The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-...The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.展开更多
Solid acid MoO_(3)/ZrO_(2)-TiO_(2)catalysts were prepared by impregnation method,and catalytic hydrolysis of difluorodichloromethane(CFC-12)over the catalyst was studied.The presence of MoO_(3)/ZrO_(2)-TiO_(2)catalyst...Solid acid MoO_(3)/ZrO_(2)-TiO_(2)catalysts were prepared by impregnation method,and catalytic hydrolysis of difluorodichloromethane(CFC-12)over the catalyst was studied.The presence of MoO_(3)/ZrO_(2)-TiO_(2)catalyst in polycrystalline state could be clearly observed by transmission electron microscopy(TEM).Mesopores were detected by N2 adsorption-desorption isotherms which further confirmed the MoO_(3)/ZrO_(2)-TiO_(2)structural characteristics of catalyst.The results of NH_(3)-TPD showed that the calcination temperatures had a great influence on the acidity of the catalyst,and the weak acidic site had a strong catalytic activity for the catalytic hydrolysis of CFC-12.Moreover,ZrO_(2)-TiO_(2)was highly dispersed in the MoO_(3)framework,suggested by powder X-ray diffraction(XRD)and N_(2)adsorption-desorption results.The effects of the catalyst calcination temperatures on the conversion rate of CFC-12 were studied.The effects of catalytic hydrolysis temperatures and water vapor concentration on the catalytic hydrolysis rate of CFC-12 were also studied.The solid acid MoO_(3)/ZrO_(2)-TiO_(2)was calcined at 500℃for 3 h at a catalytic hydrolysis temperature of 400℃and water vapor concentration of 83.18%,and catalytic hydrolysis rate of CFC-12 reached 98.65%.The hydrolysis rate of CFC-12 remained above 65.34%after 30 hours continuous reaction.展开更多
Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts wer...Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.展开更多
An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions...An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions at room temperature by grinding, which provides an efficient route to the synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one.This procedure offers several advantages including solvent-free conditions,excellent yields of products,simple work-up as well as reuse of catalysts which makes it a useful and attractive protocol for the synthesis of these compounds.展开更多
The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measuremen...The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measurement of magnetic susceptibility and rate of esterification. The structure of the superacids prepared in microwave field can be crystalline or non-crystalline, the latter has not been reported yet in literatures. Comparing with the traditional superacid, the non-crystalline Fe2O3/SO superacid prepared in microwave field has the highest magnetic susceptibility and catalytic activity. The di-coordination of Fe2O3 and SO and the S=O bi-bond were reinforced by microwave radiation, which is favorable for increasing the acid intensity of the Fe2O3/SO catalyst展开更多
A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures an...A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures and acidities were determined by XRD and Hammett method, respectively. The activity of the catalyst was studied as function of Al 2O 3 content, calcination temperature and time in the esterification of acetic acid with butanol, and a conversion of 96 5% was obtained. The catalyst gave also higher yields in syntheses of ketals and acetals: cyclohexanone ethylene ketal(86 2%), acetophenone ethylene ketal(78 5%), acetylacetic ester ketal(88 5%), benzaldehyde glycol acetal(76 3%). The chemical structures of the products were confirmed by IR spectra.展开更多
In this paper a new solid superacid catalyst SO 2- 4 MoO 3 TiO 2 was prepared.The activity of the catalyst in esterification of acetic acid and iso amyl alcohol was measured and compared with that of SO 2- 4 TiO 2 and...In this paper a new solid superacid catalyst SO 2- 4 MoO 3 TiO 2 was prepared.The activity of the catalyst in esterification of acetic acid and iso amyl alcohol was measured and compared with that of SO 2- 4 TiO 2 and MoO 3 TiO 2.The results showed that SO 2- 4 MoO 3 TiO 2 had better catalytic performance than SO 2- 4 TiO 2 and MoO 3 TiO 2.There was evident coordination between MoO 3 and SO 2- 4 when they coexisted on TiO 2.展开更多
基金supported by the National Natural Science Foundation of China (22108184)China Postdoctoral Science Foundation (2021TQ0221)+1 种基金the Sichuan Science and Technology Program (2021JDRC0117)Chengdu Science and Technology Program (2021-YF05-00378-SN)。
文摘The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.
基金Funded by the National Natural Science Foundation of China(No.51568068)the Young and Middle-aged Academic and Technical Leaders Reserve Talent Program(No.202105AC160054)。
文摘Solid acid MoO_(3)/ZrO_(2)-TiO_(2)catalysts were prepared by impregnation method,and catalytic hydrolysis of difluorodichloromethane(CFC-12)over the catalyst was studied.The presence of MoO_(3)/ZrO_(2)-TiO_(2)catalyst in polycrystalline state could be clearly observed by transmission electron microscopy(TEM).Mesopores were detected by N2 adsorption-desorption isotherms which further confirmed the MoO_(3)/ZrO_(2)-TiO_(2)structural characteristics of catalyst.The results of NH_(3)-TPD showed that the calcination temperatures had a great influence on the acidity of the catalyst,and the weak acidic site had a strong catalytic activity for the catalytic hydrolysis of CFC-12.Moreover,ZrO_(2)-TiO_(2)was highly dispersed in the MoO_(3)framework,suggested by powder X-ray diffraction(XRD)and N_(2)adsorption-desorption results.The effects of the catalyst calcination temperatures on the conversion rate of CFC-12 were studied.The effects of catalytic hydrolysis temperatures and water vapor concentration on the catalytic hydrolysis rate of CFC-12 were also studied.The solid acid MoO_(3)/ZrO_(2)-TiO_(2)was calcined at 500℃for 3 h at a catalytic hydrolysis temperature of 400℃and water vapor concentration of 83.18%,and catalytic hydrolysis rate of CFC-12 reached 98.65%.The hydrolysis rate of CFC-12 remained above 65.34%after 30 hours continuous reaction.
文摘Highly active solid superacid catalysts for n-butane isomerization, SZ/A1_2O_3-P, were prepared by supporting SO-(4-2)/ZrO2, (SZ) on y-A1_2O_3 carrier using a precipitation method. The activities of some catalysts were enhanced significantly j The activity of the most active sample. 60%SZ/Al_2O3-P, was even about 2 times more active than that of the SZ catalyst.
基金supported by the research foundation of Hebei University of Science and Technology
文摘An efficient synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one is achieved via a reaction of acenaphthe-nequinone and indoles catalyzed by solid superacid SO4^2-/TiO2 under solvent-free conditions at room temperature by grinding, which provides an efficient route to the synthesis of symmetrical 2,2-bis（1H-indol-3-yl）-2H-acenaphthen-1-one.This procedure offers several advantages including solvent-free conditions,excellent yields of products,simple work-up as well as reuse of catalysts which makes it a useful and attractive protocol for the synthesis of these compounds.
文摘The microwave radiation method was introduced to prepare the Fe_2O_3/SO solid superacid.Its structure and properties were investigated by means of X-ray diffraction and infrared spectrum analyses as well as measurement of magnetic susceptibility and rate of esterification. The structure of the superacids prepared in microwave field can be crystalline or non-crystalline, the latter has not been reported yet in literatures. Comparing with the traditional superacid, the non-crystalline Fe2O3/SO superacid prepared in microwave field has the highest magnetic susceptibility and catalytic activity. The di-coordination of Fe2O3 and SO and the S=O bi-bond were reinforced by microwave radiation, which is favorable for increasing the acid intensity of the Fe2O3/SO catalyst
文摘A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures and acidities were determined by XRD and Hammett method, respectively. The activity of the catalyst was studied as function of Al 2O 3 content, calcination temperature and time in the esterification of acetic acid with butanol, and a conversion of 96 5% was obtained. The catalyst gave also higher yields in syntheses of ketals and acetals: cyclohexanone ethylene ketal(86 2%), acetophenone ethylene ketal(78 5%), acetylacetic ester ketal(88 5%), benzaldehyde glycol acetal(76 3%). The chemical structures of the products were confirmed by IR spectra.
文摘In this paper a new solid superacid catalyst SO 2- 4 MoO 3 TiO 2 was prepared.The activity of the catalyst in esterification of acetic acid and iso amyl alcohol was measured and compared with that of SO 2- 4 TiO 2 and MoO 3 TiO 2.The results showed that SO 2- 4 MoO 3 TiO 2 had better catalytic performance than SO 2- 4 TiO 2 and MoO 3 TiO 2.There was evident coordination between MoO 3 and SO 2- 4 when they coexisted on TiO 2.
