The uniform pore size distribution and inherent particle inseparability of iron-based metal-organic frameworks(Fe-MOFs)have been shown to significantly hinder their light-harvesting capabilities and charge carrier sep...The uniform pore size distribution and inherent particle inseparability of iron-based metal-organic frameworks(Fe-MOFs)have been shown to significantly hinder their light-harvesting capabilities and charge carrier separation efficiency.These intrinsic limitations compromise catalyst recyclability and reaction kinetics in practical scenarios,thereby impeding their applicability in the degradation of antibiotic pollutants such as levofloxacin(LEV)in aquatic environments.Here,we report an S-type heterojunction photocatalyst,MnFe2O4@MIL-101(Fe),prepared via hydrothermal coupling of magnetic MnFe2O4 nanoparticles with MIL-101(Fe).The synergistic effect of Fe3+/Fe2+and Mn3+/Mn2+redox pairs,combined with the heterojunction interface and built-in electric field,significantly enhances visible-light-driven photo-Fenton activity.The catalyst degraded over 95%of LEV with a rate constant of 0.05056 min-1 and retained 87%activity after five cycles.LC-MS analysis revealed defluorination and demethylation pathways,while toxicity assessments confirmed lower LC50,mutagenicity,and developmental toxicity of intermediates,validating the environmental viability of the photo-Fenton process.展开更多
Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces...Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces was attributed to the reducibility of 2-methoxyethanol in the precursor solution.Comparative photocatalytic evaluation reveals that the Bi/Bi2Fe4O9nanocomposites significantly enhance the degradation efficiency(99.0%)of bisphenol A compared with Bi2Fe4O9nanosheets(64.2%)under 120 min simulated solar irradiation.This remarkable enhancement can be attributed to the established Bi/Bi2Fe4O9heterojunction structure,which effectively facilitates the separation of photogenerated electron-hole pairs and accelerates interfacial charge transfer between the metallic Bi nanodots and semiconductor Bi2Fe4O9nanosheets.The synergistic effects arising from this unique architecture ultimately lead to superior photocatalytic performance.展开更多
The direct conversion of methane into methanol under mild conditions represents a highly appealing pathway.Regulating the generation of hydroxyl radicals(·OH)is a representative method,but excessive release of...The direct conversion of methane into methanol under mild conditions represents a highly appealing pathway.Regulating the generation of hydroxyl radicals(·OH)is a representative method,but excessive release of·OH will inevitably lead to the over-oxidation of CH3OH.Here,we design AgPd alloy and Co3O4 cascade active sites on the TiO2 surface(AgPd-Co/TiO2)to control the release rate of·OH to improve the selectivity of CH3OH.By incorporating Co3O4 as a hole buffer and storage center,the kinetics of·OH generation at the TiO2 interface can be effectively modulated.This confines the spatial distribution of·OH to the active sites of the AgPd alloy,thus facilitating the directional combination of·CH3 and·OH.The optimal AgPd-Co/TiO2 photocatalyst demonstrates outstanding catalytic performance with the selectivity of CH3OH reaching up to 93%in the liquid phase.AgPd-Co/TiO2 exhibited significantly enhanced selectivity relative to reported TiO2-based photocatalytic systems,while simultaneously achieving comparable methanol yields.This research offers valuable insights for the precise design of composite photocatalysts to achieve highly selective methane oxidation.展开更多
To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe3O4@SiO2@Fe-MIL...To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe3O4@SiO2@Fe-MIL-101 magnetic composite material was successfully synthesized via the one-pot method.Preparation conditions were optimized and structural characterization of this material conducted using FTIR,SEM,EDS,XRD and Hysteresis analysis.The results show that this composite exhibits a more rapid fluoride adsorption dynamics and a higher fluoride adsorption capacity(18.34 mg/g)and its adsorption behavior fitted for the first order dynamic model and the Freundlich isotherm model.The adsorption of fluorine by this composite is mainly physical adsorption according to the mean adsorption energy(1.216 kJ/mol).The interfering ions co-existed in fluoride-containing solutions,like HCO3-,NO-and Cl-,have a significant effect on fluorine adsorption.This composite has also been proved with magnetism,higher adsorption selectivity and satisfactory reusability.When this composite is employed as an adsorbent for adsorption removing fluoride in zinc sulfate electrolyte,it exhibits higher pH-dependent behavior as well as high fluoride removal efficiency at pH 6.5.展开更多
According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equatio...According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.展开更多
基金supported by the National Natural Science Foundation of China(No.22178325)the Research Fund of Key Laboratory of the Ministry of Education for Advanced Catalysis Materials,Zhejiang Key Laboratory of Advanced Catalysis and Adsorption Materials。
摘要The uniform pore size distribution and inherent particle inseparability of iron-based metal-organic frameworks(Fe-MOFs)have been shown to significantly hinder their light-harvesting capabilities and charge carrier separation efficiency.These intrinsic limitations compromise catalyst recyclability and reaction kinetics in practical scenarios,thereby impeding their applicability in the degradation of antibiotic pollutants such as levofloxacin(LEV)in aquatic environments.Here,we report an S-type heterojunction photocatalyst,MnFe2O4@MIL-101(Fe),prepared via hydrothermal coupling of magnetic MnFe2O4 nanoparticles with MIL-101(Fe).The synergistic effect of Fe3+/Fe2+and Mn3+/Mn2+redox pairs,combined with the heterojunction interface and built-in electric field,significantly enhances visible-light-driven photo-Fenton activity.The catalyst degraded over 95%of LEV with a rate constant of 0.05056 min-1 and retained 87%activity after five cycles.LC-MS analysis revealed defluorination and demethylation pathways,while toxicity assessments confirmed lower LC50,mutagenicity,and developmental toxicity of intermediates,validating the environmental viability of the photo-Fenton process.
基金Funded by the National Natural Science Foundation of China(No.50902108)。
摘要Bi/Bi2Fe4O9nanocomposites consisting of Bi2Fe4O9nanosheets decorated with Bi nanodots were synthesized by a hydrothermal method.The formation of Bi nanodots on the Bi2Fe4O9nanosheet surfaces was attributed to the reducibility of 2-methoxyethanol in the precursor solution.Comparative photocatalytic evaluation reveals that the Bi/Bi2Fe4O9nanocomposites significantly enhance the degradation efficiency(99.0%)of bisphenol A compared with Bi2Fe4O9nanosheets(64.2%)under 120 min simulated solar irradiation.This remarkable enhancement can be attributed to the established Bi/Bi2Fe4O9heterojunction structure,which effectively facilitates the separation of photogenerated electron-hole pairs and accelerates interfacial charge transfer between the metallic Bi nanodots and semiconductor Bi2Fe4O9nanosheets.The synergistic effects arising from this unique architecture ultimately lead to superior photocatalytic performance.
基金Supporting information is available in the online version of this article.
摘要The direct conversion of methane into methanol under mild conditions represents a highly appealing pathway.Regulating the generation of hydroxyl radicals(·OH)is a representative method,but excessive release of·OH will inevitably lead to the over-oxidation of CH3OH.Here,we design AgPd alloy and Co3O4 cascade active sites on the TiO2 surface(AgPd-Co/TiO2)to control the release rate of·OH to improve the selectivity of CH3OH.By incorporating Co3O4 as a hole buffer and storage center,the kinetics of·OH generation at the TiO2 interface can be effectively modulated.This confines the spatial distribution of·OH to the active sites of the AgPd alloy,thus facilitating the directional combination of·CH3 and·OH.The optimal AgPd-Co/TiO2 photocatalyst demonstrates outstanding catalytic performance with the selectivity of CH3OH reaching up to 93%in the liquid phase.AgPd-Co/TiO2 exhibited significantly enhanced selectivity relative to reported TiO2-based photocatalytic systems,while simultaneously achieving comparable methanol yields.This research offers valuable insights for the precise design of composite photocatalysts to achieve highly selective methane oxidation.
基金National Natural Science Foundation of China(21865011)2024 Innovation and Entrepreneurship Project of College Student in Jishou University(JDCX20241122)。
摘要To remove the fluoride in zinc sulfate electrolyte to an appropriate level,mitigate environmental fluoride pollution,and drive the development of the hydrometallurgy industry of zinc,a novel Fe3O4@SiO2@Fe-MIL-101 magnetic composite material was successfully synthesized via the one-pot method.Preparation conditions were optimized and structural characterization of this material conducted using FTIR,SEM,EDS,XRD and Hysteresis analysis.The results show that this composite exhibits a more rapid fluoride adsorption dynamics and a higher fluoride adsorption capacity(18.34 mg/g)and its adsorption behavior fitted for the first order dynamic model and the Freundlich isotherm model.The adsorption of fluorine by this composite is mainly physical adsorption according to the mean adsorption energy(1.216 kJ/mol).The interfering ions co-existed in fluoride-containing solutions,like HCO3-,NO-and Cl-,have a significant effect on fluorine adsorption.This composite has also been proved with magnetism,higher adsorption selectivity and satisfactory reusability.When this composite is employed as an adsorbent for adsorption removing fluoride in zinc sulfate electrolyte,it exhibits higher pH-dependent behavior as well as high fluoride removal efficiency at pH 6.5.
基金Sponsored by the National Natural Science Foundation of China (Grant No. 51078100)the National Creative Research Groups granted by NSFC(Grant No. 50821002)+1 种基金Excellent Youth Foundation of Heilongjiang Scientific Committee(Grant No. JC2010-03)State Key Laboratory of Urban Water Resource and Environment(Grant No. 2010DX11)
摘要According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.