The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-...The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.展开更多
For the first time,two-dimensional FeOCl(Fe_(1-x)Co_(x)OCl)doped with Co was successfully applied to the photocatalytic and photo-Fenton degradation of Rhodamine B(RhB).The photocatalytic and photo-Fenton experiments ...For the first time,two-dimensional FeOCl(Fe_(1-x)Co_(x)OCl)doped with Co was successfully applied to the photocatalytic and photo-Fenton degradation of Rhodamine B(RhB).The photocatalytic and photo-Fenton experiments showed that the degradation rates of RhB by Fe0.94Co0.06OCl are 82.6%and 98.2%within 50 min under neutral solution,room temperature and visible light.The inclusion of Co resulted in lattice imperfections on the surface of Fe OCl,which was advantageous for the photogenerated electron-hole pair separation efficiency(consistent with the density functional theory calculation).Moreover,the RhB removal rate decreased from 98%to 82%during five successive cycles,showing good structural stability.Finally,based on the radical capture experiment,a potential mechanism for RhB degradation by Fe_(1-x)Co_(x)OCl catalyst was proposed.The idea of a synergistic mechanism for Fe_(1-x)Co_(x)OCl also offers a fresh concept for catalysts used in doping modification.展开更多
In this paper,the residue from bamboo factory has been used to design photo-Fenton catalyst,which has the advantages of low cost and magnetic recycling.The photo-Fenton catalytic performance of the biocarbon-based cat...In this paper,the residue from bamboo factory has been used to design photo-Fenton catalyst,which has the advantages of low cost and magnetic recycling.The photo-Fenton catalytic performance of the biocarbon-based catalyst was excellent and its optimal preparation process was also explored by response surface methodology.First,bamboo-carbon fiber was selected as the photo-Fenton catalyst carrier.Subsequently,the surface of the car-bon fiber was modified,with which dopamine,nano-Fe_(3)O_(4) and nano-TiO_(2) were successively loaded by hydro-thermal method.After the single factor tests,four factors including dopamine concentration,ferric chloride mass,P25 titanium dioxide mass and liquid-solid ratio were selected as the characteristic values.The degradation efficiency of photo-Fenton catalyst to methylene blue(MB)solution was treated as the response value.After the analysis of the response surface optimization,it was shown that the significance sequence of the selected 4 factors in terms of the MB degradation efficiency was arranged as follows:dopamine concentration>liquid-solid ratio>P25 titanium dioxide quality>ferric chloride quality.The optimal process parameters of fiber-carbon catalyst were affirmed as follows:the 1.7 mg/mL concentration of dopamine,the 1.2 g mass of ferric chloride,the 0.2 g mass of P25 titanium dioxide and the liquid-solid ratio of 170 mL/g.The experiment-measured average MB degra-dation efficiency performed by the optimized catalyst was 99.3%,which was nearly similar to the model-predicted value of 98.9%.It showed that the prediction model and response surface model were accurate and reliable.The results from response surface optimization could provide a good reference to design bamboo-based Fenton-like catalyst with excellent catalytic performance.展开更多
The low intrinsic activity of Fenton catalytic site and high demand for light-energy input inhibit the organic-pollution control efficiency of photo-Fenton process.Here,through structural design with density functiona...The low intrinsic activity of Fenton catalytic site and high demand for light-energy input inhibit the organic-pollution control efficiency of photo-Fenton process.Here,through structural design with density functional theory(DFT)calculations,Ce is predicted to enable the construction of coordinatively unsaturated metal centers(CUCs)in Prussian blue analogue(PBA),which can strongly adsorb H_(2)O_(2)and donate sufficient electrons for directly splitting the O-O bond to produceOH.Using a substitution-co-assembly strategy,binary Ce-Fe PBA is then prepared,which rapidly degrades sulfamethoxazole with the pseudo-first-order kinetic rate constant exceeding reported values by 1-2 orders of magnitude.Meanwhile,the photogenerated electrons reduce Fe(Ⅲ)and Ce(Ⅳ)to promote the metal valence cycle in CUCs and make sulfamethoxazole degradation efficiency only lose 6.04%in 5 runs.Overall,by introducing rare earth metals into transition metal-organic frameworks,this work guides the whole process for highly active CUCs from design and construction to mechanism exploration with DFT calculations,enabling ultrafast and stable photo-Fenton catalysis.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
Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation...Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation efficiency was undertaken. It was found that Fenton process could not completely degrade citrate in the presence of hypophosphite since it caused a series inhibition. Therefore, UV light （photo-Fenton） or electron current （electro-Fenton） was applied to improve the degradation efficiency of the Fenton process. Results showed that both photo-Fenton and electro-Fenton processes could overcome the inhibition of hypophosphite, especially the electro-Fenton.展开更多
Ordered mesoporous Fe/TiO2 was prepared by an evaporation-induced self-assembly method. The iron ions were in situ embedded in the pore wall of the TiO2 framework. The catalyst has excellent light-assisted Fenton cata...Ordered mesoporous Fe/TiO2 was prepared by an evaporation-induced self-assembly method. The iron ions were in situ embedded in the pore wall of the TiO2 framework. The catalyst has excellent light-assisted Fenton catalytic performance under UV and visible light irradiation. X-ray diffraction and transmission electron microscopy results showed that the TiO2 samples have an ordered two-dimensional hexagonal pore structure and an anatase phase structure with high crystallinity. The ordered pore structure of the TiO2 photocatalyst with a large specific surface area is beneficial to mass transfer and light harvesting. Furthermore, iron ions can be controlled by embedding them into the TiO2 framework to prevent iron ion loss and inactivation. After five cycles, the reaction rate of the ordered mesoporous Fe/TiO2 remained unchanged, indicating that the material has stable performance and broad application prospects for the purification of environmental pollutants.展开更多
Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reactio...Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reaction is challenging.In this study,2D/2D step-schemeα-Fe2O3/Bi2WO6(FO/BWO)heterostructure photo-Fenton catalysts were successfully fabricated by a facile hydrothermal method.The as-prepared materials were characterized by XRD,FT-IR,TEM,XPS,UV-vis DRS,PL,I-t,EIS,and BET analyses.Under visible light irradiation,FO/BWO exhibited remarkably high and stable photo-Fenton catalytic activity for the degradation of methyl blue(MB)at low concentrations of H2O2.It was noted that FO/BWO(0.5)displayed a significantly enhanced photo-Fenton catalytic activity,which was 11.06 and 3.29 times those of FO nanosheets and BWO nanosheets,respectively.The notably improved photo-Fenton catalytic activity of FO/BWO was mainly due to the combination of H2O2 and FO under light illumination and the presence of the 2D/2D S-scheme heterostructure,with the large contact surface,abundant active sites,and efficient separation rate of photogenerated carriers playing contributory roles.Additionally,a possible catalytic mechanism for the FO/BWO composite was preliminarily proposed via active species trapping experiments.In summary,this study provided new insights into the synthesis of an effectively heterogeneous 2D/2D S-scheme photo-Fenton catalyst for degradation of organic pollutants in wastewater.展开更多
基金supported by the National Natural Science Foundation of China(52373099)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.
基金the National Natural Science Foundation of China(Grant No.52268042)the Natural Science Foundation of Gansu Province+1 种基金China(Grant No.22JR5RA253)HongLiu First-Class Disciplines Development Program of Lanzhou University of Technology。
文摘For the first time,two-dimensional FeOCl(Fe_(1-x)Co_(x)OCl)doped with Co was successfully applied to the photocatalytic and photo-Fenton degradation of Rhodamine B(RhB).The photocatalytic and photo-Fenton experiments showed that the degradation rates of RhB by Fe0.94Co0.06OCl are 82.6%and 98.2%within 50 min under neutral solution,room temperature and visible light.The inclusion of Co resulted in lattice imperfections on the surface of Fe OCl,which was advantageous for the photogenerated electron-hole pair separation efficiency(consistent with the density functional theory calculation).Moreover,the RhB removal rate decreased from 98%to 82%during five successive cycles,showing good structural stability.Finally,based on the radical capture experiment,a potential mechanism for RhB degradation by Fe_(1-x)Co_(x)OCl catalyst was proposed.The idea of a synergistic mechanism for Fe_(1-x)Co_(x)OCl also offers a fresh concept for catalysts used in doping modification.
基金funding from Hunan Provincial Key Research and Development Program(2020WK2018)Hunan Provincial Forestry Technological Innovation Funds(XLK202107-3)+2 种基金Scientific Research Project of Hunan Education Department(19A505,21B0242)National Natural Science Foundation of China(No.21908251)Hunan Provincial Natural Science Foundation of China(No.2020JJ2058).
文摘In this paper,the residue from bamboo factory has been used to design photo-Fenton catalyst,which has the advantages of low cost and magnetic recycling.The photo-Fenton catalytic performance of the biocarbon-based catalyst was excellent and its optimal preparation process was also explored by response surface methodology.First,bamboo-carbon fiber was selected as the photo-Fenton catalyst carrier.Subsequently,the surface of the car-bon fiber was modified,with which dopamine,nano-Fe_(3)O_(4) and nano-TiO_(2) were successively loaded by hydro-thermal method.After the single factor tests,four factors including dopamine concentration,ferric chloride mass,P25 titanium dioxide mass and liquid-solid ratio were selected as the characteristic values.The degradation efficiency of photo-Fenton catalyst to methylene blue(MB)solution was treated as the response value.After the analysis of the response surface optimization,it was shown that the significance sequence of the selected 4 factors in terms of the MB degradation efficiency was arranged as follows:dopamine concentration>liquid-solid ratio>P25 titanium dioxide quality>ferric chloride quality.The optimal process parameters of fiber-carbon catalyst were affirmed as follows:the 1.7 mg/mL concentration of dopamine,the 1.2 g mass of ferric chloride,the 0.2 g mass of P25 titanium dioxide and the liquid-solid ratio of 170 mL/g.The experiment-measured average MB degra-dation efficiency performed by the optimized catalyst was 99.3%,which was nearly similar to the model-predicted value of 98.9%.It showed that the prediction model and response surface model were accurate and reliable.The results from response surface optimization could provide a good reference to design bamboo-based Fenton-like catalyst with excellent catalytic performance.
基金supported by the National Natural Science Foundation of China(No.22072064,51522805,51908273,and 22176086)the State Key Laboratory of Pollution Control and Resource Reuse(PCRR-ZZ-202106)Start-Up Funds for Jiangsu Distinguished Professor.
文摘The low intrinsic activity of Fenton catalytic site and high demand for light-energy input inhibit the organic-pollution control efficiency of photo-Fenton process.Here,through structural design with density functional theory(DFT)calculations,Ce is predicted to enable the construction of coordinatively unsaturated metal centers(CUCs)in Prussian blue analogue(PBA),which can strongly adsorb H_(2)O_(2)and donate sufficient electrons for directly splitting the O-O bond to produceOH.Using a substitution-co-assembly strategy,binary Ce-Fe PBA is then prepared,which rapidly degrades sulfamethoxazole with the pseudo-first-order kinetic rate constant exceeding reported values by 1-2 orders of magnitude.Meanwhile,the photogenerated electrons reduce Fe(Ⅲ)and Ce(Ⅳ)to promote the metal valence cycle in CUCs and make sulfamethoxazole degradation efficiency only lose 6.04%in 5 runs.Overall,by introducing rare earth metals into transition metal-organic frameworks,this work guides the whole process for highly active CUCs from design and construction to mechanism exploration with DFT calculations,enabling ultrafast and stable photo-Fenton catalysis.
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.
基金The authors thank the "National" Science Council, Taiwan, China for financially supporting (No. NSC95- 2211-E-006-032).
文摘Both citrate and hypophosphite in aqueous solution were degraded by advanced oxidation processes （Fe^2＋/H2O2, UV/Fe^2＋/H2O2, and electrolysis/Fe^2＋/H2O2） in this study. Comparison of these techniques in oxidation efficiency was undertaken. It was found that Fenton process could not completely degrade citrate in the presence of hypophosphite since it caused a series inhibition. Therefore, UV light （photo-Fenton） or electron current （electro-Fenton） was applied to improve the degradation efficiency of the Fenton process. Results showed that both photo-Fenton and electro-Fenton processes could overcome the inhibition of hypophosphite, especially the electro-Fenton.
基金supported by the National Natural Science Foundation of China(21876114,21761142011,51572174)Shanghai Government(17SG44)+2 种基金International Joint Laboratory on Resource Chemistry(IJLRC)Ministry of Education of China(PCSIRT_IRT_16R49)supported by The Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning and Shuguang Research Program of Shanghai Education Committee~~
文摘Ordered mesoporous Fe/TiO2 was prepared by an evaporation-induced self-assembly method. The iron ions were in situ embedded in the pore wall of the TiO2 framework. The catalyst has excellent light-assisted Fenton catalytic performance under UV and visible light irradiation. X-ray diffraction and transmission electron microscopy results showed that the TiO2 samples have an ordered two-dimensional hexagonal pore structure and an anatase phase structure with high crystallinity. The ordered pore structure of the TiO2 photocatalyst with a large specific surface area is beneficial to mass transfer and light harvesting. Furthermore, iron ions can be controlled by embedding them into the TiO2 framework to prevent iron ion loss and inactivation. After five cycles, the reaction rate of the ordered mesoporous Fe/TiO2 remained unchanged, indicating that the material has stable performance and broad application prospects for the purification of environmental pollutants.
文摘Although the traditional Fenton reaction is considered an effective strategy for solving problems caused by environmental pollution,construction of an efficient photocatalytic system by coordinating the Fenton reaction is challenging.In this study,2D/2D step-schemeα-Fe2O3/Bi2WO6(FO/BWO)heterostructure photo-Fenton catalysts were successfully fabricated by a facile hydrothermal method.The as-prepared materials were characterized by XRD,FT-IR,TEM,XPS,UV-vis DRS,PL,I-t,EIS,and BET analyses.Under visible light irradiation,FO/BWO exhibited remarkably high and stable photo-Fenton catalytic activity for the degradation of methyl blue(MB)at low concentrations of H2O2.It was noted that FO/BWO(0.5)displayed a significantly enhanced photo-Fenton catalytic activity,which was 11.06 and 3.29 times those of FO nanosheets and BWO nanosheets,respectively.The notably improved photo-Fenton catalytic activity of FO/BWO was mainly due to the combination of H2O2 and FO under light illumination and the presence of the 2D/2D S-scheme heterostructure,with the large contact surface,abundant active sites,and efficient separation rate of photogenerated carriers playing contributory roles.Additionally,a possible catalytic mechanism for the FO/BWO composite was preliminarily proposed via active species trapping experiments.In summary,this study provided new insights into the synthesis of an effectively heterogeneous 2D/2D S-scheme photo-Fenton catalyst for degradation of organic pollutants in wastewater.
