Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-...Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.展开更多
Flow anodic oxidation system has demonstrated to be a promising and environmental benign water treatment technology because of its advantages of high contaminant removal efficiency and low energy consumption.However,t...Flow anodic oxidation system has demonstrated to be a promising and environmental benign water treatment technology because of its advantages of high contaminant removal efficiency and low energy consumption.However,traditional setup needs an external unit for flow anode material separation and recovery,which inevitably increases the capital cost and hinders its continuous operation.Herein,a specific porous cathode is introduced to achieve continuous water purification with high contaminant removal in a flow anodic oxidation system.The efuent concentration of carbamazepine(CBZ),a common and model contaminant widely detected in natural water environment,was reduced by 99%.The linear sweep voltammetry(LSV)and quenching tests demonstrated that HO·was the dominant reactive species.While the removal of contaminants was inhibited in practical surface water,largely related to the quenching by dissolved organic matter and bicarbonate,the flow anodic oxidation process was competent in alleviating the ecotoxicity following oxidation.Our study constructs a modular device for cost-effective continuous water purification and provides insight into the mechanisms of flow andic oxidation.展开更多
Correlated phase and microstructural evolution are systematically investigated by electron microscopies in Sr-deficient Sr(Ti,Nb)O_(3)(STNO)thermoelectric ceramics incorporated with different fraction of reduced graph...Correlated phase and microstructural evolution are systematically investigated by electron microscopies in Sr-deficient Sr(Ti,Nb)O_(3)(STNO)thermoelectric ceramics incorporated with different fraction of reduced graphene oxide(RGO).It is found that while no impurity except for very few Ti_(3)O_(5) precipitates are observed in monolithic STNO,the Nb-enriched rutile TiO_(2) appears in RGO/STNO composites.With increasing RGO content,the amount of precipitates increase at first and then decrease when RGO content becomes high,which can be ascribed to the formation of local Magneli phase.In addition,the energy-dispersive X-ray spectra combined with cathodoluminescence characterization indicates that the variation of Sr deficiency experiences the opposite trend with respect to the precipitates content.These findings clearly reveal the unique reducing effect of RGO on the microstructure of doped SrTiO_(3) with Sr deficiency,which can greatly facilitate the design of perovskite based thermoelectric materials of hierarchical structure.展开更多
The thermoelectric properties of Sr1-xBixTiO_(3-δ)(0≤x≤0.07)have been investigated.Dense ceramics of Sr1-xBixTiO_(3-δ) and Sr0.95TiO_(3-δ) have been prepared by solid-state reaction and conventional sintering in ...The thermoelectric properties of Sr1-xBixTiO_(3-δ)(0≤x≤0.07)have been investigated.Dense ceramics of Sr1-xBixTiO_(3-δ) and Sr0.95TiO_(3-δ) have been prepared by solid-state reaction and conventional sintering in air followed by annealing in a reducing atmosphere.XRD and SEM analyses show that the rutile TiO_(2 i)n Sr_(0.95)TiO_(3) formed after sintering becomes Magneli phase of TinO_(2n-1) after annealing.Moreover,Bi resolves from Sr1-xBixTiO_(3 )after annealing,resulting in the formation of Sr1-xBixTiO_(3-δ)/Bi/TinO_(2n-1) composites.With increasing Bi content in Sr1-xBixTiO_(3-δ),the electrical conductivity increases while the absolute values of the Seebeck coefficient decrease as a result of increasing carrier concentration.The thermal conductivity of SrTiO_(3-δ) is reduced by doping Bi up to x=0.07.Highest ZT~0.13 is obtained in Sr0.93Bi0.07TiO_(3-δ) at 1000 K.展开更多
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.
基金financially supported by the Basic Science Center Project of the National Natural Science Foundation of China(No.52388101)Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2019ZT08L213)the National Natural Science Foundation of China(No.52100030)。
文摘Flow anodic oxidation system has demonstrated to be a promising and environmental benign water treatment technology because of its advantages of high contaminant removal efficiency and low energy consumption.However,traditional setup needs an external unit for flow anode material separation and recovery,which inevitably increases the capital cost and hinders its continuous operation.Herein,a specific porous cathode is introduced to achieve continuous water purification with high contaminant removal in a flow anodic oxidation system.The efuent concentration of carbamazepine(CBZ),a common and model contaminant widely detected in natural water environment,was reduced by 99%.The linear sweep voltammetry(LSV)and quenching tests demonstrated that HO·was the dominant reactive species.While the removal of contaminants was inhibited in practical surface water,largely related to the quenching by dissolved organic matter and bicarbonate,the flow anodic oxidation process was competent in alleviating the ecotoxicity following oxidation.Our study constructs a modular device for cost-effective continuous water purification and provides insight into the mechanisms of flow andic oxidation.
基金supported by the National Natural Science Foundation of China[Grant numbers 51532006,51432004]State Administration of Foreign Experts Affairs of China,111 project[Grant number D16002]the Opening Project of Key Laboratory of Inorganic Functional Materials and Devices,Chinese Academy of Sciences(Grant number KLIFMD201804).
文摘Correlated phase and microstructural evolution are systematically investigated by electron microscopies in Sr-deficient Sr(Ti,Nb)O_(3)(STNO)thermoelectric ceramics incorporated with different fraction of reduced graphene oxide(RGO).It is found that while no impurity except for very few Ti_(3)O_(5) precipitates are observed in monolithic STNO,the Nb-enriched rutile TiO_(2) appears in RGO/STNO composites.With increasing RGO content,the amount of precipitates increase at first and then decrease when RGO content becomes high,which can be ascribed to the formation of local Magneli phase.In addition,the energy-dispersive X-ray spectra combined with cathodoluminescence characterization indicates that the variation of Sr deficiency experiences the opposite trend with respect to the precipitates content.These findings clearly reveal the unique reducing effect of RGO on the microstructure of doped SrTiO_(3) with Sr deficiency,which can greatly facilitate the design of perovskite based thermoelectric materials of hierarchical structure.
文摘The thermoelectric properties of Sr1-xBixTiO_(3-δ)(0≤x≤0.07)have been investigated.Dense ceramics of Sr1-xBixTiO_(3-δ) and Sr0.95TiO_(3-δ) have been prepared by solid-state reaction and conventional sintering in air followed by annealing in a reducing atmosphere.XRD and SEM analyses show that the rutile TiO_(2 i)n Sr_(0.95)TiO_(3) formed after sintering becomes Magneli phase of TinO_(2n-1) after annealing.Moreover,Bi resolves from Sr1-xBixTiO_(3 )after annealing,resulting in the formation of Sr1-xBixTiO_(3-δ)/Bi/TinO_(2n-1) composites.With increasing Bi content in Sr1-xBixTiO_(3-δ),the electrical conductivity increases while the absolute values of the Seebeck coefficient decrease as a result of increasing carrier concentration.The thermal conductivity of SrTiO_(3-δ) is reduced by doping Bi up to x=0.07.Highest ZT~0.13 is obtained in Sr0.93Bi0.07TiO_(3-δ) at 1000 K.
