Homogeneous Carbon Dot-Anchored Fe(III) Catalysts with Self-Regulated Proton Transfer for Recyclable Fenton Chemistry
Ting Zhang, Zhelun Pan, Jianying Wang, Xufang Qian, Hiromi Yamashita, Zhenfeng Bian, Yixin Zhao
Abstract
High Resolution Image Download MS PowerPoint Slide Fenton chemistry has been widely studied in a broad range from geochemistry, chemical oxidation to tumor chemodynamic therapy. It was well established that Fe 3+ /H 2 O 2 resulted in a sluggish initial rate or even inactivity. Herein, we report the homogeneous carbon dot-anchored Fe(III) catalysts (CD-COOFe III ) wherein CD-COOFe III active center activates H 2 O 2 to produce hydroxyl radicals ( • OH) reaching 105 times larger than that of the Fe 3+ /H 2 O 2 system. The key is the • OH flux produced from the O–O bond reductive cleavage boosting by the high electron-transfer rate constants of CD defects and its self-regulated proton-transfer behavior probed by operando ATR-FTIR spectroscopy in D 2 O and kinetic isotope effects, respectively. Organic molecules interact with CD-COOFe III via hydrogen bonds, promoting the electron-transfer rate constants during the redox reaction of CD defects. The antibiotics removal efficiency in the CD-COOFe III /H 2 O 2 system is at least 51 times large than the Fe 3+ /H 2 O 2 system under equivalent conditions. Our findings provide a new pathway for traditional Fenton chemistry.