Soil remediation containing numerous organic contaminants is of great significance to ecological environment.Herein,the synergetic effects of Ce-Mn/Al_(2)O_(3)with different active components on catalytic thermal deso...Soil remediation containing numerous organic contaminants is of great significance to ecological environment.Herein,the synergetic effects of Ce-Mn/Al_(2)O_(3)with different active components on catalytic thermal desorption of chlorobenzene in soil were investigated.The optimized Ce-Mn/Al_(2)O_(3)drastically enhance the desorption efficiency of chlorobenzene,and the corresponding conversion reaches 100%within 1 h at a low temperature of 120℃.The superior performance is ascribed to the formation of Ce-Mn solid solution during the calcination process,resulting in a certain lattice change to the generation of abundant oxygen vacancies and acidic sites.Combining with the analysis of in-situ diffuse reflectance infrared spectroscopy and gas chromatography-mass spectrometry,the final products of chlorobenzene are decomposed into CO_(2),H_(2)O,Cl_(2)and HCl.This work sheds light on the rational design of highly-active catalysts for practical applications of sustainable soil remediation.展开更多
The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic e...The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic ecosystems and human health. To solve this problem, this study synthesized a composite of titanium dioxide (TiO2) and steel slag nanocomposites (SSNC) at a 1:2 mass ratio to create a robust photocatalyst for the treatment of synthetic wastewater. The efficacy of this catalyst in degrading various dye pollutants, including methylene blue (MB), was tested under simulated solar light conditions. Comprehensive analyses were conducted to assess the physical and chemical characteristics, crystalline structure, energy gap, and point of zero charge of the composite. The TiO2-SSNC composite catalyst exhibited excellent stability, with a point of zero charge at 8.342 and an energy gap of 2.4 eV. The degradation process conformed to pseudo-first-order kinetics. Optimization of operational parameters was achieved through the response surface methodology. Reusability tests demonstrated that the TiO2-SSNC composite catalyst effectively degraded up to 93.41% of MB in the suspended mode and 92.03% in the coated mode after five cycles. Additionally, the degradation efficiencies for various dyes were significant, highlighting the potential of the composite for broad applications in industrial wastewater treatment. This study also explored the degradation mechanisms and identified byproducts, establishing a pathway for contaminant breakdown. The cost-benefit analysis revealed a total cost of 0.842 8 USD per cubic meter for each treatment activity, indicating low operational and production costs. These findings underscore the promise of the TiO2-SSNC composite as a cost-effective and efficient alternative for wastewater purification.展开更多
Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolu...Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.展开更多
Pt-TiO2/Ce-MnOx catalysts were obtained by depositing TiO2 and platinum, respectively, on the Ce-Mn oxides prepared by co-precipitation method. The phases of CeO2 and anatase TiO2 were observed in the catalysts from X...Pt-TiO2/Ce-MnOx catalysts were obtained by depositing TiO2 and platinum, respectively, on the Ce-Mn oxides prepared by co-precipitation method. The phases of CeO2 and anatase TiO2 were observed in the catalysts from X-ray diffraction （XRD） patterns. X-ray photoelectron spectroscopy （XPS） revealed that lattice oxygen and surface active oxygen were found to be the major components of O 1 s. The experiment results showed that the kinetic constant of thermo-photocatalysis was 7.6 times of the kinetic constant of single photocatalysis, and was 2.29 times of the kinetic constant sum of photocatalytic and thermal catalytic reaction.展开更多
Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature...Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature programmed desorption(NH3-TPD),H2-temperature programmed reduction(H2-TPR)and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)techniques were used to analyze the structure and performance of catalysts.The results demonstrate that Ho doping increases the amount of acid sites and improves low temperature redox property of Ce-Mn/TiO_(2),which lead to excellent DeNOxperformance of Ho-Ce-Mn/TiO_(2)in the whole reaction temperature range.Sm doping results in decline of redox property,but it is beneficial to increasing the acid sites of Ce-Mn/TiO_(2).The increased surface acid sites and moderate oxidative ability impart Sm-Ce-Mn/TiO_(2)higher denitration activity and N2selectivity at temperature above 150℃.Lewis acid sites and redox property are the main factors affecting the activity of catalysts.Doping of Ho and Sm both improves sulfur resistance performance of Ce-Mn/TiO_(2)by inhibiting the adsorption of SO_(2)and formation of sulfate.Ce-Mn/TiO_(2)modified by Ho shows better sulfur resistance than that doped with Sm because of its more surface acid sites.展开更多
基金Project supported by the National Key Research and Development Program of China(2021YFB3500600,2021YFB3500605,2022YFB3504100)Key R&D Program of Jiangsu Province(BE2022142)+2 种基金Natural Science Foundation of Jiangsu Province(BK20220365)Jiangsu International Cooperation Project(BZ2021018)Chunhui Project Foundation of the Education Department of China(202200554)。
文摘Soil remediation containing numerous organic contaminants is of great significance to ecological environment.Herein,the synergetic effects of Ce-Mn/Al_(2)O_(3)with different active components on catalytic thermal desorption of chlorobenzene in soil were investigated.The optimized Ce-Mn/Al_(2)O_(3)drastically enhance the desorption efficiency of chlorobenzene,and the corresponding conversion reaches 100%within 1 h at a low temperature of 120℃.The superior performance is ascribed to the formation of Ce-Mn solid solution during the calcination process,resulting in a certain lattice change to the generation of abundant oxygen vacancies and acidic sites.Combining with the analysis of in-situ diffuse reflectance infrared spectroscopy and gas chromatography-mass spectrometry,the final products of chlorobenzene are decomposed into CO_(2),H_(2)O,Cl_(2)and HCl.This work sheds light on the rational design of highly-active catalysts for practical applications of sustainable soil remediation.
基金supported by the Department of Chemical and Petrochemical Engineering,Egypt-Japan University of Science and Technology.
文摘The steel industry produces many byproducts, requiring extensive land for storage and causing significant environmental contamination. Industrial effluents discharged into water bodies negatively impact both aquatic ecosystems and human health. To solve this problem, this study synthesized a composite of titanium dioxide (TiO2) and steel slag nanocomposites (SSNC) at a 1:2 mass ratio to create a robust photocatalyst for the treatment of synthetic wastewater. The efficacy of this catalyst in degrading various dye pollutants, including methylene blue (MB), was tested under simulated solar light conditions. Comprehensive analyses were conducted to assess the physical and chemical characteristics, crystalline structure, energy gap, and point of zero charge of the composite. The TiO2-SSNC composite catalyst exhibited excellent stability, with a point of zero charge at 8.342 and an energy gap of 2.4 eV. The degradation process conformed to pseudo-first-order kinetics. Optimization of operational parameters was achieved through the response surface methodology. Reusability tests demonstrated that the TiO2-SSNC composite catalyst effectively degraded up to 93.41% of MB in the suspended mode and 92.03% in the coated mode after five cycles. Additionally, the degradation efficiencies for various dyes were significant, highlighting the potential of the composite for broad applications in industrial wastewater treatment. This study also explored the degradation mechanisms and identified byproducts, establishing a pathway for contaminant breakdown. The cost-benefit analysis revealed a total cost of 0.842 8 USD per cubic meter for each treatment activity, indicating low operational and production costs. These findings underscore the promise of the TiO2-SSNC composite as a cost-effective and efficient alternative for wastewater purification.
基金support from the European Union Horizon 2020 program(project HERMES,nr.952184)the Ministry of Education,Youth and Sports of the Czech Republic for supporting CEMNAT(LM2023037)+1 种基金Czech-NanoLab(LM2023051)infrastructures for providing ALD,SEM,EDX,XPS,TEM,and XRDCzech Science Foundation(project 23-08019X,EXPRO).
文摘Synergistic interplays involving multiple active centers originating from TiO2 nanotube layers(TNT)and ruthenium(Ru)species comprising of both single atoms(SAs)and nanoparticles(NPs)augment the alkaline hydrogen evolution reaction(HER)by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H*desorption.Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8-0.4 nm NPs present on TNT layers,and it emerges with the highest HER activity among all the electrodes synthesized.A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti^(3+)states and the coexistence of Ru SAs and NPs.With insights from literature,the role of Ti^(3+),appropriate work functions of TNT layers and Ru,and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified.The aforementioned characteristics led to a remarkable performance by having 9mV onset potentials and 33 mV dec^(-1) of Tafel slopes and a higher turnover frequency of 1.72 H2 s^(-1) at 30 mV.Besides,a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.
文摘Pt-TiO2/Ce-MnOx catalysts were obtained by depositing TiO2 and platinum, respectively, on the Ce-Mn oxides prepared by co-precipitation method. The phases of CeO2 and anatase TiO2 were observed in the catalysts from X-ray diffraction （XRD） patterns. X-ray photoelectron spectroscopy （XPS） revealed that lattice oxygen and surface active oxygen were found to be the major components of O 1 s. The experiment results showed that the kinetic constant of thermo-photocatalysis was 7.6 times of the kinetic constant of single photocatalysis, and was 2.29 times of the kinetic constant sum of photocatalytic and thermal catalytic reaction.
文摘Sm and Ho were doped in Ce-Mn/TiO_(2)catalyst respectively to enhance its denitration performance at low temperature.X-ray diffraction(XRD),N2adsorption-desorption,X-ray photoelectron spectroscopy(XPS),NH3-temperature programmed desorption(NH3-TPD),H2-temperature programmed reduction(H2-TPR)and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)techniques were used to analyze the structure and performance of catalysts.The results demonstrate that Ho doping increases the amount of acid sites and improves low temperature redox property of Ce-Mn/TiO_(2),which lead to excellent DeNOxperformance of Ho-Ce-Mn/TiO_(2)in the whole reaction temperature range.Sm doping results in decline of redox property,but it is beneficial to increasing the acid sites of Ce-Mn/TiO_(2).The increased surface acid sites and moderate oxidative ability impart Sm-Ce-Mn/TiO_(2)higher denitration activity and N2selectivity at temperature above 150℃.Lewis acid sites and redox property are the main factors affecting the activity of catalysts.Doping of Ho and Sm both improves sulfur resistance performance of Ce-Mn/TiO_(2)by inhibiting the adsorption of SO_(2)and formation of sulfate.Ce-Mn/TiO_(2)modified by Ho shows better sulfur resistance than that doped with Sm because of its more surface acid sites.
