A nitrogen-doped carbon microsphere sorbent with a hierarchical porous structure was synthesized via aggregation-hydrothermal carbonization.The Hg^(0)adsorption performance of the nitrogen-doped carbon microsphere sor...A nitrogen-doped carbon microsphere sorbent with a hierarchical porous structure was synthesized via aggregation-hydrothermal carbonization.The Hg^(0)adsorption performance of the nitrogen-doped carbon microsphere sorbent was tested and compared with that of the coconut shell activated carbon prepared in the laboratory.The effect of H_(2)S on Hg^(0)adsorption was also investigated.The nitrogen-doped carbon microsphere sorbent exhibited superior mercury removal performance compared with that of coconut shell activated carbon.In the absence of H_(2)S at a low temperature(≤100℃),the Hg^(0)removal efficiency of the nitrogen-doped carbon microsphere sorbent exceeded 90%.This value is significantly higher than that of coconut shell activated carbon,which is approximately 45%.H_(2)S significantly enhanced the Hg^(0)removal performance of the nitrogen-doped carbon microsphere sorbent at higher temperatures(100–180℃).The hierarchical porous structure facilitated the diffusion and adsorption of H_(2)S and Hg^(0),while the nitrogen-containing active sites significantly improved the adsorption and dissociation capabilities of H_(2)S,contributing to the generation of more active sulfur species on the surface of the nitrogen-doped carbon microsphere sorbent.The formation of active sulfur species and HgS on the sorbent surface was further confirmed using X-ray photoelectron spectroscopy and Hg^(0)temperature-programmed desorption tests.Density functional theory was employed to elucidate the adsorption and transformation of Hg^(0)on the sorbent surface.H_(2)S adsorbed and dissociated on the sorbent surface,generating active sulfur species that reacted with gaseous Hg^(0)to form HgS.展开更多
A process capable of simultaneously oxidizing NO, SO2, and Hg^0 was proposed, using a nigh-voltage and short-duration positive pulsed corona discharge. By focusing on NO, SO2, and Hg^0 oxidation efficiencies, the infl...A process capable of simultaneously oxidizing NO, SO2, and Hg^0 was proposed, using a nigh-voltage and short-duration positive pulsed corona discharge. By focusing on NO, SO2, and Hg^0 oxidation efficiencies, the influences of pulse peak voltage, pulse frequency, initial concentration, electrode number, residence time and water vapor addition were investigated. The results indicate that NO, SO2 and Hg^0 oxidation efficiencies depend primarily on the radicals （OH, HO2, O） and the active species （O3, H2O2, etc.） produced by the pulsed corona discharge. The NO, SO2 and Hg^0 oxidation efficiencies could be improved as pulse peak voltage, pulse frequency, electrode number and residence time increased, but they were reduced with increasing initial concentrations. By adding water vapor, the SO2 oxidation efficiency was improved remarkably, while the NO oxidation efficiency decreased slightly. In our experiments, the simultaneous NO, SO2, and Hg^0 oxidation efficiencies reached to 40%, 98%, and 55% with the initial concentrations 479 mg/m^3, 1040 mg/m^3, and 15.0 μg/m^3, respectively.展开更多
This study demonstrated the impacts of the synthesis methods on the textural structures,chemical properties,and Hg^(0)capture capability of the MnO_(x)system.Compared with the samples synthesized using the precipitati...This study demonstrated the impacts of the synthesis methods on the textural structures,chemical properties,and Hg^(0)capture capability of the MnO_(x)system.Compared with the samples synthesized using the precipitation(PR)and hydrothermal(HT)methods,the adsorbent prepared via the sol-gel(SG)technique gave the best performance.At 150℃,ca.90%Hg^(0)removal efficiency was reached after 7.5 h for MnO_(x)prepared by the SG method,ca.40%higher than that of the other two methods.The specific surface area of the adsorbent synthesized via the SG technique(23 m^(2)/g)was almost double that of the adsorbent prepared by the HT method(12 m^(2)/g)and three times that of the one prepared by the PR method(7 m^(2)/g).The presence of plentiful acid sites from the SG method facilitated the physisorption of Hg^(0),making more Hg^(0)available to be oxidized to HgO by the redox sites and thus giving the adsorbent prepared by the SG method the highest Hg^(0)removal efficiency.The strong oxidative ability accelerated the oxidation of the physically adsorbed Hg^(0)to HgO,which explained the higher Hg^(0)removal efficiency of the sample prepared using the HT method than that of the one synthesized by the PR technique.During the whole Hg^(0)removal cycles,chemisorption dominated,with the initial adsorption stage and the external mass-transfer process playing important roles.展开更多
This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simu...This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simulated flue gas at 140 ℃. These surface acid oxygen function groups were identified by Boehm titration, Fourier transformation infrared spectrum, temperature programmed desorption and X-ray photoelectron spectroscopy. It indicates that the carboxyl, lactone and phenolic were formed when the benzoic acid is loaded on the surface of activated carbons. Among the surface acid oxygen function groups, the carboxyl groups enhance the adsorption capacities of Hg^0 for activated carbons to a greater extent.展开更多
基金supported by National Natural Science Foundation of China(Grant Nos.51976108 and U1906232)Shihezi University Self Funded Support Project(ZZZC2023069).
文摘A nitrogen-doped carbon microsphere sorbent with a hierarchical porous structure was synthesized via aggregation-hydrothermal carbonization.The Hg^(0)adsorption performance of the nitrogen-doped carbon microsphere sorbent was tested and compared with that of the coconut shell activated carbon prepared in the laboratory.The effect of H_(2)S on Hg^(0)adsorption was also investigated.The nitrogen-doped carbon microsphere sorbent exhibited superior mercury removal performance compared with that of coconut shell activated carbon.In the absence of H_(2)S at a low temperature(≤100℃),the Hg^(0)removal efficiency of the nitrogen-doped carbon microsphere sorbent exceeded 90%.This value is significantly higher than that of coconut shell activated carbon,which is approximately 45%.H_(2)S significantly enhanced the Hg^(0)removal performance of the nitrogen-doped carbon microsphere sorbent at higher temperatures(100–180℃).The hierarchical porous structure facilitated the diffusion and adsorption of H_(2)S and Hg^(0),while the nitrogen-containing active sites significantly improved the adsorption and dissociation capabilities of H_(2)S,contributing to the generation of more active sulfur species on the surface of the nitrogen-doped carbon microsphere sorbent.The formation of active sulfur species and HgS on the sorbent surface was further confirmed using X-ray photoelectron spectroscopy and Hg^(0)temperature-programmed desorption tests.Density functional theory was employed to elucidate the adsorption and transformation of Hg^(0)on the sorbent surface.H_(2)S adsorbed and dissociated on the sorbent surface,generating active sulfur species that reacted with gaseous Hg^(0)to form HgS.
基金supported by the Science and Technology Research of Department of Education of China (No. 0305,03087)
文摘A process capable of simultaneously oxidizing NO, SO2, and Hg^0 was proposed, using a nigh-voltage and short-duration positive pulsed corona discharge. By focusing on NO, SO2, and Hg^0 oxidation efficiencies, the influences of pulse peak voltage, pulse frequency, initial concentration, electrode number, residence time and water vapor addition were investigated. The results indicate that NO, SO2 and Hg^0 oxidation efficiencies depend primarily on the radicals （OH, HO2, O） and the active species （O3, H2O2, etc.） produced by the pulsed corona discharge. The NO, SO2 and Hg^0 oxidation efficiencies could be improved as pulse peak voltage, pulse frequency, electrode number and residence time increased, but they were reduced with increasing initial concentrations. By adding water vapor, the SO2 oxidation efficiency was improved remarkably, while the NO oxidation efficiency decreased slightly. In our experiments, the simultaneous NO, SO2, and Hg^0 oxidation efficiencies reached to 40%, 98%, and 55% with the initial concentrations 479 mg/m^3, 1040 mg/m^3, and 15.0 μg/m^3, respectively.
基金This work is supported by the Fundamental Research Funds of China Jiliang University and the Zhejiang Provincial Natural Science Foundation of China(No.LQ22E060003).
文摘This study demonstrated the impacts of the synthesis methods on the textural structures,chemical properties,and Hg^(0)capture capability of the MnO_(x)system.Compared with the samples synthesized using the precipitation(PR)and hydrothermal(HT)methods,the adsorbent prepared via the sol-gel(SG)technique gave the best performance.At 150℃,ca.90%Hg^(0)removal efficiency was reached after 7.5 h for MnO_(x)prepared by the SG method,ca.40%higher than that of the other two methods.The specific surface area of the adsorbent synthesized via the SG technique(23 m^(2)/g)was almost double that of the adsorbent prepared by the HT method(12 m^(2)/g)and three times that of the one prepared by the PR method(7 m^(2)/g).The presence of plentiful acid sites from the SG method facilitated the physisorption of Hg^(0),making more Hg^(0)available to be oxidized to HgO by the redox sites and thus giving the adsorbent prepared by the SG method the highest Hg^(0)removal efficiency.The strong oxidative ability accelerated the oxidation of the physically adsorbed Hg^(0)to HgO,which explained the higher Hg^(0)removal efficiency of the sample prepared using the HT method than that of the one synthesized by the PR technique.During the whole Hg^(0)removal cycles,chemisorption dominated,with the initial adsorption stage and the external mass-transfer process playing important roles.
文摘This article discussed the benzoic acid activated carbons which have changed the types and content of acid oxygen-function groups on the surface of activated carbons and their effect on the adsorption for Hg^0 in simulated flue gas at 140 ℃. These surface acid oxygen function groups were identified by Boehm titration, Fourier transformation infrared spectrum, temperature programmed desorption and X-ray photoelectron spectroscopy. It indicates that the carboxyl, lactone and phenolic were formed when the benzoic acid is loaded on the surface of activated carbons. Among the surface acid oxygen function groups, the carboxyl groups enhance the adsorption capacities of Hg^0 for activated carbons to a greater extent.
