Bacterial infection is a major issue after artificial bone transplantation due to the absence of antibacterial function of bone scaffold,which seriously causes the transplant failure and even amputation in severe case...Bacterial infection is a major issue after artificial bone transplantation due to the absence of antibacterial function of bone scaffold,which seriously causes the transplant failure and even amputation in severe cases.In this study,oxygen vacancy(OV)defects Fe-doped Ti O2(OV-FeTiO2)nanoparticles were synthesized by nano TiO2and Fe3O4via high-energy ball milling,which was then incorporated into polycaprolactone/polyglycolic acid(PCLGA)biodegradable polymer matrix to construct composite bone scaffold with good antibacterial activities by selective laser sintering.The results indicated that OV defects were introduced into the core/shell-structured OV-FeTiO2nanoparticles through multiple welding and breaking during the high-energy ball milling,which facilitated the adsorption of hydrogen peroxide(H2O2)in the bacterial infection microenvironment at the bone transplant site.The accumulated H2O2could amplify the Fenton reaction efficiency to induce more hydroxyl radicals(·OH),thereby resulting in more bacterial deaths through·OH-mediated oxidative damage.This antibacterial strategy had more effective broad-spectrum antibacterial properties against Gram-negative Escherichia coli(E.coli)and Gram-positive Staphylococcus aureus(S.aureus).In addition,the PCLGA/OV-FeTiO2scaffold possessed mechanical properties that match those of human cancellous bone and good biocompatibility including cell attachment,proliferation and osteogenic differentiation.展开更多
Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this s...Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.展开更多
Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal int...Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.展开更多
The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process...The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process, still contains high levels of heavy metals and other harmful substances that might make traditional disposal difficult. We have devised a facile method of converting digested sludge into a mesoporous material that acts as an effective and stable heterogeneous catalyst for the photo‐Fenton reaction. A comparison of the removal of rhodamine B under different conditions showed that FAS‐1‐350, which was synthesized by mixing the digested sludge with a 1 mol/L（NH4）2Fe（SO4）2 solution followed by calcination at 350 °C, exhibited the best catalytic activity owing to its faster reaction rate and lower degree of Fe leaching. The results indicate that Fe^（2＋）‐loaded catalysts have significant potential to act as stable and efficient heterogeneous promoters for the photo‐Fenton reaction, with better performance than Fe^3＋‐loaded catalysts because the Fe（II）/Fe（III）compounds formed in the calcination process are necessary to sustain the Fenton reaction. This protocol provides an alternative, environmentally friendly method of reusing digested sludge and demonstrates an easily synthesized mesoporous material that effectively degrades azo dyes.展开更多
To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absenc...To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absence of light instead of Fe(Ⅱ) and H 2O 2 was studied. Results showed that use of Fe (Ⅲ) is more promising than Fe(Ⅱ). The present study reflects that Fenton reaction is more efficient, in the presence of a small amount of salicylic acid is added which is a one of the priority pollutant.展开更多
Magnetic field was tentatively introduced into Fenton reactions system for the degradation and discoloration of methyl blue as the represent of organic chemical dye, which was a bio-refractory organic pollutant in ind...Magnetic field was tentatively introduced into Fenton reactions system for the degradation and discoloration of methyl blue as the represent of organic chemical dye, which was a bio-refractory organic pollutant in industry wastewater. It was found that under optimal Fenton reaction conditions, with the assistant of magnetic field in Fenton reactions, the degradation rate of methyl blue, the decomposition rate of H2O2 and the conversion rate of Fe^2＋ were accelerated, the extent of them would be improved by the increase of magnetic field intensity. Meanwhile, the mineralization of methyl blue （CODer） was improved by over 10% with magnetic field.展开更多
Active Fe-and Mn-loaded MCM-41(Fe–Mn/MCM-41),which was synthesized via a hydrothermal reaction followed by impregnation,is used in the heterogeneous Fenton reaction to degrade methyl orange(MO) in aqueous solution. T...Active Fe-and Mn-loaded MCM-41(Fe–Mn/MCM-41),which was synthesized via a hydrothermal reaction followed by impregnation,is used in the heterogeneous Fenton reaction to degrade methyl orange(MO) in aqueous solution. The synthesized samples were characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,N_2 adsorption–desorption isotherm analysis,Fourier transform infrared spectroscopy,and X-ray photoelectron spectroscopy. Compared with Fe/MCM-41 and Mn/MCM-41,Fe–Mn/MCM-41 showed higher activity for MO degradation and mineralization. Effects of various operating parameters,such as pH,Mn content,and H_2O_2 dosage,on the degradation process were subsequently investigated. Results of experiments on the effect of radical scavengers revealed that the degradation of MO could be attributed to oxidation by HO_·. The synergy of Fe and Mn species in the Fenton oxidation process was also explained.展开更多
The effect of heterogeneous Fenton reaction was studied on methylene blue（MB） and Nitrosomonas europaea（N. europaea） cells. Four Fenton systems were prepared and compared with each other, including Nickel Foam（NF...The effect of heterogeneous Fenton reaction was studied on methylene blue（MB） and Nitrosomonas europaea（N. europaea） cells. Four Fenton systems were prepared and compared with each other, including Nickel Foam（NF）/TiO2, NF/Bi2WO6, Ceramic foam（CM）/TiO2, and CM/Bi2WO6. The order of effect of fenton reaction ranked as NF/TiO2〉CM/TiO2〉NF/Bi2WO6〉CM/Bi2WO6. In acid or alkaline solution, the removal efficiency also decreased compared with neutral solution. With lower p H values, the nanoparticles were easier to break off from NF skeleton. Thus the synergetic effect of photocatalysis and fenton reaction can not take action. As for CM skeleton, the bond –Si-O-can bind with TiO2 or Bi2WO6. The membrane fluidity was used as an indicating parameter. After being treated by Fenton reaction, N. europaea surface was rougher than the native bacterium and the bulges on cell surface became irregular, which is attributed to change of lipopolysaccharide patches. Polarization of N. europaea cell membrane in acid medium increased more obvious than alkaline medium.展开更多
基金supported by the following funds:The Natural Science Foundation of China(52275393,51935014,82072084)Hunan Provincial Natural Science Foundation of China(2021JJ20061)+4 种基金Jiangxi Provincial Natural Science Foundation of China(20224ACB204013)The Project of State Key Laboratory of Precision Manufacturing for Extreme Service PerformanceTechnology Innovation Platform Project of Shenzhen Institute of Information Technology 2020(PT2020E002)Guangdong Province Precision Manufacturing and Intelligent production education Integration Innovation Platform(2022CJPT019)Independent Exploration and Innovation Project of Central South University(1053320220553)。
文摘Bacterial infection is a major issue after artificial bone transplantation due to the absence of antibacterial function of bone scaffold,which seriously causes the transplant failure and even amputation in severe cases.In this study,oxygen vacancy(OV)defects Fe-doped Ti O2(OV-FeTiO2)nanoparticles were synthesized by nano TiO2and Fe3O4via high-energy ball milling,which was then incorporated into polycaprolactone/polyglycolic acid(PCLGA)biodegradable polymer matrix to construct composite bone scaffold with good antibacterial activities by selective laser sintering.The results indicated that OV defects were introduced into the core/shell-structured OV-FeTiO2nanoparticles through multiple welding and breaking during the high-energy ball milling,which facilitated the adsorption of hydrogen peroxide(H2O2)in the bacterial infection microenvironment at the bone transplant site.The accumulated H2O2could amplify the Fenton reaction efficiency to induce more hydroxyl radicals(·OH),thereby resulting in more bacterial deaths through·OH-mediated oxidative damage.This antibacterial strategy had more effective broad-spectrum antibacterial properties against Gram-negative Escherichia coli(E.coli)and Gram-positive Staphylococcus aureus(S.aureus).In addition,the PCLGA/OV-FeTiO2scaffold possessed mechanical properties that match those of human cancellous bone and good biocompatibility including cell attachment,proliferation and osteogenic differentiation.
基金financially supported by the National Natural Science Foundation of China(No.5217042069)the Young Elite Scientist Sponsorship Program by China Association for Science and Technology(CAST)(No.YESS20200103)the Fundamental Research Funds for the Central Universities(No.265QZ2022004)。
文摘Pt-based nanocatalysts offer excellent prospects for various industries.However,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable challenge.In this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ synthesis.These~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt ions.This unique structure is beneficial for the hydrogen evolution reaction.The catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C catalysts.Mass activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(22309137,22279095)Open subject project State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2023001).
文摘Anion-exchange membrane water electrolyzers(AEMWEs)for green hydrogen production have received intensive attention due to their feasibility of using earth-abundant NiFe-based catalysts.By introducing a third metal into NiFe-based catalysts to construct asymmetrical M-NiFe units,the d-orbital and electronic structures can be adjusted,which is an important strategy to achieve sufficient oxygen evolution reaction(OER)performance in AEMWEs.Herein,the ternary NiFeM(M:La,Mo)catalysts featured with distinct M-NiFe units and varying d-orbitals are reported in this work.Experimental and theoretical calculation results reveal that the doping of La leads to optimized hybridization between d orbital in NiFeM and 2p in oxygen,resulting in enhanced adsorption strength of oxygen intermediates,and reduced rate-determining step energy barrier,which is responsible for the enhanced OER performance.More critically,the obtained NiFeLa catalyst only requires 1.58 V to reach 1 A cm^(−2) in an anion exchange membrane electrolyzer and demonstrates excellent long-term stability of up to 600 h.
基金supported by the National Key Technology Research&Development Program of China(2014BAL02B02)the National Natural Science Foundation of China(51578397)~~
文摘The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process, still contains high levels of heavy metals and other harmful substances that might make traditional disposal difficult. We have devised a facile method of converting digested sludge into a mesoporous material that acts as an effective and stable heterogeneous catalyst for the photo‐Fenton reaction. A comparison of the removal of rhodamine B under different conditions showed that FAS‐1‐350, which was synthesized by mixing the digested sludge with a 1 mol/L（NH4）2Fe（SO4）2 solution followed by calcination at 350 °C, exhibited the best catalytic activity owing to its faster reaction rate and lower degree of Fe leaching. The results indicate that Fe^（2＋）‐loaded catalysts have significant potential to act as stable and efficient heterogeneous promoters for the photo‐Fenton reaction, with better performance than Fe^3＋‐loaded catalysts because the Fe（II）/Fe（III）compounds formed in the calcination process are necessary to sustain the Fenton reaction. This protocol provides an alternative, environmentally friendly method of reusing digested sludge and demonstrates an easily synthesized mesoporous material that effectively degrades azo dyes.
文摘To develop more efficient chemical methods for the demineralization of organic pollutants from water bodies, which one was also mimic to the nature, a degradation of methylene blue by Fe(Ⅲ) and H 2O 2 in the absence of light instead of Fe(Ⅱ) and H 2O 2 was studied. Results showed that use of Fe (Ⅲ) is more promising than Fe(Ⅱ). The present study reflects that Fenton reaction is more efficient, in the presence of a small amount of salicylic acid is added which is a one of the priority pollutant.
基金support by the Natural Science Research Foundation of Jiangnan University(No.005796).
文摘Magnetic field was tentatively introduced into Fenton reactions system for the degradation and discoloration of methyl blue as the represent of organic chemical dye, which was a bio-refractory organic pollutant in industry wastewater. It was found that under optimal Fenton reaction conditions, with the assistant of magnetic field in Fenton reactions, the degradation rate of methyl blue, the decomposition rate of H2O2 and the conversion rate of Fe^2＋ were accelerated, the extent of them would be improved by the increase of magnetic field intensity. Meanwhile, the mineralization of methyl blue （CODer） was improved by over 10% with magnetic field.
基金supported by the National Basic Research Program of China ("973" Program, No. 2012CB720302)Program for Changjiang Scholars and the Innovative Research Team in Universities (No. IRT0936)
文摘Active Fe-and Mn-loaded MCM-41(Fe–Mn/MCM-41),which was synthesized via a hydrothermal reaction followed by impregnation,is used in the heterogeneous Fenton reaction to degrade methyl orange(MO) in aqueous solution. The synthesized samples were characterized by X-ray diffraction,scanning electron microscopy,transmission electron microscopy,N_2 adsorption–desorption isotherm analysis,Fourier transform infrared spectroscopy,and X-ray photoelectron spectroscopy. Compared with Fe/MCM-41 and Mn/MCM-41,Fe–Mn/MCM-41 showed higher activity for MO degradation and mineralization. Effects of various operating parameters,such as pH,Mn content,and H_2O_2 dosage,on the degradation process were subsequently investigated. Results of experiments on the effect of radical scavengers revealed that the degradation of MO could be attributed to oxidation by HO_·. The synergy of Fe and Mn species in the Fenton oxidation process was also explained.
基金Funded by National Natural Science Foundation of Chinathe State Key Laboratory of Urban Water Resource and Environment(No.51208141)the National Key Research and Development Program of China(No.2016YFC0401102)
文摘The effect of heterogeneous Fenton reaction was studied on methylene blue（MB） and Nitrosomonas europaea（N. europaea） cells. Four Fenton systems were prepared and compared with each other, including Nickel Foam（NF）/TiO2, NF/Bi2WO6, Ceramic foam（CM）/TiO2, and CM/Bi2WO6. The order of effect of fenton reaction ranked as NF/TiO2〉CM/TiO2〉NF/Bi2WO6〉CM/Bi2WO6. In acid or alkaline solution, the removal efficiency also decreased compared with neutral solution. With lower p H values, the nanoparticles were easier to break off from NF skeleton. Thus the synergetic effect of photocatalysis and fenton reaction can not take action. As for CM skeleton, the bond –Si-O-can bind with TiO2 or Bi2WO6. The membrane fluidity was used as an indicating parameter. After being treated by Fenton reaction, N. europaea surface was rougher than the native bacterium and the bulges on cell surface became irregular, which is attributed to change of lipopolysaccharide patches. Polarization of N. europaea cell membrane in acid medium increased more obvious than alkaline medium.
