Wet Flue Gas Desulfurization(WFGD)unit based upon spray scrubber has beenwidely employed to control SO_(2) emissions from flue gas in coal-fired power plant.To clarify the dependence of desulfurization performance on ...Wet Flue Gas Desulfurization(WFGD)unit based upon spray scrubber has beenwidely employed to control SO_(2) emissions from flue gas in coal-fired power plant.To clarify the dependence of desulfurization performance on inter-phase transfer behaviors with non-ideal contacting patterns of flue gas and slurry droplets,three regions in spray scrubber are distinguished in terms of gas-slurry flow structures using CFD method in the Eulerian-Lagrangian framework.A comprehensive model is established by involving the transfer process between two phases and chemical reactions in aqueous phase,which is validatedwith the measured data froma WFGD scrubber of 330 MW coal-fired power unit.Numerical results show that the overall uniformity degree of flue gas in whole scrubber is largely determined by the force-balanced droplets in the middle part of scrubber,which is dominated by counter-current mode.Both momentum transfer behavior and SO_(2) chemical absorption process present the synchronicity with the evolution of gas-slurry flow pattern,whilst the heat transfer together with H_(2)O evaporation has little effect on overall absorption process.Three regions are firstly defined as Gas Inlet Region(GIR),Dominant Absorption Region(DAR)and Slurry Dispersed Region(SDR)from the bottom to top of scrubber.SO_(2) is mainly scrubbed in DAR,which provides much more intensive interaction between two phases compared to GIR or SDR.A better understanding of the desulfurization process is obtained from the fundamental relationship between transport phenomena and chemical reactions based upon the complicated hydrodynamics of gas-slurry two-phase flow,which should be useful for designing and optimizing the scrubber in coal-fired power unit.展开更多
Fe-based ionic liquid (Fe-IL) was synthesized by mixing FeCl3·6H2O and 1-butyl-3-methylimidazolium chloride [Bmim]C1 in this paper. The phase diagram of a ternary Fe-IL, ethanol and water system was investigate...Fe-based ionic liquid (Fe-IL) was synthesized by mixing FeCl3·6H2O and 1-butyl-3-methylimidazolium chloride [Bmim]C1 in this paper. The phase diagram of a ternary Fe-IL, ethanol and water system was investigated to construct a ternary desulfurization solution for wet flue gas desulfurization. The effects of flow rate and concentration of SO2, reaction temperature, pH and Fe-IL fraction in aqueous desulfurization solution on the desulfiariza- tion efficiency were investigated. The results shows that the best composition of ternary desulfurization solution of Fe-IL, ethanol and water is 1 : 1.5 : 3 by volume ratio, and pH should be controlled at 2.0. Under such conditions, a desulfurization rate greater than 90% could be obtained. The product of sulfuric acid had inhibition effect on the wet desulfurization process. With applying this new ternary desulfurization solution, not only the catalyst Fe-IL can be recycled and reused, but also the product sulfuric acid can be separated directly from the ternary desulfurization system.展开更多
The absorbent composing of Bayer red mud and water was prepared and applied to removing SO2 from flue gas.Effects of the ratio of liquid to solid(L/S),the absorption temperature,the inlet SO2 concentration,the O2 conc...The absorbent composing of Bayer red mud and water was prepared and applied to removing SO2 from flue gas.Effects of the ratio of liquid to solid(L/S),the absorption temperature,the inlet SO2 concentration,the O2 concentration,SO4^2-and other different components of Bayer red mud on desulfurization were conducted.The mechanism of flue gas desulfurization was also established.The results indicated that L/S was the prominent factor,followed by the inlet SO2 concentration and the temperature was the least among them.The optimum condition was as follows:L/S,the temperature and the SO2 concentration were 20:1,25℃and 1000 mg/m^3,respectively,under the gas flow of 1.5 L/min.The desulfurization efficiency was not significantly influenced when O2 concentration was above 7%.The accumulation of SO4^2-inhibited the desulfurization efficiency.The alkali absorption and metal ions liquid catalytic oxidation were involved in the process,which accounted for 98.61%.展开更多
The relationship between the fine particles emitted after desulfurization and gypsum crystals in the desulfurization slurry was investigated,and the crystallization characteristics varying with the operation parameter...The relationship between the fine particles emitted after desulfurization and gypsum crystals in the desulfurization slurry was investigated,and the crystallization characteristics varying with the operation parameters and compositions of the desulfurization slurry were discussed.The results showed that the fine particles generated during the desulfurization process were closely related to the crystal characteristics in the desulfurization slurry by comparison of their morphology and elements. With the higher proportion of fine crystals in the desulfurization slurry,the number concentration of fine particles after desulfurization was increased and their particle sizes were smaller,indicating that the optimization of gypsum crystallization was beneficial for the reduction of the fine particle emission. The lower p H value and an optimal temperature of the desulfurization slurry were beneficial to restrain the generation of fine crystals in the desulfurization slurry. In addition,the higher concentrations of the Fe3+ions and the F- ions in the desulfurization slurry both promoted the generation of fine crystals with corresponding change of the morphology and the effect of the Fe3+ ions was more obvious.With the application of the desulfurization synergist additive,it was beneficial for the inhibition of fine crystals while the thinner crystals were generated.展开更多
In order to improve the slurry pH control accuracy of the absorption tower in the wet flue gas desulfurization process,a model free adaptive predictive control algorithm for the desulfurization slurry pH which is base...In order to improve the slurry pH control accuracy of the absorption tower in the wet flue gas desulfurization process,a model free adaptive predictive control algorithm for the desulfurization slurry pH which is based on a cyber physical systems framework is proposed.First,aiming to address system characteristics of non-linearity and pure hysteresis in slurry pH change process,a model free adaptive predictive control algorithm based on compact form dynamic linearization is proposed by combining model free adaptive control algorithm with model predictive control algorithm.Then,by integrating information resources with the physical resources in the absorption tower slurry pH control process,an absorption tower slurry pH optimization control system based on cyber physical systems is constructed.It is turned out that the model free adaptive predictive control algorithm under the framework of the cyber physical systems can effectively realize the high-precision tracking control of the slurry pH of the absorption tower,and it has strong robustness.展开更多
In this study, the characteristics of fine particles before and after wet flue gas desulfurization(WFGD) in three coal-fired heating boilers in northern China were investigated by using a dilution-based emission sampl...In this study, the characteristics of fine particles before and after wet flue gas desulfurization(WFGD) in three coal-fired heating boilers in northern China were investigated by using a dilution-based emission sampling experimental system. The influences of the WFGD process on the mass and number concentrations as well as the chemical composition of fine particles were analyzed. The removal efficiency of desulfurization processes on particulate matter mass was 30.06%–56.25% for the three study units. The WFGD had a great influence on the size distributions of particle mass concentration and number concentration. A significant increase in the number and mass concentration of particles in the size range of 0.094–0.946 μm was observed. The watersoluble ion content accounted for a very large proportion of PM_(2.5) mass, and its proportion in PM_(2.5) increased from 28.39%–41.08% to 48.96%–61.21% after the WFGD process for the three units. The desulfurizing process also drastically increased the proportion of cation component(Ca^(2+) for unit A, Mg^(2+) for unit B, and Na+for unit C) and the proportion of SO_4^(2-) in PM_(2.5), and it increased the CE/AE values of PM_(2.5) from 0.82–0.98 to 0.93–1.27 for the three study units.展开更多
Selective catalytic reduction(SCR) denitration may increase the emission of NH4+and NH3.The removal and transformation characteristics of ammonium sulfate aerosols and ammonia slip during the wet flue gas desulfurizat...Selective catalytic reduction(SCR) denitration may increase the emission of NH4+and NH3.The removal and transformation characteristics of ammonium sulfate aerosols and ammonia slip during the wet flue gas desulfurization(WFGD) process, as well as the effect of desulfurization parameters, were investigated in an experimental system equipped with a simulated SCR flue gas generation system and a limestone-based WFGD system.The results indicate that the ammonium sulfate aerosols and ammonia slip in the flue gas from SCR can be partly removed by slurry scrubbing, while the entrainment and evaporation of desulfurization slurry with accumulated NH4+will generate new ammoniumcontaining particles and gaseous ammonia.The ammonium-containing particles formed by desulfurization are not only derived from the entrainment of slurry droplets, but also from the re-condensation of gaseous ammonia generated by slurry evaporation.Therefore,even if the concentration of NH4+in the desulfurization slurry is quite low, a high level of NH4+was still contained in the fine particles at the outlet of the scrubber.When the accumulated NH4+in the desulfurization slurry was high enough, the WFGD system promoted the conversion of NH3 to NH4+and increased the additional emission of primary NH4+aerosols.With the decline of the liquid/gas ratio and flue gas temperature, the removal efficiency of ammonia sulfate aerosols increased, and the NH4+emitted from entrainment and evaporation of the desulfurization slurry decreased.In addition, the volatile ammonia concentration after the WFGD system was reduced with the decrease of the NH4+concentration and p H values of the slurry.展开更多
脱硫过程是具有高度动态非线性和较大延迟时间的复杂工业过程,为了解决烟气脱硫过程的建模问题,设计了注意力机制下的深度长短期记忆(attention mechanism-based long short-term memory,AttLSTM)网络,并基于该网络设计自动编码器,完成...脱硫过程是具有高度动态非线性和较大延迟时间的复杂工业过程,为了解决烟气脱硫过程的建模问题,设计了注意力机制下的深度长短期记忆(attention mechanism-based long short-term memory,AttLSTM)网络,并基于该网络设计自动编码器,完成脱硫过程异常点的检测。该文首次提出使用AttLSTM网络自编码器对脱硫过程进行离群点检测,并且该网络模型同样首次应用于脱硫过程的辨识任务中。从更深的意义上讲,该文尝试使用深度学习模型对复杂系统进行辨识,所建立的AttLSTM网络之前未出现在系统辨识领域,该网络的出现可以丰富辨识模型的选择,同时为人工智能技术在系统辨识领域和控制领域的应用与推广提供参考。实验结果表明,相比于之前文献出现的脱硫过程建模方法,所提方法在不同性能指标上均具有更好的表现,由此可以证明深度AttLSTM网络在脱硫场景下的有效性。展开更多
The low-temperature wet oxidation behavior of semi-dry desulfurization ash from iron ore sintering flue gas in ammonium citrate solution was investigated for efficiently utilizing the low-quality desulfurization ash. ...The low-temperature wet oxidation behavior of semi-dry desulfurization ash from iron ore sintering flue gas in ammonium citrate solution was investigated for efficiently utilizing the low-quality desulfurization ash. The effects of the ammonium citrate concentration, oxidation temperature, solid/liquid ratio, and oxidation time on the wet oxidation behavior of desulfurization ash were studied. Simultaneously, the oxidation mechanism of desulfurization ash was revealed by means of X-ray diffraction, Zeta electric resistance, and X-ray photoelectron spectroscopy (XPS) analysis. Under the optimal conditions with ammonium citrate, the oxidation ratio of CaSO_(3) was up to the maximum value (98.49%), while that of CaSO_(3) was only 8.92% without ammonium citrate. Zeta electric resistance and XPS results indicate that the dissolution process of CaSO_(3) could be significantly promoted by complexation derived from the ammonium citrate hydrolysis. As a result, the oxidation process of CaSO_(3) was transformed from particle oxidation to SO_(3)^(2−) ion oxidation, realizing the rapid transformation of desulfurization ash from CaSO_(3) to CaSO_(4) at low temperature. It provides a reference for the application of semi-dry desulfurization ash and contributes to sustainable management for semi-dry desulfurization ash.展开更多
基金This work was supported by the National Natural Science Foundation of China(51706070 and U1910215)the Fundamental Research Funds for the Central Universities(2018ZD03,2020MS008 and 2020MS078).
文摘Wet Flue Gas Desulfurization(WFGD)unit based upon spray scrubber has beenwidely employed to control SO_(2) emissions from flue gas in coal-fired power plant.To clarify the dependence of desulfurization performance on inter-phase transfer behaviors with non-ideal contacting patterns of flue gas and slurry droplets,three regions in spray scrubber are distinguished in terms of gas-slurry flow structures using CFD method in the Eulerian-Lagrangian framework.A comprehensive model is established by involving the transfer process between two phases and chemical reactions in aqueous phase,which is validatedwith the measured data froma WFGD scrubber of 330 MW coal-fired power unit.Numerical results show that the overall uniformity degree of flue gas in whole scrubber is largely determined by the force-balanced droplets in the middle part of scrubber,which is dominated by counter-current mode.Both momentum transfer behavior and SO_(2) chemical absorption process present the synchronicity with the evolution of gas-slurry flow pattern,whilst the heat transfer together with H_(2)O evaporation has little effect on overall absorption process.Three regions are firstly defined as Gas Inlet Region(GIR),Dominant Absorption Region(DAR)and Slurry Dispersed Region(SDR)from the bottom to top of scrubber.SO_(2) is mainly scrubbed in DAR,which provides much more intensive interaction between two phases compared to GIR or SDR.A better understanding of the desulfurization process is obtained from the fundamental relationship between transport phenomena and chemical reactions based upon the complicated hydrodynamics of gas-slurry two-phase flow,which should be useful for designing and optimizing the scrubber in coal-fired power unit.
基金Supported by the National Natural Science Foundation of China (21076019,90610007)the National High Technology Research and Development Program of China (2007AA06Z115)+1 种基金the Ph.D. Programs Foundation of Ministry of Education of China (20090010110003)the Fundamental Research Funds for the Central Universities (ZD1001)
文摘Fe-based ionic liquid (Fe-IL) was synthesized by mixing FeCl3·6H2O and 1-butyl-3-methylimidazolium chloride [Bmim]C1 in this paper. The phase diagram of a ternary Fe-IL, ethanol and water system was investigated to construct a ternary desulfurization solution for wet flue gas desulfurization. The effects of flow rate and concentration of SO2, reaction temperature, pH and Fe-IL fraction in aqueous desulfurization solution on the desulfiariza- tion efficiency were investigated. The results shows that the best composition of ternary desulfurization solution of Fe-IL, ethanol and water is 1 : 1.5 : 3 by volume ratio, and pH should be controlled at 2.0. Under such conditions, a desulfurization rate greater than 90% could be obtained. The product of sulfuric acid had inhibition effect on the wet desulfurization process. With applying this new ternary desulfurization solution, not only the catalyst Fe-IL can be recycled and reused, but also the product sulfuric acid can be separated directly from the ternary desulfurization system.
基金Project(2017YFC0210500)supported by the National Key Technology R&D Program of ChinaProject(2017ACA092)supported by the Major Projects of Technical Innovation in Hubei Province,China
文摘The absorbent composing of Bayer red mud and water was prepared and applied to removing SO2 from flue gas.Effects of the ratio of liquid to solid(L/S),the absorption temperature,the inlet SO2 concentration,the O2 concentration,SO4^2-and other different components of Bayer red mud on desulfurization were conducted.The mechanism of flue gas desulfurization was also established.The results indicated that L/S was the prominent factor,followed by the inlet SO2 concentration and the temperature was the least among them.The optimum condition was as follows:L/S,the temperature and the SO2 concentration were 20:1,25℃and 1000 mg/m^3,respectively,under the gas flow of 1.5 L/min.The desulfurization efficiency was not significantly influenced when O2 concentration was above 7%.The accumulation of SO4^2-inhibited the desulfurization efficiency.The alkali absorption and metal ions liquid catalytic oxidation were involved in the process,which accounted for 98.61%.
基金supported by the National Natural Science Foundation of China(No.21276049)the National Basic Research Program of China(973 Program)(No.2013CB228505)the Science and Technology Support Program of Jiangsu(No.BE2014856) for their financial support
文摘The relationship between the fine particles emitted after desulfurization and gypsum crystals in the desulfurization slurry was investigated,and the crystallization characteristics varying with the operation parameters and compositions of the desulfurization slurry were discussed.The results showed that the fine particles generated during the desulfurization process were closely related to the crystal characteristics in the desulfurization slurry by comparison of their morphology and elements. With the higher proportion of fine crystals in the desulfurization slurry,the number concentration of fine particles after desulfurization was increased and their particle sizes were smaller,indicating that the optimization of gypsum crystallization was beneficial for the reduction of the fine particle emission. The lower p H value and an optimal temperature of the desulfurization slurry were beneficial to restrain the generation of fine crystals in the desulfurization slurry. In addition,the higher concentrations of the Fe3+ions and the F- ions in the desulfurization slurry both promoted the generation of fine crystals with corresponding change of the morphology and the effect of the Fe3+ ions was more obvious.With the application of the desulfurization synergist additive,it was beneficial for the inhibition of fine crystals while the thinner crystals were generated.
基金Supported by National Natural Science Foundation of China(61873006,61673053)National Key Research and Development Project(2018YFC1602704,2018YFB1702704)。
文摘In order to improve the slurry pH control accuracy of the absorption tower in the wet flue gas desulfurization process,a model free adaptive predictive control algorithm for the desulfurization slurry pH which is based on a cyber physical systems framework is proposed.First,aiming to address system characteristics of non-linearity and pure hysteresis in slurry pH change process,a model free adaptive predictive control algorithm based on compact form dynamic linearization is proposed by combining model free adaptive control algorithm with model predictive control algorithm.Then,by integrating information resources with the physical resources in the absorption tower slurry pH control process,an absorption tower slurry pH optimization control system based on cyber physical systems is constructed.It is turned out that the model free adaptive predictive control algorithm under the framework of the cyber physical systems can effectively realize the high-precision tracking control of the slurry pH of the absorption tower,and it has strong robustness.
基金supported by the National Key R&D Program of China(No.2017YFC0209905)the National Natural Science Foundation of China(Nos.91544232&51638001)+2 种基金the National Key Technology Research and Development Program of the Ministry of Science and Technology of China(Nos.2013BAC17B01,2014BAC23B00)the Ministry of Environmental Protection Special Funds for Scientific Research on Public Causes(No.201409006)the fund support from Beijing Municipal Commission of Science and Technology(Nos.D161100004416001,Z161100004516013)
文摘In this study, the characteristics of fine particles before and after wet flue gas desulfurization(WFGD) in three coal-fired heating boilers in northern China were investigated by using a dilution-based emission sampling experimental system. The influences of the WFGD process on the mass and number concentrations as well as the chemical composition of fine particles were analyzed. The removal efficiency of desulfurization processes on particulate matter mass was 30.06%–56.25% for the three study units. The WFGD had a great influence on the size distributions of particle mass concentration and number concentration. A significant increase in the number and mass concentration of particles in the size range of 0.094–0.946 μm was observed. The watersoluble ion content accounted for a very large proportion of PM_(2.5) mass, and its proportion in PM_(2.5) increased from 28.39%–41.08% to 48.96%–61.21% after the WFGD process for the three units. The desulfurizing process also drastically increased the proportion of cation component(Ca^(2+) for unit A, Mg^(2+) for unit B, and Na+for unit C) and the proportion of SO_4^(2-) in PM_(2.5), and it increased the CE/AE values of PM_(2.5) from 0.82–0.98 to 0.93–1.27 for the three study units.
基金supported by the National Natural Science Foundation of China(Nos.51576039 and 51576039).
文摘Selective catalytic reduction(SCR) denitration may increase the emission of NH4+and NH3.The removal and transformation characteristics of ammonium sulfate aerosols and ammonia slip during the wet flue gas desulfurization(WFGD) process, as well as the effect of desulfurization parameters, were investigated in an experimental system equipped with a simulated SCR flue gas generation system and a limestone-based WFGD system.The results indicate that the ammonium sulfate aerosols and ammonia slip in the flue gas from SCR can be partly removed by slurry scrubbing, while the entrainment and evaporation of desulfurization slurry with accumulated NH4+will generate new ammoniumcontaining particles and gaseous ammonia.The ammonium-containing particles formed by desulfurization are not only derived from the entrainment of slurry droplets, but also from the re-condensation of gaseous ammonia generated by slurry evaporation.Therefore,even if the concentration of NH4+in the desulfurization slurry is quite low, a high level of NH4+was still contained in the fine particles at the outlet of the scrubber.When the accumulated NH4+in the desulfurization slurry was high enough, the WFGD system promoted the conversion of NH3 to NH4+and increased the additional emission of primary NH4+aerosols.With the decline of the liquid/gas ratio and flue gas temperature, the removal efficiency of ammonia sulfate aerosols increased, and the NH4+emitted from entrainment and evaporation of the desulfurization slurry decreased.In addition, the volatile ammonia concentration after the WFGD system was reduced with the decrease of the NH4+concentration and p H values of the slurry.
文摘脱硫过程是具有高度动态非线性和较大延迟时间的复杂工业过程,为了解决烟气脱硫过程的建模问题,设计了注意力机制下的深度长短期记忆(attention mechanism-based long short-term memory,AttLSTM)网络,并基于该网络设计自动编码器,完成脱硫过程异常点的检测。该文首次提出使用AttLSTM网络自编码器对脱硫过程进行离群点检测,并且该网络模型同样首次应用于脱硫过程的辨识任务中。从更深的意义上讲,该文尝试使用深度学习模型对复杂系统进行辨识,所建立的AttLSTM网络之前未出现在系统辨识领域,该网络的出现可以丰富辨识模型的选择,同时为人工智能技术在系统辨识领域和控制领域的应用与推广提供参考。实验结果表明,相比于之前文献出现的脱硫过程建模方法,所提方法在不同性能指标上均具有更好的表现,由此可以证明深度AttLSTM网络在脱硫场景下的有效性。
基金the National Natural Science Foundation of China(NSFC)(Grant Nos.51704004 and 51674002)the Natural Science Foundation of Anhui Province(Grant No.1808085QE133).
文摘The low-temperature wet oxidation behavior of semi-dry desulfurization ash from iron ore sintering flue gas in ammonium citrate solution was investigated for efficiently utilizing the low-quality desulfurization ash. The effects of the ammonium citrate concentration, oxidation temperature, solid/liquid ratio, and oxidation time on the wet oxidation behavior of desulfurization ash were studied. Simultaneously, the oxidation mechanism of desulfurization ash was revealed by means of X-ray diffraction, Zeta electric resistance, and X-ray photoelectron spectroscopy (XPS) analysis. Under the optimal conditions with ammonium citrate, the oxidation ratio of CaSO_(3) was up to the maximum value (98.49%), while that of CaSO_(3) was only 8.92% without ammonium citrate. Zeta electric resistance and XPS results indicate that the dissolution process of CaSO_(3) could be significantly promoted by complexation derived from the ammonium citrate hydrolysis. As a result, the oxidation process of CaSO_(3) was transformed from particle oxidation to SO_(3)^(2−) ion oxidation, realizing the rapid transformation of desulfurization ash from CaSO_(3) to CaSO_(4) at low temperature. It provides a reference for the application of semi-dry desulfurization ash and contributes to sustainable management for semi-dry desulfurization ash.