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 ^(1)O_(2) 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 Generating ^(1)O_(2) .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
The two-dimensional(2D)nanosheet zinc cobaltate(ZnCo_(2)O_(4))was added into polyether block amide(Pebax)matrix to prepare mixing matrix membrane(MMM)for separating carbon dioxide(CO_(2))/methane(CH4)gas mixture.The 2...The two-dimensional(2D)nanosheet zinc cobaltate(ZnCo_(2)O_(4))was added into polyether block amide(Pebax)matrix to prepare mixing matrix membrane(MMM)for separating carbon dioxide(CO_(2))/methane(CH4)gas mixture.The 2D porous ZnCo_(2)O_(4)nanosheets were composed of chemically interconnected metal oxide nanoparticles.The ZnCo_(2)O_(4)nanoparticles in the nanosheets constructed large-quantity pores of 11.78 nm and provided abundant transfer channels for gas molecule.Moreover,the synergistic effect of bimetallic Zn^(2+)and Co^(2+)would promote the generation of oxygen vacancies(Oδ-),which could provide more CO_(2)(Cδ+)adsorption sites,thereby increased the selectivity of the membrane.The large aspect ratio of the ultra-thin ZnCo_(2)O_(4)nanosheets showed better dispersion in the membrane.The pure gas separation performance data showed the CO_(2)permeability and CO_(2)/CH4 selectivity of Pebax/ZnCo_(2)O_(4)membrane were 139.10 Barrer and 15.38,respectively,when the filling amount was 0.5 wt%.Compared with pure Pebax membrane,the separation performance(permeability and selectivity)were increased with 165.67%and 75.57%,respectively.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 ^(1)O_(2) 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 Generating ^(1)O_(2) .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.
基金the National High Technology Research and Development Program of China(2012AA03A611)the National Natural Science Foundation of China,grant No.21868031.
文摘The two-dimensional(2D)nanosheet zinc cobaltate(ZnCo_(2)O_(4))was added into polyether block amide(Pebax)matrix to prepare mixing matrix membrane(MMM)for separating carbon dioxide(CO_(2))/methane(CH4)gas mixture.The 2D porous ZnCo_(2)O_(4)nanosheets were composed of chemically interconnected metal oxide nanoparticles.The ZnCo_(2)O_(4)nanoparticles in the nanosheets constructed large-quantity pores of 11.78 nm and provided abundant transfer channels for gas molecule.Moreover,the synergistic effect of bimetallic Zn^(2+)and Co^(2+)would promote the generation of oxygen vacancies(Oδ-),which could provide more CO_(2)(Cδ+)adsorption sites,thereby increased the selectivity of the membrane.The large aspect ratio of the ultra-thin ZnCo_(2)O_(4)nanosheets showed better dispersion in the membrane.The pure gas separation performance data showed the CO_(2)permeability and CO_(2)/CH4 selectivity of Pebax/ZnCo_(2)O_(4)membrane were 139.10 Barrer and 15.38,respectively,when the filling amount was 0.5 wt%.Compared with pure Pebax membrane,the separation performance(permeability and selectivity)were increased with 165.67%and 75.57%,respectively.
