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
Combining microwave radiation with photocatalytic systems is a promising method to inhibit photogenerated electron-hole recombination and enhance the photocatalytic reaction performance. In this study, we have designe...Combining microwave radiation with photocatalytic systems is a promising method to inhibit photogenerated electron-hole recombination and enhance the photocatalytic reaction performance. In this study, we have designed Pd/Pb TiO3 catalysts that can use both microwave fields and photocatalysis. Benefiting from the synergistic effect of microwave field and UV light, the Pb TiO3 crystals convert thermal energy into electrical energy via the pyroelectricity effect, generating positive and negative charges(q+ and q-), while Pd nanoparticles significantly improve the quantum efficiency of the photocatalytic process. The composite catalyst significantly enhances the reaction rate and selectivity of the model Suzuki coupling reaction performed with bromobenzene. Microwave fields can directly act on chemical systems, promoting or changing various chemical reactions in unique ways.展开更多
NH_(2)-UIO66(NU)is a promising photocatalyst for the reduction of Cr(VI)to low-toxic Cr(III)driven by visible light under ambient conditions.However,the main limitation in this process is the ineffi cient ligand to me...NH_(2)-UIO66(NU)is a promising photocatalyst for the reduction of Cr(VI)to low-toxic Cr(III)driven by visible light under ambient conditions.However,the main limitation in this process is the ineffi cient ligand to metal charge transfer(LMCT)of photo-excited electrons,which is caused by inherent energy gap(ΔE_(LMCT)).This study synthesized the defective NU(NUXH,where X is the molar equivalent of the modulator)with reducedΔE_(LMCT)through linkers removal via acid treatment.The electronic structure of NUX-H was systematically investigated,and the results indicated that the structural defects in NUX-H strongly altered the environment of the Zr atoms.Furthermore,they substantially lowered the energy of the unoccupied d orbitals(LUMO),which was benefi cial to effi cient LMCT,resulting in an improved photocatalytic activity of NUX-H toward high-concentration(100 mg/L)Cr(VI)reduction.Compared to NU with defect-free structure,the reducing rate of Cr(VI)was increased by 47 times.This work introduced an alternative strategy in terms of designing effi cient photocatalysts for reducing Cr(VI)under ambient conditions.展开更多
The mitigation of environmental and energy crises could be advanced by reclaiming platinum group precious metals(PGMs) from decommissioned air purification catalysts. However, the complexity of catalyst composition an...The mitigation of environmental and energy crises could be advanced by reclaiming platinum group precious metals(PGMs) from decommissioned air purification catalysts. However, the complexity of catalyst composition and the high chemical inertness of PGMs significantly impede this process. Consequently,recovering PGMs from used industrial catalysts is crucial and challenging. This study delves into an environmentally friendly approach to selectively recover PGMs from commercial air purifiers using photocatalytic redox technology. Our investigation focuses on devising a comprehensive strategy for treating three-way catalysts employed in automotive exhaust treatment. By meticulously pretreating and modifying reaction conditions, we achieved noteworthy results, completely dissolving and separating rhodium(Rh), palladium(Pd), and platinum(Pt) within a 12-h time frame. Importantly, the solubility selectivity persists despite the remarkably similar physicochemical properties of Rh, Pd, and Pt. To bolster the environmental sustainability of our method, we harness sunlight as the energy source to activate the photocatalysts, facilitating the complete dissolution of precious metals under natural light irradiation. This ecofriendly recovery approach demonstrated on commercial air purifiers, exhibits promise for broader application to a diverse range of deactivated air purification catalysts, potentially enabling implementation on a large scale.展开更多
Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) ...Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) is one of the most critical steps in the whole process.Herein,we regulated the different adsorption intensity of oxygen on the surface by designing phosphate (PO_(4)^(3-)) modified titanium oxide(TiO_(2)).The results show that the adsorption of oxygen on the photocatalyst surface is gradually enhanced,which effectively improves the dissolution rate of precious metals.PO_(4)^(3-)modification increased the photocatalytic dissolution rate of gold (Au) by 2.8 times.The photocatalytic activity of other precious metals dissolution (such as palladium (Pd),platinum (Pt),rhodium (Rh),ruthenium (Ru) and iridium (Ir)) was also significantly improved.It is applied to the recovery of precious metals from spent catalysts and electronic devices to significantly promote the recovery efficiency.This indicates the direction for designing more efficient photocatalysts for precious metal recovery.展开更多
Photocatalytic Fenton reactions combined the advantages from both photocatalysis and Fenton reaction in mineralizing organic pollutants. The key problems are the efficiency and recycling stability. Herein, we reported...Photocatalytic Fenton reactions combined the advantages from both photocatalysis and Fenton reaction in mineralizing organic pollutants. The key problems are the efficiency and recycling stability. Herein, we reported a novel Fe_(2)O_(3)/TiO_(2)/reduced graphene oxide(FTG) nanocomposite synthesized by a facile solvothermal method. The TiO_(2)in FTG degraded organic pollutants and mineralized intermediates via photocatalysis under visible light irradiation, which could also promote Fenton reaction by accelerating Fe^(3+)-Fe^(2+)recycle. Meanwhile, the Fe_(2)O_(3)rapidly degraded organic pollutants via Fenton reactions, which also promoted photocatalysis by enhancing visible light absorbance and diminishing photoelectronhole recombination. The high distribution of TiO_(2)and Fe_(2)O_(3)on rGO, together with their strong interaction resulted in enhanced synergetic cooperation between photocatalysis and Fenton reactions, leading to the high mineralization efficiency of organic pollutants. More importantly, it could also inhibit the leaching of Fe species, leading to the long lifetime of FTG during photocatalytic Fenton reactions in a wide pH range from 3.4 to 9.2.展开更多
In order to develop efficient photocatalysts,great efforts have been made to reduce hexavalent chromium to trivalent chromium.The photocatalytic efficiency of this reduction depends largely on the adsorption and diffu...In order to develop efficient photocatalysts,great efforts have been made to reduce hexavalent chromium to trivalent chromium.The photocatalytic efficiency of this reduction depends largely on the adsorption and diffusion of hexavalent chromium ions on the surface of the photocatalyst.In this paper,polyanilineTiO2 composite can effectively improve the photocatalytic reduction performance and stability of hexavalent chromium ion.The effect of polyaniline(PANI) thickness on Cr(VI) activity and stability of photocatalytic reduction was studied by adjusting the content of PANI on Mesoporous TiO2(MT) surface.Under the irradiation conditions,the reaction results showed that the reduction rate was 100%,and the maximum reaction rate reached 0.62 min-1 when the PANI modification was 3.0%.Moreover,the results showed that the reduction performance remained 100% after ten cycles.The main reason is that the PANI modified on the surface of TiO2 is rich in positively charged amino group,which can efficiently adsorb the reactant Cr(VI),and make the product Cr(III) leave the reaction interface quickly,thus ensuring the performance of photocatalyst.展开更多
Environmental deterioration,especially water pollution,is widely dispersed and could affect the quality of people's life at large.Though the sewage treatment plants are constructed to meet the demands of cities,di...Environmental deterioration,especially water pollution,is widely dispersed and could affect the quality of people's life at large.Though the sewage treatment plants are constructed to meet the demands of cities,distributed treatment units are still in request for the supplementary of centralized purification beyond the range of plants.Electrochemical degradation can reduce organic pollution to some degree,but it has to be powered.Triboelectric nanogenerator(TENG)is a newly-invented technology for low-frequency mechanical energy harvesting.Here,by integrating a rotary TENG(R-TENG)as electric power source with an electrochemical cell containing a modified graphite felt cathode for hydrogen peroxide(H2O2)along with hydroxyl radical(·OH)generation by Fenton reaction and a platinum sheet anode for active chlorine generation,a self-powered electrochemical system(SPECS)was constructed.Under the driven of mechanical energy or wind flow,such SPECS can efficiently degrade dyes after power management in neutral condition without any O2 aeration.This work not only provides a guideline for optimizing self-powered electrochemical reaction,but also displays a strategy based on the conversion from distributed mechanical energy to chemical energy for environmental remediation.展开更多
In this paper, the process of photocatalytic reduction of hexavalent chromium was investigated over Ti3+- modified TiO2 photocatalysts. The Ti3+ surface defects were repaired by annealing as-prepared sample at diffe...In this paper, the process of photocatalytic reduction of hexavalent chromium was investigated over Ti3+- modified TiO2 photocatalysts. The Ti3+ surface defects were repaired by annealing as-prepared sample at different temperatures to control the amount of Ti3+ sites. The samples were characterized by SEM, XRD, BET, UV-Vis absorption, EPR and XPS. The results showed Ti3+ defects were successfully doped in TiO2. The surface selective adsorption of hexavalent chromium [Cr2072 (Cr(VI))] and the desorption of trivalent chromium [Cr3+ (Cr(III))] were investigated during the process ofphotocatalytic reduction positive charges due to more Ti3+ defects on the surface show a Accordingly, the surface positive reduction of Cr(VI). charges controlled by the Ti3+ Zeta potential results presented that the increased significant improvement for adsorption of Cr(VI). defects play important roles in the photocatalytic展开更多
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Combining microwave radiation with photocatalytic systems is a promising method to inhibit photogenerated electron-hole recombination and enhance the photocatalytic reaction performance. In this study, we have designed Pd/Pb TiO3 catalysts that can use both microwave fields and photocatalysis. Benefiting from the synergistic effect of microwave field and UV light, the Pb TiO3 crystals convert thermal energy into electrical energy via the pyroelectricity effect, generating positive and negative charges(q+ and q-), while Pd nanoparticles significantly improve the quantum efficiency of the photocatalytic process. The composite catalyst significantly enhances the reaction rate and selectivity of the model Suzuki coupling reaction performed with bromobenzene. Microwave fields can directly act on chemical systems, promoting or changing various chemical reactions in unique ways.
基金This work was supported by the National Key Research and Development Program of China(No.2020YFA0211000)the National Natural Science Foundation of China(Nos.21876114,21761142011,and 51572174)+3 种基金the Shanghai Government(Nos.19DZ1205102 and 19160712900)the International Joint Laboratory on Resource Chemistry(No.IJLRC)the Ministry of Education of China(No.PCSIRT_IRT_16R49)This research was also supported by The Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning,the Shuguang Research Program of Shanghai Education Committee,and the Shanghai Engineering Research Center of Green Energy Chemical Engineering(No.18DZ2254200).
文摘NH_(2)-UIO66(NU)is a promising photocatalyst for the reduction of Cr(VI)to low-toxic Cr(III)driven by visible light under ambient conditions.However,the main limitation in this process is the ineffi cient ligand to metal charge transfer(LMCT)of photo-excited electrons,which is caused by inherent energy gap(ΔE_(LMCT)).This study synthesized the defective NU(NUXH,where X is the molar equivalent of the modulator)with reducedΔE_(LMCT)through linkers removal via acid treatment.The electronic structure of NUX-H was systematically investigated,and the results indicated that the structural defects in NUX-H strongly altered the environment of the Zr atoms.Furthermore,they substantially lowered the energy of the unoccupied d orbitals(LUMO),which was benefi cial to effi cient LMCT,resulting in an improved photocatalytic activity of NUX-H toward high-concentration(100 mg/L)Cr(VI)reduction.Compared to NU with defect-free structure,the reducing rate of Cr(VI)was increased by 47 times.This work introduced an alternative strategy in terms of designing effi cient photocatalysts for reducing Cr(VI)under ambient conditions.
基金supported by the National Key Research and Development Program of China (2020YFA0211004)the National Natural Science Foundation of China (22176128 and 22236005)+7 种基金the Innovation Program of Shanghai Municipal Education Commission (2023ZKZD50)Program of Shanghai Academic Research Leader (21XD1422800)Shanghai Government (22dz1205400 and 23520711100)Chinese Education Ministry Key Laboratory and International Joint Laboratory on Resource ChemistryShanghai Eastern Scholar Programthe “111 Innovation and Talent Recruitment Base on Photochemical and Energy Materials” (D18020)Shanghai Engineering Research Center of Green Energy Chemical Engineering (18DZ2254200)Shanghai Frontiers Science Center of Biomimetic Catalysis。
文摘The mitigation of environmental and energy crises could be advanced by reclaiming platinum group precious metals(PGMs) from decommissioned air purification catalysts. However, the complexity of catalyst composition and the high chemical inertness of PGMs significantly impede this process. Consequently,recovering PGMs from used industrial catalysts is crucial and challenging. This study delves into an environmentally friendly approach to selectively recover PGMs from commercial air purifiers using photocatalytic redox technology. Our investigation focuses on devising a comprehensive strategy for treating three-way catalysts employed in automotive exhaust treatment. By meticulously pretreating and modifying reaction conditions, we achieved noteworthy results, completely dissolving and separating rhodium(Rh), palladium(Pd), and platinum(Pt) within a 12-h time frame. Importantly, the solubility selectivity persists despite the remarkably similar physicochemical properties of Rh, Pd, and Pt. To bolster the environmental sustainability of our method, we harness sunlight as the energy source to activate the photocatalysts, facilitating the complete dissolution of precious metals under natural light irradiation. This ecofriendly recovery approach demonstrated on commercial air purifiers, exhibits promise for broader application to a diverse range of deactivated air purification catalysts, potentially enabling implementation on a large scale.
基金supported by the National Key Research and Development Program of China (No. 2020YFA0211004)the National Natural Science Foundation of China (Nos. 22176128, 21876114)+4 种基金Sponsored by Program of Shanghai Government (Nos. 21XD1422800, 19DZ1205102, 19160712900)Chinese Education Ministry Key Laboratory and International Joint Laboratory on Resource Chemistry, and Shanghai Eastern Scholar Program“111 Innovation and Talent Recruitment Base on Photochemical and Energy Materials” (No. D18020)Shanghai Engineering Research Center of Green Energy Chemical Engineering (No. 18DZ2254200)Shanghai Frontiers Science Center of Biomimetic Catalysis。
文摘Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) is one of the most critical steps in the whole process.Herein,we regulated the different adsorption intensity of oxygen on the surface by designing phosphate (PO_(4)^(3-)) modified titanium oxide(TiO_(2)).The results show that the adsorption of oxygen on the photocatalyst surface is gradually enhanced,which effectively improves the dissolution rate of precious metals.PO_(4)^(3-)modification increased the photocatalytic dissolution rate of gold (Au) by 2.8 times.The photocatalytic activity of other precious metals dissolution (such as palladium (Pd),platinum (Pt),rhodium (Rh),ruthenium (Ru) and iridium (Ir)) was also significantly improved.It is applied to the recovery of precious metals from spent catalysts and electronic devices to significantly promote the recovery efficiency.This indicates the direction for designing more efficient photocatalysts for precious metal recovery.
基金supported by the National Key Research and Development Program of China (No.2020YFA0211004)the National Natural Science Foundation of China (Nos.22176128 and 21876114)+4 种基金the Program of Shanghai Academic Research Leader (No. 21XD1422800)Shanghai Government (Nos. 19DZ1205102 and 19160712900)Chinese Education Ministry Key Laboratory and International Joint Laboratory on Resource Chemistry, and Shanghai Eastern Scholar Program, “111 Innovation and Talent Recruitment Base on Photochemical and Energy Materials” (No. D18020)Shanghai Engineering Research Center of Green Energy Chemical Engineering (No. 18DZ2254200)Shanghai Frontiers Science Center of Biomimetic Catalysis。
文摘Photocatalytic Fenton reactions combined the advantages from both photocatalysis and Fenton reaction in mineralizing organic pollutants. The key problems are the efficiency and recycling stability. Herein, we reported a novel Fe_(2)O_(3)/TiO_(2)/reduced graphene oxide(FTG) nanocomposite synthesized by a facile solvothermal method. The TiO_(2)in FTG degraded organic pollutants and mineralized intermediates via photocatalysis under visible light irradiation, which could also promote Fenton reaction by accelerating Fe^(3+)-Fe^(2+)recycle. Meanwhile, the Fe_(2)O_(3)rapidly degraded organic pollutants via Fenton reactions, which also promoted photocatalysis by enhancing visible light absorbance and diminishing photoelectronhole recombination. The high distribution of TiO_(2)and Fe_(2)O_(3)on rGO, together with their strong interaction resulted in enhanced synergetic cooperation between photocatalysis and Fenton reactions, leading to the high mineralization efficiency of organic pollutants. More importantly, it could also inhibit the leaching of Fe species, leading to the long lifetime of FTG during photocatalytic Fenton reactions in a wide pH range from 3.4 to 9.2.
基金supported by the National Natural Science Foundation of China(21876114,21761142011,and 51572174)Shanghai Government(19160712900)+2 种基金International Joint Laboratory on Resource Chemistry(IJLRC),and Ministry of Education of China(PCSIRT_IRT_16R49)supported by The Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher LearningShuguang Research Program of Shanghai Education Committee.
文摘In order to develop efficient photocatalysts,great efforts have been made to reduce hexavalent chromium to trivalent chromium.The photocatalytic efficiency of this reduction depends largely on the adsorption and diffusion of hexavalent chromium ions on the surface of the photocatalyst.In this paper,polyanilineTiO2 composite can effectively improve the photocatalytic reduction performance and stability of hexavalent chromium ion.The effect of polyaniline(PANI) thickness on Cr(VI) activity and stability of photocatalytic reduction was studied by adjusting the content of PANI on Mesoporous TiO2(MT) surface.Under the irradiation conditions,the reaction results showed that the reduction rate was 100%,and the maximum reaction rate reached 0.62 min-1 when the PANI modification was 3.0%.Moreover,the results showed that the reduction performance remained 100% after ten cycles.The main reason is that the PANI modified on the surface of TiO2 is rich in positively charged amino group,which can efficiently adsorb the reactant Cr(VI),and make the product Cr(III) leave the reaction interface quickly,thus ensuring the performance of photocatalyst.
基金the National Key Technology R&D Program of China(No.2016YFA0202704)Beijing Municipal Science 8c Technology Commission(Nos.Z171100000317001,Z171100002017017,and Y3993113DF)the National Natural Science Foundation of China(Nos.51432005,5151101243,51561145021,and 21761142011).
文摘Environmental deterioration,especially water pollution,is widely dispersed and could affect the quality of people's life at large.Though the sewage treatment plants are constructed to meet the demands of cities,distributed treatment units are still in request for the supplementary of centralized purification beyond the range of plants.Electrochemical degradation can reduce organic pollution to some degree,but it has to be powered.Triboelectric nanogenerator(TENG)is a newly-invented technology for low-frequency mechanical energy harvesting.Here,by integrating a rotary TENG(R-TENG)as electric power source with an electrochemical cell containing a modified graphite felt cathode for hydrogen peroxide(H2O2)along with hydroxyl radical(·OH)generation by Fenton reaction and a platinum sheet anode for active chlorine generation,a self-powered electrochemical system(SPECS)was constructed.Under the driven of mechanical energy or wind flow,such SPECS can efficiently degrade dyes after power management in neutral condition without any O2 aeration.This work not only provides a guideline for optimizing self-powered electrochemical reaction,but also displays a strategy based on the conversion from distributed mechanical energy to chemical energy for environmental remediation.
文摘In this paper, the process of photocatalytic reduction of hexavalent chromium was investigated over Ti3+- modified TiO2 photocatalysts. The Ti3+ surface defects were repaired by annealing as-prepared sample at different temperatures to control the amount of Ti3+ sites. The samples were characterized by SEM, XRD, BET, UV-Vis absorption, EPR and XPS. The results showed Ti3+ defects were successfully doped in TiO2. The surface selective adsorption of hexavalent chromium [Cr2072 (Cr(VI))] and the desorption of trivalent chromium [Cr3+ (Cr(III))] were investigated during the process ofphotocatalytic reduction positive charges due to more Ti3+ defects on the surface show a Accordingly, the surface positive reduction of Cr(VI). charges controlled by the Ti3+ Zeta potential results presented that the increased significant improvement for adsorption of Cr(VI). defects play important roles in the photocatalytic