Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH r...Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range.Herein,we fabricate surface Co defect-rich spinel ZnCo_(2)O_(4)porous nanosheets,which can generate≡CoIV=O and 1O2 over a wide pH range of 3.81-10.96 by the formation of amphoteric≡Zn(OH)2 in peroxymonosulfate(PMS)activation process.Density functional theory(DFT)calculations show Co defect-rich ZnCo_(2)O_(4)possesses much stronger adsorption ability and more electron transfer to PMS.Moreover,the adsorption mode changes from terminal oxygen Co-O-Co to Co-O,accelerating the polarization of adjacent oxygen,which is beneficial to the generation of≡CoIV=O and 1O2.Co defect-rich ZnCo_(2)O_(4)porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol(PNP)degradation,whose toxicity of degradation intermediates is significant reduction.The Co defect-rich ZnCo_(2)O_(4)nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93%over 10 h.This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.展开更多
基金supported by the National Natural Science Foundation of China(NSFC)(No.22308336).
文摘Heterogeneous advanced oxidation processes(AOPs)based on non-radical reactive species are considered as a powerful technology for wastewater purification due to their long half-lives and high adaptation in a wide pH range.Herein,we fabricate surface Co defect-rich spinel ZnCo_(2)O_(4)porous nanosheets,which can generate≡CoIV=O and 1O2 over a wide pH range of 3.81-10.96 by the formation of amphoteric≡Zn(OH)2 in peroxymonosulfate(PMS)activation process.Density functional theory(DFT)calculations show Co defect-rich ZnCo_(2)O_(4)possesses much stronger adsorption ability and more electron transfer to PMS.Moreover,the adsorption mode changes from terminal oxygen Co-O-Co to Co-O,accelerating the polarization of adjacent oxygen,which is beneficial to the generation of≡CoIV=O and 1O2.Co defect-rich ZnCo_(2)O_(4)porous nanosheets exhibit highly active PMS activation activity and stability in p-nitrophenol(PNP)degradation,whose toxicity of degradation intermediates is significant reduction.The Co defect-rich ZnCo_(2)O_(4)nanosheet catalyst sponge/PMS system achieved stable and efficient removal of PNP with a removal efficiency higher than 93%over 10 h.This work highlights the development of functional catalyst and provides an atomic-level understanding into non-radical PMS activation process in wastewater treatment.
