This work reports an improved method for the wet desulfurization of high-sulfur petroleum coke(petcoke)powder based on the combination of pre-calcination,H_(2)O_(2),and ultrasound.The results demonstrated that over 45...This work reports an improved method for the wet desulfurization of high-sulfur petroleum coke(petcoke)powder based on the combination of pre-calcination,H_(2)O_(2),and ultrasound.The results demonstrated that over 45%of the sulfur atoms were efficiently removed from Tianjin coke and Qilu coke(particle size<0.1 mm)by pre-calcination at 800℃ for 6 h followed by desulfurization with HNO3(8 mol/L)and H_(2)O_(2)(2 mol/L)solution at a reaction temperature of 60℃,a reaction time of 6 h,a liquid-to-solid ratio of 10 mL/g,and a 40 kHz ultrasonic power of 400 W.In addition,the specific surface area of the petcoke particles increased from 0.7 to 301.49 m^(2)/g.After desulfurization,the pore size distribution of the petcoke particles was more concentrated on micropores compared with the samples prior to petcoke treatment.Reactive force field molecular dynamics simulation results indicated that HNO_(3) continuously oxidized the carbon atoms adjacent to sulfur atoms in the petcoke macromolecules and promoted sulfur removal from petcoke via the cleavage of C-S bonds.The sulfur transformation mechanism can be summarized as follows:thiophene sulfur→branched chain carbon sulfur→CO_(2)S→C_(2)O_(2)S→C_(2)O_(3)NS→C_(2)O_(4)S→CO_(2)S.展开更多
基金This work was financially supported by the Scientific Research Project of Hunan Education Department(20C0410)the Fundamental Research Funds for the Central Universities of Central South University.
文摘This work reports an improved method for the wet desulfurization of high-sulfur petroleum coke(petcoke)powder based on the combination of pre-calcination,H_(2)O_(2),and ultrasound.The results demonstrated that over 45%of the sulfur atoms were efficiently removed from Tianjin coke and Qilu coke(particle size<0.1 mm)by pre-calcination at 800℃ for 6 h followed by desulfurization with HNO3(8 mol/L)and H_(2)O_(2)(2 mol/L)solution at a reaction temperature of 60℃,a reaction time of 6 h,a liquid-to-solid ratio of 10 mL/g,and a 40 kHz ultrasonic power of 400 W.In addition,the specific surface area of the petcoke particles increased from 0.7 to 301.49 m^(2)/g.After desulfurization,the pore size distribution of the petcoke particles was more concentrated on micropores compared with the samples prior to petcoke treatment.Reactive force field molecular dynamics simulation results indicated that HNO_(3) continuously oxidized the carbon atoms adjacent to sulfur atoms in the petcoke macromolecules and promoted sulfur removal from petcoke via the cleavage of C-S bonds.The sulfur transformation mechanism can be summarized as follows:thiophene sulfur→branched chain carbon sulfur→CO_(2)S→C_(2)O_(2)S→C_(2)O_(3)NS→C_(2)O_(4)S→CO_(2)S.
