The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalys...The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalysts was proposed.The process included alkali (NaOH) hydrothermal treatment,sulfuric acid washing,and calcination.Anatase TiO_(2) in spent SCR catalyst was reconstructed by forming Na_(2)Ti_(2)O_(4)(OH)_(2) nanosheet during NaOH hydrothermal treatment and H_(2)Ti_(2)O_(4)(OH)_(2) during sulfuric acid washing.Anatase TiO_(2) was recovered by decomposing H_(2)Ti_(2)O_(4)(OH)_(2) during calcination.The surface pore properties of the recovered anatase TiO_(2) were adequately improved,and its specific surface area (SSA) and pore volume (PV) were 85 m^(2)·g^(-1)and 0.40 cm^(3)·g^(-1),respectively.The elements affecting catalytic abilities(arsenic and sodium) were also removed.The SCR catalyst was resynthesized using the recovered TiO_(2) as raw material,and its catalytic performance in NO selective reduction was comparable with that of commercial SCR catalyst.This study realized the sustainable recycling of anatase TiO_(2) from spent SCR catalyst.展开更多
Bronze phase titanium dioxide(TiO_(2)(B))could be a promising high-power anode for lithium ion battery.However,TiO_(2)(B)is a metastable material,so the as-synthesized samples are inevitably accompanied by the existen...Bronze phase titanium dioxide(TiO_(2)(B))could be a promising high-power anode for lithium ion battery.However,TiO_(2)(B)is a metastable material,so the as-synthesized samples are inevitably accompanied by the existence of anatase phases.It has been found that the TiO_(2)(B)'s purity is positively correlated with its electrochemical performance.Herein,we have established an accurate quantification of the TiO_(2)(B)/anatase ratio,by figuring out the function between the purity of TiO_(2)(B)phase in the high purity range and its Raman spectra features in combination of the calibration by the synchrotron radiation X-ray diffraction(XRD).Compared with the time-consuming electrochemical method,the rapid,sensitive and non-destructive features of Raman spectroscopy have made it a promising candidate for determining the purity of TiO_(2)(B).Further,the correlations developed in this work should be instructive in synthesizing pure TiO_(2)(B)and furthermore optimizing its electrochemical charge storage properties.展开更多
Effect of rare earth oxide Tb2O3 additive on transformation behavior and grain growth of anatase and photocatalytic activity for TiO2/(O′+β′)-Sialon multi-phase ceramic was investigated and the mechanism was dis...Effect of rare earth oxide Tb2O3 additive on transformation behavior and grain growth of anatase and photocatalytic activity for TiO2/(O′+β′)-Sialon multi-phase ceramic was investigated and the mechanism was discussed. X-ray diffractometer (XRD) was employed for the analysis of phase composition, grain size and lattice parameters of anatase. Photocatalytic activity of the composites was investigated through its photocatalytic degradation to methylene blue (MB) solution. The results showed that Tb2O3 significantly inhibited the transformarion process, which displayed an appreciably intensified effect with increasing Tb2O3 content. It could be attributed to the coaction of the active and passive influence mechanisms. For Tb3+ entering TiO2 lattice, replacing Ti4+ accelerated the transformation, whereas the lattice distortion caused by it was unfavorable for the process. On the other hand, the redox reaction between Tb3+ and TiO2 as well as the Tb2O3 deposited on the surface of TiO2 inhibited the transformation. The addition of Tb2O3 effectively restrained the grain growth of TiO2 and the effect became significant with the increase of its content. With the increase of Tb2O3 addition, the photocatalytic activity of the catalysts increased and then dropped after reaching the maximum at about 2%. The action mechanism of Tb2O3 could be attributed to its optical properties and its effect on phase transformation, grain growth and crystal structure of TiO2.展开更多
TiO2/(O' + β')-Sialon multiphase ceramics were prepared with nano TiO2 (anatase) powder and (O' + β')-Sialon powder as raw materials. Effect of Yb2O3 additive on transformation behavior of anatase for Ti...TiO2/(O' + β')-Sialon multiphase ceramics were prepared with nano TiO2 (anatase) powder and (O' + β')-Sialon powder as raw materials. Effect of Yb2O3 additive on transformation behavior of anatase for TiO2/(O' + β')-Sialon multi phase ceramic was investigated and its influence mechanism was discussed. XRD was employed for the analysis of phase composition and lattice parameters. The results show that even though Yb2O3 has no obvious influence on starting temperature of phase transformation, it significantly accelerates the transformation process, which displays a weakened effect with more Yb2O3 addition. There exist two forms of the added Yb2O3 : some enters TiO2 lattice and the other deposits on the surface of TiO2. The function of Yb2O3 on phase transformation of anatase can be attributed to the coaction of active and negative influence mechanisms as follows: some Yb^n+ enter TiO2 lattice and replace Ti^4+ , as well as the redox reaction between Yb^3+ and TiO2, which promote the transformation, whereas other Yb2O3 deposits on the surface of TiO2, and Ti- O-Yb bond is formed by the coaction of Yb^3+ and TiO2, which inhibit the process.展开更多
TiO_(2)-ZnO nanocomposites were synthesized by varying Ti:Zn molar ratio from 1:0.1(TZ-1:0.1)to 1:1(TZ-1:1).With increase in Zn content,from TZ-1:0.1 to TZ-1:0.2,anatase transformed to rutile phase.TZ-1:0.3,which cont...TiO_(2)-ZnO nanocomposites were synthesized by varying Ti:Zn molar ratio from 1:0.1(TZ-1:0.1)to 1:1(TZ-1:1).With increase in Zn content,from TZ-1:0.1 to TZ-1:0.2,anatase transformed to rutile phase.TZ-1:0.3,which contained a blend of phases,including rutile and anatase TiO_(2),ZnO,and zinc titanates,exhibited the narrowest bandgap(2.5±0.1 e V),and showed the highest photocatalytic activity.TZ-1:1 was predominated by zinc titanates.All the nanocomposites exhibited narrower bandgaps compared to pure TiO_(2)nanoparticles,facilitating visible light activity.This study was designed to explore whether a method targeting the removal of a specific crystalline phase(anatase)influenced the properties and photocatalytic activity of the nanocomposite.Selective dissolution not only removed anatase phase,but also led to significant loss of crystallinity,widened the bandgap,and adversely affected photocatalytic performance,in nanocomposites that contained>80%anatase phase(TZ-1:0.1 and TZ-1:0.2).However,in nanocomposites that contained less of anatase phase(TZ-1:0.3and TZ-1:1),the morphology,bandgap,crystallinity,and the extent of photocatalytic activity at the end of 240 min remained largely unaffected.Photocatalytic activity in TZ-1:0.3 and TZ-1:1 originated from a blend of phases comprising of less photocatalytically active phases,such as rutile TiO_(2),Zn TiO3,and Zn2TiO4,rather than from the anatase phase.The Ti:Zn molar ratio controlled the phases present in TiO_(2)-ZnO nanocomposites,which,in turn,controlled the physicochemical properties and visible light activity.Thus,in nanocomposites that contained a mix of several phases,the properties and photocatalytic activity were not dependent on anatase phase.展开更多
基金supported by the National Natural Science Foundation of China (52274411)the National Natural Science Foundation of China (51904287)the Innovation Academy for Green Manufacture,Chinese Academy of Sciences (IAGM2022D11)。
文摘The improper disposal of spent selective catalytic reduction (SCR) catalysts causes environmental pollution and metal resource waste.A novel process to recover anatase titanium dioxide (TiO_(2)) from spent SCR catalysts was proposed.The process included alkali (NaOH) hydrothermal treatment,sulfuric acid washing,and calcination.Anatase TiO_(2) in spent SCR catalyst was reconstructed by forming Na_(2)Ti_(2)O_(4)(OH)_(2) nanosheet during NaOH hydrothermal treatment and H_(2)Ti_(2)O_(4)(OH)_(2) during sulfuric acid washing.Anatase TiO_(2) was recovered by decomposing H_(2)Ti_(2)O_(4)(OH)_(2) during calcination.The surface pore properties of the recovered anatase TiO_(2) were adequately improved,and its specific surface area (SSA) and pore volume (PV) were 85 m^(2)·g^(-1)and 0.40 cm^(3)·g^(-1),respectively.The elements affecting catalytic abilities(arsenic and sodium) were also removed.The SCR catalyst was resynthesized using the recovered TiO_(2) as raw material,and its catalytic performance in NO selective reduction was comparable with that of commercial SCR catalyst.This study realized the sustainable recycling of anatase TiO_(2) from spent SCR catalyst.
基金This work was financially supported by the National Natural Science Foundation of China(22075074)Outstanding Young Scientists Research Funds from Hunan Province(2020JJ2004)+3 种基金Major Science and Technology Program of Hunan Province(2020WK2013)Natural Science Foundation of Hunan Province(2020JJ5035)National Natural Science Foundation of China(Grant No.11704185)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure(SKL201802SIC).
文摘Bronze phase titanium dioxide(TiO_(2)(B))could be a promising high-power anode for lithium ion battery.However,TiO_(2)(B)is a metastable material,so the as-synthesized samples are inevitably accompanied by the existence of anatase phases.It has been found that the TiO_(2)(B)'s purity is positively correlated with its electrochemical performance.Herein,we have established an accurate quantification of the TiO_(2)(B)/anatase ratio,by figuring out the function between the purity of TiO_(2)(B)phase in the high purity range and its Raman spectra features in combination of the calibration by the synchrotron radiation X-ray diffraction(XRD).Compared with the time-consuming electrochemical method,the rapid,sensitive and non-destructive features of Raman spectroscopy have made it a promising candidate for determining the purity of TiO_(2)(B).Further,the correlations developed in this work should be instructive in synthesizing pure TiO_(2)(B)and furthermore optimizing its electrochemical charge storage properties.
基金supported by the National Natural Science Foundation of China (50202004)
文摘Effect of rare earth oxide Tb2O3 additive on transformation behavior and grain growth of anatase and photocatalytic activity for TiO2/(O′+β′)-Sialon multi-phase ceramic was investigated and the mechanism was discussed. X-ray diffractometer (XRD) was employed for the analysis of phase composition, grain size and lattice parameters of anatase. Photocatalytic activity of the composites was investigated through its photocatalytic degradation to methylene blue (MB) solution. The results showed that Tb2O3 significantly inhibited the transformarion process, which displayed an appreciably intensified effect with increasing Tb2O3 content. It could be attributed to the coaction of the active and passive influence mechanisms. For Tb3+ entering TiO2 lattice, replacing Ti4+ accelerated the transformation, whereas the lattice distortion caused by it was unfavorable for the process. On the other hand, the redox reaction between Tb3+ and TiO2 as well as the Tb2O3 deposited on the surface of TiO2 inhibited the transformation. The addition of Tb2O3 effectively restrained the grain growth of TiO2 and the effect became significant with the increase of its content. With the increase of Tb2O3 addition, the photocatalytic activity of the catalysts increased and then dropped after reaching the maximum at about 2%. The action mechanism of Tb2O3 could be attributed to its optical properties and its effect on phase transformation, grain growth and crystal structure of TiO2.
文摘TiO2/(O' + β')-Sialon multiphase ceramics were prepared with nano TiO2 (anatase) powder and (O' + β')-Sialon powder as raw materials. Effect of Yb2O3 additive on transformation behavior of anatase for TiO2/(O' + β')-Sialon multi phase ceramic was investigated and its influence mechanism was discussed. XRD was employed for the analysis of phase composition and lattice parameters. The results show that even though Yb2O3 has no obvious influence on starting temperature of phase transformation, it significantly accelerates the transformation process, which displays a weakened effect with more Yb2O3 addition. There exist two forms of the added Yb2O3 : some enters TiO2 lattice and the other deposits on the surface of TiO2. The function of Yb2O3 on phase transformation of anatase can be attributed to the coaction of active and negative influence mechanisms as follows: some Yb^n+ enter TiO2 lattice and replace Ti^4+ , as well as the redox reaction between Yb^3+ and TiO2, which promote the transformation, whereas other Yb2O3 deposits on the surface of TiO2, and Ti- O-Yb bond is formed by the coaction of Yb^3+ and TiO2, which inhibit the process.
基金provided by Department of Science and Technology,New Delhi,India,under the Water Technology Initiative(WTI)scheme(Project code:DST/TM/WTI/2K15/101(G)).
文摘TiO_(2)-ZnO nanocomposites were synthesized by varying Ti:Zn molar ratio from 1:0.1(TZ-1:0.1)to 1:1(TZ-1:1).With increase in Zn content,from TZ-1:0.1 to TZ-1:0.2,anatase transformed to rutile phase.TZ-1:0.3,which contained a blend of phases,including rutile and anatase TiO_(2),ZnO,and zinc titanates,exhibited the narrowest bandgap(2.5±0.1 e V),and showed the highest photocatalytic activity.TZ-1:1 was predominated by zinc titanates.All the nanocomposites exhibited narrower bandgaps compared to pure TiO_(2)nanoparticles,facilitating visible light activity.This study was designed to explore whether a method targeting the removal of a specific crystalline phase(anatase)influenced the properties and photocatalytic activity of the nanocomposite.Selective dissolution not only removed anatase phase,but also led to significant loss of crystallinity,widened the bandgap,and adversely affected photocatalytic performance,in nanocomposites that contained>80%anatase phase(TZ-1:0.1 and TZ-1:0.2).However,in nanocomposites that contained less of anatase phase(TZ-1:0.3and TZ-1:1),the morphology,bandgap,crystallinity,and the extent of photocatalytic activity at the end of 240 min remained largely unaffected.Photocatalytic activity in TZ-1:0.3 and TZ-1:1 originated from a blend of phases comprising of less photocatalytically active phases,such as rutile TiO_(2),Zn TiO3,and Zn2TiO4,rather than from the anatase phase.The Ti:Zn molar ratio controlled the phases present in TiO_(2)-ZnO nanocomposites,which,in turn,controlled the physicochemical properties and visible light activity.Thus,in nanocomposites that contained a mix of several phases,the properties and photocatalytic activity were not dependent on anatase phase.