The acidity and acid distribution of hierarchical porous ZSM-5 were tailored via phosphate modification. The catalytic results showed that both benzene conversion and selectivity of toluene and xylene increased with t...The acidity and acid distribution of hierarchical porous ZSM-5 were tailored via phosphate modification. The catalytic results showed that both benzene conversion and selectivity of toluene and xylene increased with the presence of appropriate amount of phosphorus. Meanwhile, side reactions such as methanol to olefins related with the formation of by-product ethylbenzene formation and isomerization of xylene to meta-xylene were suppressed efficiently. The acid strength and sites amount of Br?nsted acid of the catalyst were crucial for improving benzene conversion and yield of xylene, whereas passivation of external surface acid sites played an important role in breaking thermodynamic equilibrium distribution of xylene isomers.展开更多
Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM,...Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM, XPS and TG techniques. We set the products selectivity as a function of butane conversion over various phosphate loading, and it is found that the PoCNT catalyst with the 0.8% phosphate weight loading(0.8PoCNT) exhibits the best catalytic performance. When the phosphate loading is higher than 0.8 wt%, the difference of catalytic activity among the PoCNT catalysts is neglectable. Consequently, the ODH of n-butane over the 0.8PoCNT catalyst is particularly discussed via changing the reaction conditions including reaction temperatures, residence time and n-butane/O;ratios. The interacting mechanism of phosphate with the oxygen functional groups on the CNT surface is also proposed.展开更多
Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) ...Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) is one of the most critical steps in the whole process.Herein,we regulated the different adsorption intensity of oxygen on the surface by designing phosphate (PO_(4)^(3-)) modified titanium oxide(TiO_(2)).The results show that the adsorption of oxygen on the photocatalyst surface is gradually enhanced,which effectively improves the dissolution rate of precious metals.PO_(4)^(3-)modification increased the photocatalytic dissolution rate of gold (Au) by 2.8 times.The photocatalytic activity of other precious metals dissolution (such as palladium (Pd),platinum (Pt),rhodium (Rh),ruthenium (Ru) and iridium (Ir)) was also significantly improved.It is applied to the recovery of precious metals from spent catalysts and electronic devices to significantly promote the recovery efficiency.This indicates the direction for designing more efficient photocatalysts for precious metal recovery.展开更多
This study was performed to investigate the removal of phosphate from domestic wastewater using a modified steel slag as the adsorbent. The adsorption effects of alkalinity, salt, water,and thermal modification were i...This study was performed to investigate the removal of phosphate from domestic wastewater using a modified steel slag as the adsorbent. The adsorption effects of alkalinity, salt, water,and thermal modification were investigated. The results showed that thermal activation at 800℃ for 1 hr was the optimum operation to improve the adsorption capacity. The adsorption process of the thermally modified slag was well described by the Elovich kinetic model and the Langmuir isotherm model. The maximum adsorption capacity calculated from the Langmuir model reached 13.62 mg/g. Scanning electron microscopy indicated that the surface of the modified slag was cracked and that the texture became loose after heating. The surface area and pore volume did not change after thermal modification. In the treatment of domestic wastewater, the modified slag bed(35.5 kg) removed phosphate effectively and operated for 158 days until the effluent P rose above the limit concentration of 0.5 mg/L. The phosphate fractionation method, which is often applied in soil research, was used to analyze the phosphate adsorption behavior in the slag bed. The analysis revealed that the total contents of various Ca-P forms accounted for 81.4%-91.1%, i.e., Ca10-P 50.6%-65.1%, Ca8-P 17.8%-25.0%,and Ca2-P 4.66%-9.20%. The forms of Al-P, Fe-P, and O-P accounted for only 8.9%-18.6%. The formation of Ca10-P precipitates was considered to be the main mechanism of phosphate removal in the thermally modified slag bed.展开更多
基金Supported by the National Natural Science Foundation of China(21476207,21506189)Zhejiang Postdoctoral Research Funded Projects(BSH1502147)
文摘The acidity and acid distribution of hierarchical porous ZSM-5 were tailored via phosphate modification. The catalytic results showed that both benzene conversion and selectivity of toluene and xylene increased with the presence of appropriate amount of phosphorus. Meanwhile, side reactions such as methanol to olefins related with the formation of by-product ethylbenzene formation and isomerization of xylene to meta-xylene were suppressed efficiently. The acid strength and sites amount of Br?nsted acid of the catalyst were crucial for improving benzene conversion and yield of xylene, whereas passivation of external surface acid sites played an important role in breaking thermodynamic equilibrium distribution of xylene isomers.
基金supported by the National Natural Science Foundation of China(No.91545110,21573254,21203214,21133010,21473223,21261160487,51221264)the Institute of Metal Research,Youth Innovation Promotion Association(CAS)the Sinopec China and the Strategic Priority Research Program of the Chinese Academy of Sciences,Grant No.XDA09030103
文摘Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM, XPS and TG techniques. We set the products selectivity as a function of butane conversion over various phosphate loading, and it is found that the PoCNT catalyst with the 0.8% phosphate weight loading(0.8PoCNT) exhibits the best catalytic performance. When the phosphate loading is higher than 0.8 wt%, the difference of catalytic activity among the PoCNT catalysts is neglectable. Consequently, the ODH of n-butane over the 0.8PoCNT catalyst is particularly discussed via changing the reaction conditions including reaction temperatures, residence time and n-butane/O;ratios. The interacting mechanism of phosphate with the oxygen functional groups on the CNT surface is also proposed.
基金supported by the National Key Research and Development Program of China (No. 2020YFA0211004)the National Natural Science Foundation of China (Nos. 22176128, 21876114)+4 种基金Sponsored by Program of Shanghai Government (Nos. 21XD1422800, 19DZ1205102, 19160712900)Chinese Education Ministry Key Laboratory and International Joint Laboratory on Resource Chemistry, and Shanghai Eastern Scholar Program“111 Innovation and Talent Recruitment Base on Photochemical and Energy Materials” (No. D18020)Shanghai Engineering Research Center of Green Energy Chemical Engineering (No. 18DZ2254200)Shanghai Frontiers Science Center of Biomimetic Catalysis。
文摘Photocatalytic recovery,a novel precious metal recycling technology,dedicates to solving the environmental and energy consumption problems caused by traditional technologies.The activation of molecular oxygen (O_(2)) is one of the most critical steps in the whole process.Herein,we regulated the different adsorption intensity of oxygen on the surface by designing phosphate (PO_(4)^(3-)) modified titanium oxide(TiO_(2)).The results show that the adsorption of oxygen on the photocatalyst surface is gradually enhanced,which effectively improves the dissolution rate of precious metals.PO_(4)^(3-)modification increased the photocatalytic dissolution rate of gold (Au) by 2.8 times.The photocatalytic activity of other precious metals dissolution (such as palladium (Pd),platinum (Pt),rhodium (Rh),ruthenium (Ru) and iridium (Ir)) was also significantly improved.It is applied to the recovery of precious metals from spent catalysts and electronic devices to significantly promote the recovery efficiency.This indicates the direction for designing more efficient photocatalysts for precious metal recovery.
基金supported by the Mega-projects of Science Research for Water Environment Improvement of China (Nos. 2013ZX07209-001-003, 2012ZX07307-001-006)
文摘This study was performed to investigate the removal of phosphate from domestic wastewater using a modified steel slag as the adsorbent. The adsorption effects of alkalinity, salt, water,and thermal modification were investigated. The results showed that thermal activation at 800℃ for 1 hr was the optimum operation to improve the adsorption capacity. The adsorption process of the thermally modified slag was well described by the Elovich kinetic model and the Langmuir isotherm model. The maximum adsorption capacity calculated from the Langmuir model reached 13.62 mg/g. Scanning electron microscopy indicated that the surface of the modified slag was cracked and that the texture became loose after heating. The surface area and pore volume did not change after thermal modification. In the treatment of domestic wastewater, the modified slag bed(35.5 kg) removed phosphate effectively and operated for 158 days until the effluent P rose above the limit concentration of 0.5 mg/L. The phosphate fractionation method, which is often applied in soil research, was used to analyze the phosphate adsorption behavior in the slag bed. The analysis revealed that the total contents of various Ca-P forms accounted for 81.4%-91.1%, i.e., Ca10-P 50.6%-65.1%, Ca8-P 17.8%-25.0%,and Ca2-P 4.66%-9.20%. The forms of Al-P, Fe-P, and O-P accounted for only 8.9%-18.6%. The formation of Ca10-P precipitates was considered to be the main mechanism of phosphate removal in the thermally modified slag bed.