Hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites were selected for elemental mercury(Hg^0) removal from non-ferrous metal smelting flue gas in this study. Results showed that the hierarchical Ag-SiO_2@Fe_3O_4 magneti...Hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites were selected for elemental mercury(Hg^0) removal from non-ferrous metal smelting flue gas in this study. Results showed that the hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites had favorable Hg^0 removal ability at low temperature. Moreover, the adsorption capacity of hierarchical magnetic composite is much larger than that of pure Fe_3O_4 and SiO_2@Fe_3O_4. The Hg^0 removal efficiency reached the highest value as approximately 92% under the reaction temperature of 150°C, while the removal efficiency sharply reduced in the absence of O_2. The characterization results indicated that Ag nanoparticles grew on the surface of SiO_2@Fe_3O_4 support. The large surface area of SiO_2 supplied efficient reaction room for Hg and Ag atoms. Ag–Hg amalgam is generated on the surface of the composites. In addition, this magnetic material could be easily separated from fly ashes when adopted for treating real flue gas, and the spent materials could be regenerated using a simple thermal-desorption method.展开更多
Air pollutant emissions represent a critical challenge in the green development of the non-ferrous metallurgy industry.This work studied the emission characteristics,formation mechanisms,phase transformation and separ...Air pollutant emissions represent a critical challenge in the green development of the non-ferrous metallurgy industry.This work studied the emission characteristics,formation mechanisms,phase transformation and separation of typical air pollutants,such as heavy metal particles,mercury,sulfur oxides and fluoride,during non-ferrous smelting.A series of purification technologies,including optimization of the furnace throat and hightemperature discharge,were developed to collaboratively control and recover fine particles from the flue gas of heavy metal smelting processes,including copper,lead and zinc.Significant improvements have been realized in wet scrubbing technology for removing mercury,fluoride and SO_(2)from flue gas.Gas-liquid sulfidation technology by applying H_(2)S was invented to recycle the acid scrubbing wastewater more efficiently and in an eco-friendly manner.Based on digital technology,a source reduction method was designed for sulfur and fluoride control during the whole aluminum electrolysis process.New desulfurization technologies were developed for catalytic reduction of the sulfur content in petroleum coke at low temperature and catalytic reduction of SO_(2)to elemental sulfur.This work has established the technology for coupling multi-pollutant control and resource recovery from the flue gas from non-ferrous metallurgy,which provides the scientific theoretical basis and application technology for the treatment of air pollutants in the non-ferrous metallurgy industry.展开更多
Oxidation of sulfite and competitive absorption existed in Na_(2)SO_(3) solution for simultaneous removal of NO_(x) and SO_(2),inhibited the long-term high-efficiency when used for practical applications.A matching st...Oxidation of sulfite and competitive absorption existed in Na_(2)SO_(3) solution for simultaneous removal of NO_(x) and SO_(2),inhibited the long-term high-efficiency when used for practical applications.A matching strategy was developed to solve these problems.Antioxidants combination was used to retard the oxidation of antioxidant and enhance inhibition of S(IV)(tetravalent sulfur)oxidation.Hydroquinone(HQ)and sodium thiosulfate(ST)showed a positive synergistic effect on inhibition of S(IV)oxidation.When SO_(2) concentration was 500 and 2000 ppmV,the addition of 0.1 wt.%HQ and 1 wt.%ST decreased the percentage of S(IV)oxidized by oxygen by over 30%and 40%,respectively.Alkali(Na_(2)CO_(3))alleviated the competitive absorption between NO_(x) and SO_(2).Moreover,Na_(2)CO_(3) exhibited an enhancement effect on the absorption of NO_(x) and SO_(2) when coupled with anti-oxidants.While the increase of oxygen pressure accelerated the oxidation of S(IV),the anti-oxidants can retard the oxidation.The measurement of pH suggested the removal efficiency of NO_(x) highly depended on SO_(3)^(2-) concentration rather than pH.The further investigation of the mechanism suggested the match effect was related to the interaction between ST and the intermediate product of HQ.The match strategy holds a potential for application of SO_(3)^(2-) to denitration.展开更多
Elemental mercury (Hg^0) in flue gases can be efficiently captured by mercury chloride (HgCl2) solution. However, the absorption behaviors and the influencing effects are still poorly understood. The mechanism of ...Elemental mercury (Hg^0) in flue gases can be efficiently captured by mercury chloride (HgCl2) solution. However, the absorption behaviors and the influencing effects are still poorly understood. The mechanism of Hg^0 absorption by HgCl2 and the factors that control the removal were studied in this paper. It was found that when the mole ratio of Cl^- to HgCl2 is 10:1, the Hg^0 removal efficiency is the highest. Among the main mercury chloride species, HgCl3^- is the most efficient ion for Hg^0 removal in the HgCl2 absorption system when moderate concentrations of chloride ions exist. The Hg^0 absorption reactions in the aqueous phase were investigated computationaIIy using Moller-Plesset perturbation theory. The calculated Gibbs free energies and energy barriers are in excellent agreement with the results obtained from experiments. In the presence of SO3^2- and SO2, Hg^2+ reduction occurred and Hg^0 removal efficiency decreased. The reduced Hg^0 removal can be controlled through increased chloride concentration to some degree. Low pH value in HgCla solution enhanced the Hg^0 removal efficiency, and the effect was more significant in dilute HgCl2 solutions. The presence of SO4^2- and NO3^- did not affect Hg^0 removal by HgCl2.展开更多
基金supported by the National Key R&D Program of China (No. 2017YFC0210500)the National Natural Science Foundation of China (No. 51508525)the Key Research and Development Program of Ningxia Hui Autonomous Region (No. 2016KJHM31)
文摘Hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites were selected for elemental mercury(Hg^0) removal from non-ferrous metal smelting flue gas in this study. Results showed that the hierarchical Ag-SiO_2@Fe_3O_4 magnetic composites had favorable Hg^0 removal ability at low temperature. Moreover, the adsorption capacity of hierarchical magnetic composite is much larger than that of pure Fe_3O_4 and SiO_2@Fe_3O_4. The Hg^0 removal efficiency reached the highest value as approximately 92% under the reaction temperature of 150°C, while the removal efficiency sharply reduced in the absence of O_2. The characterization results indicated that Ag nanoparticles grew on the surface of SiO_2@Fe_3O_4 support. The large surface area of SiO_2 supplied efficient reaction room for Hg and Ag atoms. Ag–Hg amalgam is generated on the surface of the composites. In addition, this magnetic material could be easily separated from fly ashes when adopted for treating real flue gas, and the spent materials could be regenerated using a simple thermal-desorption method.
基金supported by the National Natural Science Foundation of China(No.52234011)the National Key R&D Program of China(No.2017YFC0210400)。
文摘Air pollutant emissions represent a critical challenge in the green development of the non-ferrous metallurgy industry.This work studied the emission characteristics,formation mechanisms,phase transformation and separation of typical air pollutants,such as heavy metal particles,mercury,sulfur oxides and fluoride,during non-ferrous smelting.A series of purification technologies,including optimization of the furnace throat and hightemperature discharge,were developed to collaboratively control and recover fine particles from the flue gas of heavy metal smelting processes,including copper,lead and zinc.Significant improvements have been realized in wet scrubbing technology for removing mercury,fluoride and SO_(2)from flue gas.Gas-liquid sulfidation technology by applying H_(2)S was invented to recycle the acid scrubbing wastewater more efficiently and in an eco-friendly manner.Based on digital technology,a source reduction method was designed for sulfur and fluoride control during the whole aluminum electrolysis process.New desulfurization technologies were developed for catalytic reduction of the sulfur content in petroleum coke at low temperature and catalytic reduction of SO_(2)to elemental sulfur.This work has established the technology for coupling multi-pollutant control and resource recovery from the flue gas from non-ferrous metallurgy,which provides the scientific theoretical basis and application technology for the treatment of air pollutants in the non-ferrous metallurgy industry.
基金financially supported by the National Key R and D Program of China(No.2018YFC0213400)the National Natural Science Foundation of China(No.21976118)supported by the Startup Fund for Youngman Research at SJTU(No.19X100040083)。
文摘Oxidation of sulfite and competitive absorption existed in Na_(2)SO_(3) solution for simultaneous removal of NO_(x) and SO_(2),inhibited the long-term high-efficiency when used for practical applications.A matching strategy was developed to solve these problems.Antioxidants combination was used to retard the oxidation of antioxidant and enhance inhibition of S(IV)(tetravalent sulfur)oxidation.Hydroquinone(HQ)and sodium thiosulfate(ST)showed a positive synergistic effect on inhibition of S(IV)oxidation.When SO_(2) concentration was 500 and 2000 ppmV,the addition of 0.1 wt.%HQ and 1 wt.%ST decreased the percentage of S(IV)oxidized by oxygen by over 30%and 40%,respectively.Alkali(Na_(2)CO_(3))alleviated the competitive absorption between NO_(x) and SO_(2).Moreover,Na_(2)CO_(3) exhibited an enhancement effect on the absorption of NO_(x) and SO_(2) when coupled with anti-oxidants.While the increase of oxygen pressure accelerated the oxidation of S(IV),the anti-oxidants can retard the oxidation.The measurement of pH suggested the removal efficiency of NO_(x) highly depended on SO_(3)^(2-) concentration rather than pH.The further investigation of the mechanism suggested the match effect was related to the interaction between ST and the intermediate product of HQ.The match strategy holds a potential for application of SO_(3)^(2-) to denitration.
基金supported by the Major State Basic Research Development Program (No. 2013CB430005)the National Natural Science Foundation of China (No. 51278294)the National High Technology Research and Development Program (No. 2012AA062504)
文摘Elemental mercury (Hg^0) in flue gases can be efficiently captured by mercury chloride (HgCl2) solution. However, the absorption behaviors and the influencing effects are still poorly understood. The mechanism of Hg^0 absorption by HgCl2 and the factors that control the removal were studied in this paper. It was found that when the mole ratio of Cl^- to HgCl2 is 10:1, the Hg^0 removal efficiency is the highest. Among the main mercury chloride species, HgCl3^- is the most efficient ion for Hg^0 removal in the HgCl2 absorption system when moderate concentrations of chloride ions exist. The Hg^0 absorption reactions in the aqueous phase were investigated computationaIIy using Moller-Plesset perturbation theory. The calculated Gibbs free energies and energy barriers are in excellent agreement with the results obtained from experiments. In the presence of SO3^2- and SO2, Hg^2+ reduction occurred and Hg^0 removal efficiency decreased. The reduced Hg^0 removal can be controlled through increased chloride concentration to some degree. Low pH value in HgCla solution enhanced the Hg^0 removal efficiency, and the effect was more significant in dilute HgCl2 solutions. The presence of SO4^2- and NO3^- did not affect Hg^0 removal by HgCl2.