Copper-catalyzed activation of molecular oxygen for oxidative destruction of acetaminophen: The mechanism and superoxide-mediated cycling of copper species.
In this study, the commercial zero-valent copper (ZVC) was investigated to activate the molecular oxygen (O2) for the degradation of acetaminophen (ACT). 50 mg/L ACT could be completely decomposed within 4 h in the ZVC/air system at initial pH 3.0. The H2O2, hydroxyl radical (OH) and superoxide anion radical (O2-) were identified as the main reactive oxygen species (ROSs) generated in the above reaction; however, only OH caused the decomposition and mineralization of ACT in the copper-catalyzed O2activation process. In addition, the in-situ generated Cu+from ZVC dissolution not only activated O2to produce H2O2, but also initiated the decomposition of H2O2to generate OH. Meanwhile, the H2O2could also be partly decomposed into O2-, which served as a mediator for copper cycling by reduction of Cu2+to Cu+in the ZVC/air system. Therefore, OH could be continuously generated; and then ACT was effectively degraded. Additionally, the effect of solution pH and the dosage of ZVC were also investigated. As a result, this study indicated the key behavior of the O2-during Cu-catalyzed activation of O2, which further improved the understanding of O2activation mechanism by zero-valent metals.
National Engineering Research Center for Urban Pollution Control, State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 200092 Shanghai, PR China; Department of Environmental Engineering, College of Chemistry and Environmental Engineering, Shenzhen University, 518060 Shenzhen, PR China.
Yunfei
Y
Zhang
National Engineering Research Center for Urban Pollution Control, State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 200092 Shanghai, PR China. Electronic address: jinhongfan@tongji.edu.cn.
Jinhong
J
Fan
Department of Environmental Engineering, College of Chemistry and Environmental Engineering, Shenzhen University, 518060 Shenzhen, PR China. Electronic address: boyang@szu.edu.cn.
Bo
B
Yang
National Engineering Research Center for Urban Pollution Control, State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 200092 Shanghai, PR China.
Wutao
W
Huang
National Engineering Research Center for Urban Pollution Control, State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, 200092 Shanghai, PR China.
Luming
L
Ma
D000082:Acetaminophen / Q000737:chemistry*; D000332:Aerobiosis; D001673:Biodegradation, Environmental; D002384:Catalysis; D003300:Copper / Q000737:chemistry*; D006861:Hydrogen Peroxide / Q000737:chemistry*; D006863:Hydrogen-Ion Concentration; D017665:Hydroxyl Radical / Q000737:chemistry; D010084:Oxidation-Reduction; D010100:Oxygen / Q000737:chemistry*; D017382:Reactive Oxygen Species / Q000378:metabolism; D012996:Solutions; D013481:Superoxides / Q000737:chemistry*; D014961:X-Ray Diffraction
D017382:Reactive Oxygen Species; D012996:Solutions; D013481:Superoxides; D017665:Hydroxyl Radical; D000082:Acetaminophen; D003300:Copper; D006861:Hydrogen Peroxide; D010100:Oxygen
Acetaminophen; Activation molecular oxygen; Oxidative destruction; Superoxide anion radical; Zero-valent copper