For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concent...For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_x(OH)_y~(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_2(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.展开更多
Compound casting is an efficient method for bonding dissimilar metals,in which a dramatic reaction can occur between the melt and solid.The centrifugal casting process,a type of compound casting,was applied to cast Al...Compound casting is an efficient method for bonding dissimilar metals,in which a dramatic reaction can occur between the melt and solid.The centrifugal casting process,a type of compound casting,was applied to cast Al/Mg dissimilar bimetals.Magnesium melt was poured at 700 °C,with melt-to-solid volume ratios(Vm/Vs) of 1.5 and 3,into a preheated hollow aluminum cylinder.The preheating temperatures of the solid part were 320,400,and 450 °C,and the constant rotational speed was 1,600 rpm.The cast parts were kept inside the casting machine until reaching the cooling temperature of 150 °C.The result showed that an increase in preheating temperature from 320 to 450 °C led to an enhanced reaction layer thickness.In addition,an increase in the Vm/Vs from 1.5 to 3 resulted in raising the interface thickness from 1.2 to 1.8 mm.Moreover,the interface was not continuously formed when a Vm/Vs of 3 was selected.In this case,the force of contraction overcame the resultant acting force on the interface.An interface formed at the volume ratio of 1.5 was examined using scanning electron microscopy(SEM) equipped with energy-dispersive X-ray spectroscopy(EDS),and the results demonstrated the formation of Al_(3)Mg_(2),Al_(12)Mg_(17) and(δ+Al_(12)Mg_(17)) eutectic structures in the interface.展开更多
In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrot...In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest mesoporous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluenexylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behavior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylbenzene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.展开更多
Methacrylic acid,an important organic chemical,is commercially manufactured starting from fossil feedstock.The decarboxylation of itaconic acid derived for biomass is a green route to the synthesis of methacrylic acid...Methacrylic acid,an important organic chemical,is commercially manufactured starting from fossil feedstock.The decarboxylation of itaconic acid derived for biomass is a green route to the synthesis of methacrylic acid.In view of the problems existing in the researches on this route such as use of noble metal catalyst,harsh reaction conditions and low desired-product yield,we prepared a series of hydroxyapatite catalysts with different Ca/P molar ratios and evaluated their catalytic performance.The results showed that the hydroxyapatite catalyst with a Ca/P molar ratio of 1.58 had the best catalytic activity.The highest yield of MAA up to 61.2%was achieved with basically complete conversion of itaconic acid under the suitable reaction conditions of 1 equivalent of NaOH,2 MPa of N_(2),250℃,and 2 h.On this basis,a reaction network for the decarboxylation of itaconic acid to methacrylic acid catalyzed by hydroxyapatite was established.With the aid of catalyst characterization using X-ray powder diffraction,NH3/CO2 temperature-programmed desorption,N_(2)physisorption,inductively coupled plasma optical emission spectrometry,and scanning electron microscopy,we found that the distribution of surface acid sites and basic sites,crystal growth orientation,texture properties and morphology of hydroxyapatite varied with the Ca/P molar ratio.Furthermore,the change of the crystal growth orientation and its influence on the surface acidity and alkalinity were clarified.展开更多
基金financial supports from the National Key Research and Development Program of China(No.2022YFB3504501)the National Natural Science Foundation of China(Nos.52274355,91962211)the Gansu Province Science and Technology Major Special Project,China(No.22ZD6GD061)。
文摘For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_x(OH)_y~(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_2(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.
基金supported by the Key P rogram of National Natural Science Foundation of China(No.51931003)the National Natural Science Foundation of China(Nos.52271033,52071179)+1 种基金the Natural Science Foundation of Jiangsu Province,China(No.BK20221493)the Foundation of Qinglan Project for Colleges and Universities in Jiangsu Province,China.
文摘Compound casting is an efficient method for bonding dissimilar metals,in which a dramatic reaction can occur between the melt and solid.The centrifugal casting process,a type of compound casting,was applied to cast Al/Mg dissimilar bimetals.Magnesium melt was poured at 700 °C,with melt-to-solid volume ratios(Vm/Vs) of 1.5 and 3,into a preheated hollow aluminum cylinder.The preheating temperatures of the solid part were 320,400,and 450 °C,and the constant rotational speed was 1,600 rpm.The cast parts were kept inside the casting machine until reaching the cooling temperature of 150 °C.The result showed that an increase in preheating temperature from 320 to 450 °C led to an enhanced reaction layer thickness.In addition,an increase in the Vm/Vs from 1.5 to 3 resulted in raising the interface thickness from 1.2 to 1.8 mm.Moreover,the interface was not continuously formed when a Vm/Vs of 3 was selected.In this case,the force of contraction overcame the resultant acting force on the interface.An interface formed at the volume ratio of 1.5 was examined using scanning electron microscopy(SEM) equipped with energy-dispersive X-ray spectroscopy(EDS),and the results demonstrated the formation of Al_(3)Mg_(2),Al_(12)Mg_(17) and(δ+Al_(12)Mg_(17)) eutectic structures in the interface.
基金supported by the National Natural Science Foundation of China (51974312, 51974308)the National Key Research & Development Program of China (2019YFE0100100)。
文摘In order to further improve the catalytic performance of zeolite catalyst for methanol to aromatics(MTA)technology, the double-tier SAPO-34/ZSM-5/quartz composite zeolite films were successfully synthesized via hydrothermal crystallization. The Si/Al ratio of SAPO-34 film was used as the only variable to study this material. The composite zeolite material with 0.6Si/Al ratio of SAPO-34 has the largest mesoporous specific surface area and the most suitable acid distribution. The catalytic performance for the MTA process showed that 0.6-SAPO-34/ZSM-5/quartz film has as high as 50.3% benzene-toluenexylene selectivity and 670 min lifetime. The MTA reaction is carried out through the path we designed to effectively avoid the hydrocarbon pool circulation of ZSM-5 zeolite, so as to improve the aromatics selectivity and inhibit the occurrence of deep side reactions to a great extent. The coke deposition behavior was monitored by thermogravimetric analysis and gas chromatograph/mass spectrometer, it is found that with the increase of Si/Al ratio, the active intermediates changed from low-substituted methylbenzene to high-substituted methylbenzene, which led to the rapid deactivation of the catalyst. This work provides a possibility to employ the synergy effect of composite zeolite film synthesizing anti-carbon deposition catalyst in MTA reaction.
基金supported by the National Natural Science Foundation of China(Grant No.21978066)Basic Research Program of Hebei Province for Natural Science Foundation and Key Basic Research Project(Grant No.18964308D)the Key Program of Natural Science Foundation of Hebei Province(Grant No.B2020202048).
文摘Methacrylic acid,an important organic chemical,is commercially manufactured starting from fossil feedstock.The decarboxylation of itaconic acid derived for biomass is a green route to the synthesis of methacrylic acid.In view of the problems existing in the researches on this route such as use of noble metal catalyst,harsh reaction conditions and low desired-product yield,we prepared a series of hydroxyapatite catalysts with different Ca/P molar ratios and evaluated their catalytic performance.The results showed that the hydroxyapatite catalyst with a Ca/P molar ratio of 1.58 had the best catalytic activity.The highest yield of MAA up to 61.2%was achieved with basically complete conversion of itaconic acid under the suitable reaction conditions of 1 equivalent of NaOH,2 MPa of N_(2),250℃,and 2 h.On this basis,a reaction network for the decarboxylation of itaconic acid to methacrylic acid catalyzed by hydroxyapatite was established.With the aid of catalyst characterization using X-ray powder diffraction,NH3/CO2 temperature-programmed desorption,N_(2)physisorption,inductively coupled plasma optical emission spectrometry,and scanning electron microscopy,we found that the distribution of surface acid sites and basic sites,crystal growth orientation,texture properties and morphology of hydroxyapatite varied with the Ca/P molar ratio.Furthermore,the change of the crystal growth orientation and its influence on the surface acidity and alkalinity were clarified.
