It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile ...The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile self-sacrifice template method is developed to prepare FeS encapsulated into N,S co-doped carbon(FeS/NSC)composite using melamine-cyanuric acid(MCA)supermolecule as a multifunctional template precursor.The function of MCA supermolecule for material synthesis is explored,revealing its special function as a dispersant,dopant and pore-forming agent.Furthermore,the effect of Fe source dosage on the morphology,structure and composition of the final products is explored.The resultant FeS/NSC-0.1(where 0.1 represents the mass of added Fe source)exhibits the most optimal proportion,characterized by a good dispersion status of FeS within the NSC matrix,effective N,S co-doping and ample porosity.Benefiting from these merits,the FeS/NSC-0.1 anode demonstrates significantly improved cycling stability and rate capability when compared to the counterparts.Undoubtedly,this work offers a universal method to produce advanced transition metal sulfide/carbon composite electrodes for energy storage and conversion systems.展开更多
Fe^3+and Zn^2+ions were doped into the lattice of CeO2 via the hydrothermal method.The micro structure and spectra features were analyzed systemically.XRD results show that the solid solubility of Fe^3+and Zn^2+ions i...Fe^3+and Zn^2+ions were doped into the lattice of CeO2 via the hydrothermal method.The micro structure and spectra features were analyzed systemically.XRD results show that the solid solubility of Fe^3+and Zn^2+ions in Ce1-x(Fe0.5Zn0.5)xO2 can be identified as x=0.16.The cell volumes are decreased by increasing the doped content.The TEM graphs prove that the grain size of the sample is about 10 nm,and the EDS result indicates that the doped contents are in accordance with that of the theory concentrations.Meanwhile,the doping also causes the increasing concentrations of the defects and oxygen vacancies which are supported by the XPS,Raman,UV and PL characterizations.The samples exhibit better catalytic activities for improving the hydrogen storage properties and the electrochemical kinetics of the ball milled Mg2Ni based composites.Further,the catalysis effects are improved by increasing the doped contents,which can be ascribed to the increasing contents of the oxygen vacancies,defects,the special electron transition states and the nature of the doped ions in CeO2-based solid solutions.展开更多
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
基金supported by the Science Technology Talents Lifting Project of Hunan Province(No.2022TJ-N16)the Natural Science Foundation of Hunan Province(Nos.2024JJ4022,2023JJ30277,2025JJ60382)+3 种基金the China Postdoctoral Fellowship Program(GZC20233205)the Scientifc Research Fund of Hunan Provincial Education Department,China(No.24B0270)the National Natural Science Foundation of China(No.32201646)the Key Project of Jiangxi Provincial Research and Development Program(No.20243BBI91001).
文摘The development of high-performance transition metal sulfide(TMS)/carbon composites to replace conventional graphite anode remains a critical challenge for advancing lithium-ion batteries(LIBs).In this study,a facile self-sacrifice template method is developed to prepare FeS encapsulated into N,S co-doped carbon(FeS/NSC)composite using melamine-cyanuric acid(MCA)supermolecule as a multifunctional template precursor.The function of MCA supermolecule for material synthesis is explored,revealing its special function as a dispersant,dopant and pore-forming agent.Furthermore,the effect of Fe source dosage on the morphology,structure and composition of the final products is explored.The resultant FeS/NSC-0.1(where 0.1 represents the mass of added Fe source)exhibits the most optimal proportion,characterized by a good dispersion status of FeS within the NSC matrix,effective N,S co-doping and ample porosity.Benefiting from these merits,the FeS/NSC-0.1 anode demonstrates significantly improved cycling stability and rate capability when compared to the counterparts.Undoubtedly,this work offers a universal method to produce advanced transition metal sulfide/carbon composite electrodes for energy storage and conversion systems.
基金supported by the National Natural Science Foundation of China(51962028,51501095)the Natural Science Foundation of Inner Mongolia(2017MS(LH)0516,2018MS05040,2018BS05010,2017MS(LH)0519)the Innovation Fund of Inner Mongolia University of Science and Technology(2018YQL02).
文摘Fe^3+and Zn^2+ions were doped into the lattice of CeO2 via the hydrothermal method.The micro structure and spectra features were analyzed systemically.XRD results show that the solid solubility of Fe^3+and Zn^2+ions in Ce1-x(Fe0.5Zn0.5)xO2 can be identified as x=0.16.The cell volumes are decreased by increasing the doped content.The TEM graphs prove that the grain size of the sample is about 10 nm,and the EDS result indicates that the doped contents are in accordance with that of the theory concentrations.Meanwhile,the doping also causes the increasing concentrations of the defects and oxygen vacancies which are supported by the XPS,Raman,UV and PL characterizations.The samples exhibit better catalytic activities for improving the hydrogen storage properties and the electrochemical kinetics of the ball milled Mg2Ni based composites.Further,the catalysis effects are improved by increasing the doped contents,which can be ascribed to the increasing contents of the oxygen vacancies,defects,the special electron transition states and the nature of the doped ions in CeO2-based solid solutions.
