To better understand the mechanisms of hydrogen peroxide(H_(2)O_(2))’s decomposition and reactive oxygen species(ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental applicati...To better understand the mechanisms of hydrogen peroxide(H_(2)O_(2))’s decomposition and reactive oxygen species(ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental application of Fenton/Fenton-like reaction.We here report a new approach to activate H_(2)O_(2) in a co-catalytic Fenton system with oxygen incorporated MoS2,namely MoS_(2−x) O_(x) nanosheets.The MoS_(2−x) O_(x) nanosheets assisted co-catalytic Fenton system exhibited superior degradation activity of emerging antibiotic contaminants(e.g.,sulfamethoxazole).Combining density functional theory(DFT)calculation and experimental investigation,we demonstrated that oxygen incorporation could improve the intrinsic conductivity of MoS_(2−x) O_(x) nanosheets and accelerate surface/interfacial charge transfer,which further leads to the efficacious activation of H_(2)O_(2).Moreover,by tuning the oxygen proportion in MoS_(2−x) O_(x) nanosheets,we are able to modulate the generation of ROS and further direct the oriented-conversion of H_(2)O_(2) to surface-bounded superoxide radical(·O_(2−surface)).It sheds light on the generation and transformation of ROS in the engineered system(e.g.,Fenton,Fenton-like reaction)for efficient degradation of persistent pollutants.展开更多
基金the National Natural Science Foundation of China(Nos.42077293 and 22006088)Natural Science Foundation of Guangdong Province(Nos.2019A1515011692 and 2019QN01L797)+2 种基金Shenzhen Municipal Science and Technology Innovation Committee(Nos.JCYJ20190809181413713 and WDZC20200817103015002)Y.X.H.also thanks the financial support from Overseas Cooperation Research Fund of Tsinghua Shenzhen International Graduate School(Nos.HW2020002 and QD2021010N)This work was also supported by the China Postdoctoral Science Foundation(No.2019M66067).
文摘To better understand the mechanisms of hydrogen peroxide(H_(2)O_(2))’s decomposition and reactive oxygen species(ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental application of Fenton/Fenton-like reaction.We here report a new approach to activate H_(2)O_(2) in a co-catalytic Fenton system with oxygen incorporated MoS2,namely MoS_(2−x) O_(x) nanosheets.The MoS_(2−x) O_(x) nanosheets assisted co-catalytic Fenton system exhibited superior degradation activity of emerging antibiotic contaminants(e.g.,sulfamethoxazole).Combining density functional theory(DFT)calculation and experimental investigation,we demonstrated that oxygen incorporation could improve the intrinsic conductivity of MoS_(2−x) O_(x) nanosheets and accelerate surface/interfacial charge transfer,which further leads to the efficacious activation of H_(2)O_(2).Moreover,by tuning the oxygen proportion in MoS_(2−x) O_(x) nanosheets,we are able to modulate the generation of ROS and further direct the oriented-conversion of H_(2)O_(2) to surface-bounded superoxide radical(·O_(2−surface)).It sheds light on the generation and transformation of ROS in the engineered system(e.g.,Fenton,Fenton-like reaction)for efficient degradation of persistent pollutants.
