Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investig...Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investigated.The roasting and leaching conditions were optimized:the leaching efficiencies of vanadium and tungsten were 91.19%and 85.36%,respectively,when 18 equivalents of K_(2)CO_(3)were added to perform the roasting at 900℃ for 2 h,followed by leaching at 90°C for 1 h.Notably,in the described conditions,the leaching rate of silicon was only 28.55%.Titanates,including K_(2)Ti_(6)O_(13)and KTi8017,were also produced.Si removal was achieved in 85%efficiency adjusting the pH to 9.5,and the Si impurity thus isolated was composed of amorphous Si.Tungsten and vanadium were precipitated using CaCl_(2).At pH 10 and following the addition of 0.10 mol of H_(2)O_(2)and 16 equivalents of CaCl_(2),the precipitating efficiencies of tungsten and vanadium were 96.89%and 99.65%,respectively.The overall yield of tungsten and vanadium was 82.71%and 90.87%,respectively.展开更多
The surface reaction of Co 3Ti alloys (with and without Fe) with water vapor was investigated by using Auger electron spectroscopy (AES). The results showed that the rate of the surface reaction is much lower in Co 21...The surface reaction of Co 3Ti alloys (with and without Fe) with water vapor was investigated by using Auger electron spectroscopy (AES). The results showed that the rate of the surface reaction is much lower in Co 21 5Ti 3Fe alloy as compared with Co 3Ti (Co 23Ti) alloy. The surface reaction of Co 21 5Ti 3Fe alloy with water vapor saturates at exposure of 2×10 -3 Pa·s, but it does not saturate even at 0 1 Pa·s exposure for Co 3Ti alloy without Fe. The results also indicated that the kinetic of the surface reaction of Co 21 5Ti 3Fe with water vapor is much smaller than that of Co 3Ti at the same exposure. All the above results illustrate that the suppression of environmental embrittlement by addition of Fe to Co 3Ti alloy is attributed to its reduction of the surface reaction kinetics with water vapor.展开更多
The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, w...The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, we hydrothermally synthesized a Fe2O3 photoanode. In addition, d-Fe OOH synthesized via dip-coating and hydrothermally prepared h-FeOOH were used as cocatalysts and their synergistic combinations with cobalt phosphate(Co-Pi) were investigated. The synergy between h-FeOOH and Co-Pi was remarkable, whereas that between d-Fe OOH and Co-Pi was negligible. For example, the onset potentials of the Co-Pi/h-FeOOH and Co-Pi/d-FeOOH dual catalysts, were cathodically shifted by 270 and 170 m V, respectively. Moreover, the photocurrent density of the Co-Pi/h-FeOOH/Fe2O3 anode was significantly higher than that of the Co-Pi/d-FeOOH/Fe2O3 one. The synergistic effect of Co-Pi and h-FeOOH could be attributed to the significantly inhibited recombination of surface charges owing to the formation of a p-n junction between β-FeOOH and Fe2O3 and the large contact area between the granular h-FeOOH and Co-Pi. However, the thin amorphous FeOOH layer of the Co-Pi/d-FeOOH/Fe2O3 anode acted as a hole-transfer medium, and weakly promoted the kinetics of the charge transfer process.展开更多
In this work. phenol and oxalic acid （OA） degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe3 ＋/TiO2 catalyst. The ferrioxalate complex formed between Fe3＋ and oxalate ...In this work. phenol and oxalic acid （OA） degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe3 ＋/TiO2 catalyst. The ferrioxalate complex formed between Fe3＋ and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of-OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe3＋/TiO2 catalyzed processes, because Fe＋ was greatly reduced but not regenerated in many cases. The synergetic effect was found to be highly related with the property of the target pollutants. Fe3 ＋/TiO2 catalyzed system showed the highest ability to destroy organics, but the TiO2 catalyzed system showed little higher synergy.展开更多
Doping of foreign atoms and construction of unique structures are considered as effective approaches to design high-activity and strongdurability electrocatalysts.Herein,we report Fe-doped nickel hydroxide carbonate h...Doping of foreign atoms and construction of unique structures are considered as effective approaches to design high-activity and strongdurability electrocatalysts.Herein,we report Fe-doped nickel hydroxide carbonate hierarchical microtubes with Ag nanoparticles(denoted Ag/NiFeHC HMTs)through hydrolysis precipitation process.Experimental tests and density functional theory calculations reveal that Fe doping can tune the electron configuration to enhance the conductivity,markedly improve the electrochemical surface area to expose more active sites,and act as reactive centers to lower the free energy of the rate determination step.In addition,the unique hierarchical structure can also offer active sites and excellent cycling stability.Benefitting from these advantages,the as-obtained Ag/NiFeHC HMTs show excellent oxygen evolution reaction activity,with an overpotential of 208 mV at 10 mA cm^(−2)in 1.0M KOH.Also,it could achieve long-term stability at a current density of 20 mA cm^(−2)for 24 h.展开更多
Humic acid(HA)was carbonized at 300,400 and 500℃ and then functionalized with 1 wt%–12 wt%Fe(Ⅲ)respectively[CHA300/400/500-Fe(Ⅲ)].Adsorption of such Fe(III)-functionalized carbonized HA as adsorbents to aqueous te...Humic acid(HA)was carbonized at 300,400 and 500℃ and then functionalized with 1 wt%–12 wt%Fe(Ⅲ)respectively[CHA300/400/500-Fe(Ⅲ)].Adsorption of such Fe(III)-functionalized carbonized HA as adsorbents to aqueous tetracycline(TC:25 mg·L^-1)was studied.The adsorption equilibrium time for CHA400-Fe(Ⅲ)to TC was 6 h faster and the adsorption removal efficiency(Re)was two times higher than that of HA/CHA.The adsorption Reof CHA400-Fe(Ⅲ)loaded 10%iron[CHA400-(10%)Fe(Ⅲ)]to TC could reach 99.8%at 8 h and still kept80.6%after 8 cycles.The adsorption kinetics were well fitted to the pseudo-second-order equation and the adsorption isotherms could be well delineated via Langmuir equations(R^2N 0.99),indicating that the homogeneous chemical adsorption of TC occurred on the adsorbents.The main adsorption mechanisms of TC were complexation Fe(III)and hydrophobic distribution.Electropositive and electronegative repulsion between TC and CHA400-(10%)Fe(Ⅲ)at lowly p H(2)and highly p H(8–10)respectively,leaded to the relatively low adsorption capacity and more notable influence of ion concentration.When the p H was between 4 and 8,TC mainly existed in neutral molecules(TCH2),so the influence of ion concentration was not obvious.The dynamic adsorption results showed that the CHA400-(10%)Fe(Ⅲ)could continuously treat about 2.4 L TC(27 mg·L^-1)wastewater with the effluent concentration as low as 0.068 mg·L^-1.Our study suggested a broad application prospect of a new,effective,lowcost and environment-friendly adsorbent CHA400-(10%)Fe(Ⅲ)for treatment of low-concentration TC polluted wastewater.展开更多
β-Fe2O3·H2O is prepared by reacting FeCl3, K2CO3, an oxidizing agent HIO4 and a metal chelating agent K3PO4 at 65~ 70℃. The prepared β-Fe2O3' H2O is introduced into the mixture of KOH, KOCl and a ferrate s...β-Fe2O3·H2O is prepared by reacting FeCl3, K2CO3, an oxidizing agent HIO4 and a metal chelating agent K3PO4 at 65~ 70℃. The prepared β-Fe2O3' H2O is introduced into the mixture of KOH, KOCl and a ferrate stabilizer KI, and reacted at room temperature for 5 h to produce a ferrate-containing cake. The cake is dried to give a water-free dried potassium ferrate (VI).展开更多
基金from the Fundamental Research Funds for the Central Universities(2010YH14).
文摘Waste selective catalytic reduction(SCR)catalysts are potential environmental hazards.In this study,the recovery of vanadium and tungsten from waste SCR catalysts by K_(2)CO_(3)roasting and water leaching was investigated.The roasting and leaching conditions were optimized:the leaching efficiencies of vanadium and tungsten were 91.19%and 85.36%,respectively,when 18 equivalents of K_(2)CO_(3)were added to perform the roasting at 900℃ for 2 h,followed by leaching at 90°C for 1 h.Notably,in the described conditions,the leaching rate of silicon was only 28.55%.Titanates,including K_(2)Ti_(6)O_(13)and KTi8017,were also produced.Si removal was achieved in 85%efficiency adjusting the pH to 9.5,and the Si impurity thus isolated was composed of amorphous Si.Tungsten and vanadium were precipitated using CaCl_(2).At pH 10 and following the addition of 0.10 mol of H_(2)O_(2)and 16 equivalents of CaCl_(2),the precipitating efficiencies of tungsten and vanadium were 96.89%and 99.65%,respectively.The overall yield of tungsten and vanadium was 82.71%and 90.87%,respectively.
文摘The surface reaction of Co 3Ti alloys (with and without Fe) with water vapor was investigated by using Auger electron spectroscopy (AES). The results showed that the rate of the surface reaction is much lower in Co 21 5Ti 3Fe alloy as compared with Co 3Ti (Co 23Ti) alloy. The surface reaction of Co 21 5Ti 3Fe alloy with water vapor saturates at exposure of 2×10 -3 Pa·s, but it does not saturate even at 0 1 Pa·s exposure for Co 3Ti alloy without Fe. The results also indicated that the kinetic of the surface reaction of Co 21 5Ti 3Fe with water vapor is much smaller than that of Co 3Ti at the same exposure. All the above results illustrate that the suppression of environmental embrittlement by addition of Fe to Co 3Ti alloy is attributed to its reduction of the surface reaction kinetics with water vapor.
文摘The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, we hydrothermally synthesized a Fe2O3 photoanode. In addition, d-Fe OOH synthesized via dip-coating and hydrothermally prepared h-FeOOH were used as cocatalysts and their synergistic combinations with cobalt phosphate(Co-Pi) were investigated. The synergy between h-FeOOH and Co-Pi was remarkable, whereas that between d-Fe OOH and Co-Pi was negligible. For example, the onset potentials of the Co-Pi/h-FeOOH and Co-Pi/d-FeOOH dual catalysts, were cathodically shifted by 270 and 170 m V, respectively. Moreover, the photocurrent density of the Co-Pi/h-FeOOH/Fe2O3 anode was significantly higher than that of the Co-Pi/d-FeOOH/Fe2O3 one. The synergistic effect of Co-Pi and h-FeOOH could be attributed to the significantly inhibited recombination of surface charges owing to the formation of a p-n junction between β-FeOOH and Fe2O3 and the large contact area between the granular h-FeOOH and Co-Pi. However, the thin amorphous FeOOH layer of the Co-Pi/d-FeOOH/Fe2O3 anode acted as a hole-transfer medium, and weakly promoted the kinetics of the charge transfer process.
基金Supported by the Natural Science Foundation of Beijing City(8172043)the National Science Fund for Distinguished Young Scholars(51425405)National Natural Science Foundation of China(51378487)
文摘In this work. phenol and oxalic acid （OA） degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe3 ＋/TiO2 catalyst. The ferrioxalate complex formed between Fe3＋ and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of-OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe3＋/TiO2 catalyzed processes, because Fe＋ was greatly reduced but not regenerated in many cases. The synergetic effect was found to be highly related with the property of the target pollutants. Fe3 ＋/TiO2 catalyzed system showed the highest ability to destroy organics, but the TiO2 catalyzed system showed little higher synergy.
基金Zhejiang Provincial Natural Science Foundation of China,Grant/Award Number:LQ20B010002。
文摘Doping of foreign atoms and construction of unique structures are considered as effective approaches to design high-activity and strongdurability electrocatalysts.Herein,we report Fe-doped nickel hydroxide carbonate hierarchical microtubes with Ag nanoparticles(denoted Ag/NiFeHC HMTs)through hydrolysis precipitation process.Experimental tests and density functional theory calculations reveal that Fe doping can tune the electron configuration to enhance the conductivity,markedly improve the electrochemical surface area to expose more active sites,and act as reactive centers to lower the free energy of the rate determination step.In addition,the unique hierarchical structure can also offer active sites and excellent cycling stability.Benefitting from these advantages,the as-obtained Ag/NiFeHC HMTs show excellent oxygen evolution reaction activity,with an overpotential of 208 mV at 10 mA cm^(−2)in 1.0M KOH.Also,it could achieve long-term stability at a current density of 20 mA cm^(−2)for 24 h.
基金financially supported by the National Natural Science Foundation of China(No.51641209)。
文摘Humic acid(HA)was carbonized at 300,400 and 500℃ and then functionalized with 1 wt%–12 wt%Fe(Ⅲ)respectively[CHA300/400/500-Fe(Ⅲ)].Adsorption of such Fe(III)-functionalized carbonized HA as adsorbents to aqueous tetracycline(TC:25 mg·L^-1)was studied.The adsorption equilibrium time for CHA400-Fe(Ⅲ)to TC was 6 h faster and the adsorption removal efficiency(Re)was two times higher than that of HA/CHA.The adsorption Reof CHA400-Fe(Ⅲ)loaded 10%iron[CHA400-(10%)Fe(Ⅲ)]to TC could reach 99.8%at 8 h and still kept80.6%after 8 cycles.The adsorption kinetics were well fitted to the pseudo-second-order equation and the adsorption isotherms could be well delineated via Langmuir equations(R^2N 0.99),indicating that the homogeneous chemical adsorption of TC occurred on the adsorbents.The main adsorption mechanisms of TC were complexation Fe(III)and hydrophobic distribution.Electropositive and electronegative repulsion between TC and CHA400-(10%)Fe(Ⅲ)at lowly p H(2)and highly p H(8–10)respectively,leaded to the relatively low adsorption capacity and more notable influence of ion concentration.When the p H was between 4 and 8,TC mainly existed in neutral molecules(TCH2),so the influence of ion concentration was not obvious.The dynamic adsorption results showed that the CHA400-(10%)Fe(Ⅲ)could continuously treat about 2.4 L TC(27 mg·L^-1)wastewater with the effluent concentration as low as 0.068 mg·L^-1.Our study suggested a broad application prospect of a new,effective,lowcost and environment-friendly adsorbent CHA400-(10%)Fe(Ⅲ)for treatment of low-concentration TC polluted wastewater.
文摘β-Fe2O3·H2O is prepared by reacting FeCl3, K2CO3, an oxidizing agent HIO4 and a metal chelating agent K3PO4 at 65~ 70℃. The prepared β-Fe2O3' H2O is introduced into the mixture of KOH, KOCl and a ferrate stabilizer KI, and reacted at room temperature for 5 h to produce a ferrate-containing cake. The cake is dried to give a water-free dried potassium ferrate (VI).
