocatalyst to effectively convert photocatalytic generation of H2O2 into oxygen-related radicals. This system includes light energy as power, alkalinized g-C3N4-based photocatalyst as an in situ and robust H2O2 generator, and surface-decorated Fe3+ as a trigger of H2O2 conversion, which attains highly efficient and universal activity for photodegradation of volatile organic compounds (VOCs). Taking the photooxidation of isopropanol as model reaction, this system achieves a photoactivity of 2–3 orders of magnitude higher than that of pristine g-C3N4, which corresponds to a high apparent quantum yield of 49% at around 420 nm. In-situ electron spin resonance (ESR) spectroscopy and sacrificial-reagent incorporated photocatalytic characterizations indicate that the notable photoactivity promotion could be ascribed to the collaboration between photocarriers (electrons and holes) and Fenton process to produce abundant and reactive oxygen-related radicals. The strategy of coupling solid–gas interfacial Fenton process into semiconductor-based photocatalysis provides a facile and promising solution to the remediation of air pollution via solar energy.