NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Am...NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Among the technologies for NF_(3)abatement,the destructive sorption of NF_(3)over metal oxides sorbents is an effective way.Thus,the search for a highly reactive and utilized sorbent for NF_(3)destruction is in great demand.In this work,AlOOH supported on carbon-sphere(AlOOH/CS)as precursors were synthesized hydrothermally and heat-treated to prepare the Al_(2)O_(3)sorbents.The influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al_(2)O_(3)sorbents for NF_(3)destruction was investigated,and it is shown that the Al2O3 from AlOOH/CS hydro-thermalized at 120℃is superior to others.Subsequently,the optimized Al_(2)O_(3)was covered by Mn(OH)x to prepare Mn/Al_(2)O_(3)sorbents via changing hydrothermal temperatures and Mn loadings.The results show that the Mn/Al_(2)O_(3)sorbents are more utilized than bare Al_(2)O_(3)in NF_(3)destructive sorption due to the promotional effect of Mn_(2)O_(3)as surface layer on the fluorination of Al_(2)O_(3)as substrate,especially the optimal 5%Mn/Al2O3(160℃)exhibits a utilization percentage as high as 90.4%,and remarkably exceeds all the sorbents reported so far.These findings are beneficial to develop more efficient sorbents for the destruction of NF_(3).展开更多
Supported ionic liquid(IL) sorbents for CO_2 capture were prepared by impregnating tetramethylammonium glycinate([N1111][Gly]) into four types of porous materials in this study. The CO_2 adsorption behavior was invest...Supported ionic liquid(IL) sorbents for CO_2 capture were prepared by impregnating tetramethylammonium glycinate([N1111][Gly]) into four types of porous materials in this study. The CO_2 adsorption behavior was investigated in a thermogravimetric analyzer(TGA). Among them, poly(methyl methacrylate)(PMMA)-[N1111][Gly]exhibits the best CO_2 adsorption properties in terms of adsorption capacity and rate. The CO_2 adsorption capacity reaches up to 2.14 mmol·g-1 sorbent at 35 °C. The fast CO_2 adsorption rate of PMMA-[N1111][Gly] allows 60 min of adsorption equilibrium time at 35 °C and much shorter time of 4 min is achieved at 75 °C. Further, Avrami's fractional-order kinetic model was used and fitted well with the experiment data, which shows good consistency between experimental results and theoretical model. In addition, PMMA-[N1111][Gly] remained excellent durability in the continuous adsorption–desorption cycling test. Therefore, this stable PMMA-[N1111][Gly] sorbent has great potential to be used for fast CO_2 adsorption from flue-gas.展开更多
Under the Paris agreement, China has committed to reducing CO_2 emissions by 60%–65% per unit of GDP by 2030.Since CO_2 emissions from coal-fired power plants currently account for over 30% of the total carbon emissi...Under the Paris agreement, China has committed to reducing CO_2 emissions by 60%–65% per unit of GDP by 2030.Since CO_2 emissions from coal-fired power plants currently account for over 30% of the total carbon emissions in China, it will be necessary to mitigate at least some of these emissions to achieve this goal. Studies by the International Energy Agency(IEA) indicate CCS technology has the potential to contribute 14% of global emission reductions, followed by 40% of higher energy efficiency and 35% of renewable energy, which is considered as the most promising technology to significantly reduce carbon emissions for current coal-fired power plants.Moreover, the announcement of a Chinese national carbon trading market in late 2017 signals an opportunity for the commercial deployment of CO_2 capture technologies.Currently, the only commercially demonstrated technology for post-combustion CO_2 capture technology from power plants is solvent-based absorption. While commercially viable, the costs of deploying this technology are high. This has motivated efforts to develop more affordable alternatives, including advanced solvents, membranes,and sorbent capture systems. Of these approaches, advanced solvents have received the most attention in terms of research and demonstration. In contrast, sorbent capture technology has less attention, despite its potential for much lower energy consumption due to the absence of water in the sorbent. This paper reviews recent progress in the development of sorbent materials modified by amine functionalities with an emphasis on material characterization methods and the effects of operating conditions on performance. The main problems and challenges that need to be overcome to improve the competitiveness of sorbent-based capture technologies are discussed.展开更多
A new industrial S Zorb sorbent(Ni/Zn O-P) was prepared by using the spray drying technique. The other two traditional sorbents(Ni/Zn O-M and Ni/Zn O-H) were prepared in exactly the same way except the use of differen...A new industrial S Zorb sorbent(Ni/Zn O-P) was prepared by using the spray drying technique. The other two traditional sorbents(Ni/Zn O-M and Ni/Zn O-H) were prepared in exactly the same way except the use of different silica-alumina binder matrices. The XRD, Rietveld quantitative phase analysis, BET, and laser particle size analysis were employed to characterize their physico-chemical properties. The deactivation mechanism and desulfurization kinetics of sorbent was investigated on a water vapor aging treatment device. It was shown that both the water vapor pressure and reaction temperature significantly could influence the formation rate of inactive Zn2 Si O4, which could decrease the sulfur storage capacity of sorbents. The Zn2 Si O4 content profiles could be fitted into the zero order equation, from which the apparent rate constant k and the activation energy E a were calculated. The matrix P greatly raised the E a of Zn2 Si O4 formation due to the less bridged hydroxyl silanol groups on its surface, which accounted for the high stability of Ni/Zn O-P. The desulfurization performance of the fresh and aged sorbents showed that the overall average sulfur conversion of Ni/Zn O-P(aged) was 92%, which was close to that of fresh sorbents(95%), and was higher than that of Ni/Zn O-M(aged)(86%) and Ni/Zn O-H(aged)(90%). Based on these findings, the application of Ni/Zn O-P can greatly improve the long-term running stability of the industrial unit.展开更多
The objective of this work is to study the influences of silica supports and PEG additive on the sorption performance of molecular basket sorbent(MBS) for COcapture consisting of polyethylenimine and one of the foll...The objective of this work is to study the influences of silica supports and PEG additive on the sorption performance of molecular basket sorbent(MBS) for COcapture consisting of polyethylenimine and one of the following supports: SBA-15(2-D structure), TUD-1(3-D sponge-like structure) and fumed silica HS-5(3-D disordered structure). Effects of the supports regarding pore structures and pore properties, the PEI loading amount as well as the sorption temperature were examined. Furthermore, polyethylene glycol(PEG) was introduced as an additive into the sorbents and its effect was investigated at different PEI loadings and sorption temperatures. The results suggest that the pore properties of MBS(after PEI loading) play a more important role in the COsorption capacity, rather than those of the supports alone.MBS with 3D pore structure exhibits higher COsorption capacity and amine efficiency than those with 2D-structured support. Among the sorbents studied, fumed silica(HS-5) based MBS showed the highest COsorption capacity in the temperature range of 30-95 °C, probably due to its unique interstitial pores formed by the aggregation of polymer-loaded SiOparticles. It was found that the temperature dependence is directly related to the PEI surface coverage layers. The more PEI surface coverage layers, the higher diffusion barrier for COand the stronger temperature dependence of COcapacity. 3D MBS exceeds 2D MBS at the same PEI coverage layers due to lower diffusion barrier. Adding PEG can significantly enhance the COsorption capacity and improve amine efficiency of all MBS, most likely by alleviating the diffusion barrier within PEI bulk layers through the inter-molecular interaction between PEI and PEG.展开更多
By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candi...By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials has been proposed and validated. The ab initio thermodynamic technique has the advantage of allowing identification of thermodynamic properties of CO2 capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. For a given solid, the first step is to attempt to extract thermodynamic properties from thermodynamic databases and the available literatures. If the thermodynamic properties of the compound of interest are unknown, an ab initio thermodynamic approach is used to calculate them. These properties expressed conveniently as chemical potentials and heat of reactions, which obtained either from databases or from calculations, are further used for computing the thermodynamic reaction equilibrium properties of the CO2 absorption/desorption cycles. Only those solid materials for which lower capture energy costs are predicted at the desired process conditions are selected as CO2 sorbent candidates and are further considered for ex- perimental validations. Solid sorbents containing alkali and alkaline earth metals have been reported in several previous studies to be good candidates for CO2 sorbent applications due to their high CO2 absorption capacity at moderate work- ing temperatures. In addition to introducing our computational screening procedure, in this presentation we will sum- marize our results for solid systems composed by alkali and alkaline earth metal oxides, hydroxides, and carbonates/bicarbonates to validate our methodology. Additionally, applications of our computational method to mixed solid systems of Li2O with SiO2/ZrO2 with different mixing ratios, our preliminary results showed that increasing the Li2O/SiO2 ratio in lithium silicates increases their corresponding turnover temperatures for CO2 capture reactions. Overall these theoretical predictions are found to be in good agreement with available experimental findings.展开更多
In this paper, study on the effect of preparation conditions of K2CO3/Al2O3 sorbent was done. Box-Behnken design was applied to study the influence of four parameters involve initial solution concentration, impregnati...In this paper, study on the effect of preparation conditions of K2CO3/Al2O3 sorbent was done. Box-Behnken design was applied to study the influence of four parameters involve initial solution concentration, impregnation time and calcination step temperature and time. A quadratic model was used to correlate the sorbent capture capacity. The model was used to calculate the optimum conditions for preparing sorbent. From the analysis of variance (ANOVA), the most influential factor on each experimental design response was identified. The potassium-based sorbents used in this study were prepared by impregnating K2CO3 on Al2O3 support. The CO2 capture capacity was measured in the presence of H2O in a fixed-bed reactor at CO2 capture temperature of 60°C using breakthrough curves. The optimum sorbent prepared by this method showed CO2 capture capacity of 77.21 mg CO2/g sorbent. It was observed that the experimental values obtained were in good agreement with the values predicted by the model, with relatively small errors between the predicted and the actual values. The results obtained in this study can be used as basic data for study on design and operating condition optimization of CO2 capture process using these sorbents.展开更多
High-temperature pyrolysis technology can effectively solve the problem of municipal solid waste pollution.However,the pyrolysis gas contains a large amount of CO_(2),which would adversely affect the subsequent utiliz...High-temperature pyrolysis technology can effectively solve the problem of municipal solid waste pollution.However,the pyrolysis gas contains a large amount of CO_(2),which would adversely affect the subsequent utilization.To address this problem,a novel method of co-precipitation modification with Ca,Mg and Zr metals was proposed to improve the CO_(2)capture performance.X-ray diffraction(XRD)patterns and energy dispersive X-ray spectroscopy analysis showed that the two inert supports MgO and CaZrO_(3)were uniformly distributed in the modified calcium-based sorbents.In addition,the XRD results indicated that CaZrO_(3)was produced by the reaction of ZrO_(2)and CaO at high temperatures.The effects of doping ratios,adsorption temperature,calcination temperature,CO_(2)concentration and calcination atmosphere on the adsorption capacity and cycle stability of the modified calcium-based sorbent were studied.The modified calcium-based sorbent achieved the best CO_(2)capture performance when the doping ratio was 10:1:1 with carbonation at 700℃ under 20%CO_(2)/80%N_(2)atmosphere and calcination at 900℃ under100%N_(2)atmosphere.After ten cycles,the average carbonation conversion rate of Ca-10 sorbent was 72%.Finally,the modified calcium-based sorbents successfully reduced the CO_(2)concentration of the pyrolysis gas from 37%to 5%.展开更多
CuMn_(2)O_(4)spinel has been regarded as a highly efficient sorbent for Hg^(0)capture from flue gas.The regenerability and recyclability of CuMn_(2)O_(4)sorbent are mainly associated with the mercury speciation adsorb...CuMn_(2)O_(4)spinel has been regarded as a highly efficient sorbent for Hg^(0)capture from flue gas.The regenerability and recyclability of CuMn_(2)O_(4)sorbent are mainly associated with the mercury speciation adsorbed on its surface.However,the effect mechanism of HCl on Hg^(0)transformation over CuMn_(2)O_(4)sorbent is still elusive.Experiments were conducted to understand the effect of HCl on Hg^(0)transformation over CuMn_(2)O_(4)sorbent.The results indicate thatCuMn_(2)O_(4)sorbent is a mesoporousmaterial and possesses a good thermal stability.CuMn_(2)O_(4)shows>95%Hg^(0)removal efficiency in a wide temperature window of 50-350℃.The favorable electron-transfer environment caused by the mixed valence states of Cu and Mn cations is responsible for the excellent Hg^(0)removal performance of CuMn_(2)O_(4)sorbent.CuMn_(2)O_(4)shows a higherHg^(0)adsorption capacity of 4774.57μg/g.Hg^(0)adsorption process over CuMn_(2)O_(4)sorbent can bewell described by the developed kinetic model.Hg^(0)removal efficiency of CuMn_(2)O_(4)sorbent does not depend on the presence of HCl.Mercury species adsorbed on the CuMn_(2)O_(4)sorbent in the presence of HCl mainly exist in the forms of Hg^(O)and HgCl_(2)O_(8)·H_(2)O.HCl shows a significant effect on mercury speciation over CuMn_(2)O_(4)sorbent.Most of Hg^(O)species will be transformed into HgCl_(2)O_(8)·H_(2)O in the presence of HCl.展开更多
In this paper,a low-cost and environmental-friendly leaching agent citric acid(C_(6)H_(8)O_(7))was used to treat the sediment of Dianchi Lake(SDL)to synthesize lithium silicate(Li_(4)SiO_(4))based CO_(2)sorbent.The re...In this paper,a low-cost and environmental-friendly leaching agent citric acid(C_(6)H_(8)O_(7))was used to treat the sediment of Dianchi Lake(SDL)to synthesize lithium silicate(Li_(4)SiO_(4))based CO_(2)sorbent.The results were compared with that treated with strong acid.Moreover,the effects of preparation conditions,sorption conditions and desorption conditions on the CO_(2)sorption performance of prepared Li_(4)SiO_(4)were systematically studied.Under optimal conditions,the Li_(4)SiO_(4)sorbent was successfully synthesized and its CO_(2)sorption capacity reached 31.37%(mass),which is much higher than that synthesized from SDL treated with strong acid.It is speculated that the presence of some elements after C_(6)H_(8)O_(7)treatment may promote the sorption of synthetic Li_(4)SiO_(4)to CO_(2).In addition,after doping with K_(2)CO_(3),the CO_(2)uptake increases from the original 12.02%and 22.12%to 23.96%and 32.41%(mass)under the 20%and 50%CO_(2)partial pressure,respectively.More importantly,after doping K_(2)CO_(3),the synthesized Li_(4)SiO_(4)has a high cyclic stability under the low CO_(2)partial pressure.展开更多
The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered dow...The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered down to 600℃,while its reactivity increased with increased temperature and the equilibrium conversion reached up to over 60% at temperatLlre of 900℃.However, side reactions of H2S in conjunction with high-temperature decomposition and mineral catalysis to elemental sulfur and sulfur dioxide were testified.展开更多
基金The financial support from the Natural Science Foundation of Shandong Province (ZR2020KB003)
文摘NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Among the technologies for NF_(3)abatement,the destructive sorption of NF_(3)over metal oxides sorbents is an effective way.Thus,the search for a highly reactive and utilized sorbent for NF_(3)destruction is in great demand.In this work,AlOOH supported on carbon-sphere(AlOOH/CS)as precursors were synthesized hydrothermally and heat-treated to prepare the Al_(2)O_(3)sorbents.The influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al_(2)O_(3)sorbents for NF_(3)destruction was investigated,and it is shown that the Al2O3 from AlOOH/CS hydro-thermalized at 120℃is superior to others.Subsequently,the optimized Al_(2)O_(3)was covered by Mn(OH)x to prepare Mn/Al_(2)O_(3)sorbents via changing hydrothermal temperatures and Mn loadings.The results show that the Mn/Al_(2)O_(3)sorbents are more utilized than bare Al_(2)O_(3)in NF_(3)destructive sorption due to the promotional effect of Mn_(2)O_(3)as surface layer on the fluorination of Al_(2)O_(3)as substrate,especially the optimal 5%Mn/Al2O3(160℃)exhibits a utilization percentage as high as 90.4%,and remarkably exceeds all the sorbents reported so far.These findings are beneficial to develop more efficient sorbents for the destruction of NF_(3).
基金Supported by the National Basic Research Program of China(2013CB733503)the National Natural Science Foundation of China(21136001,21136004,21476106,21428601,21776123)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)and the Jiangsu Natural Science Foundation(BK20130062)
文摘Supported ionic liquid(IL) sorbents for CO_2 capture were prepared by impregnating tetramethylammonium glycinate([N1111][Gly]) into four types of porous materials in this study. The CO_2 adsorption behavior was investigated in a thermogravimetric analyzer(TGA). Among them, poly(methyl methacrylate)(PMMA)-[N1111][Gly]exhibits the best CO_2 adsorption properties in terms of adsorption capacity and rate. The CO_2 adsorption capacity reaches up to 2.14 mmol·g-1 sorbent at 35 °C. The fast CO_2 adsorption rate of PMMA-[N1111][Gly] allows 60 min of adsorption equilibrium time at 35 °C and much shorter time of 4 min is achieved at 75 °C. Further, Avrami's fractional-order kinetic model was used and fitted well with the experiment data, which shows good consistency between experimental results and theoretical model. In addition, PMMA-[N1111][Gly] remained excellent durability in the continuous adsorption–desorption cycling test. Therefore, this stable PMMA-[N1111][Gly] sorbent has great potential to be used for fast CO_2 adsorption from flue-gas.
基金Supported by the National Key Research and Development Program of China(2017YFB0603301)
文摘Under the Paris agreement, China has committed to reducing CO_2 emissions by 60%–65% per unit of GDP by 2030.Since CO_2 emissions from coal-fired power plants currently account for over 30% of the total carbon emissions in China, it will be necessary to mitigate at least some of these emissions to achieve this goal. Studies by the International Energy Agency(IEA) indicate CCS technology has the potential to contribute 14% of global emission reductions, followed by 40% of higher energy efficiency and 35% of renewable energy, which is considered as the most promising technology to significantly reduce carbon emissions for current coal-fired power plants.Moreover, the announcement of a Chinese national carbon trading market in late 2017 signals an opportunity for the commercial deployment of CO_2 capture technologies.Currently, the only commercially demonstrated technology for post-combustion CO_2 capture technology from power plants is solvent-based absorption. While commercially viable, the costs of deploying this technology are high. This has motivated efforts to develop more affordable alternatives, including advanced solvents, membranes,and sorbent capture systems. Of these approaches, advanced solvents have received the most attention in terms of research and demonstration. In contrast, sorbent capture technology has less attention, despite its potential for much lower energy consumption due to the absence of water in the sorbent. This paper reviews recent progress in the development of sorbent materials modified by amine functionalities with an emphasis on material characterization methods and the effects of operating conditions on performance. The main problems and challenges that need to be overcome to improve the competitiveness of sorbent-based capture technologies are discussed.
基金supported by the Science and Technology Development projects of SINOPEC, China (Nos. 113138, 112008 and 110099)
文摘A new industrial S Zorb sorbent(Ni/Zn O-P) was prepared by using the spray drying technique. The other two traditional sorbents(Ni/Zn O-M and Ni/Zn O-H) were prepared in exactly the same way except the use of different silica-alumina binder matrices. The XRD, Rietveld quantitative phase analysis, BET, and laser particle size analysis were employed to characterize their physico-chemical properties. The deactivation mechanism and desulfurization kinetics of sorbent was investigated on a water vapor aging treatment device. It was shown that both the water vapor pressure and reaction temperature significantly could influence the formation rate of inactive Zn2 Si O4, which could decrease the sulfur storage capacity of sorbents. The Zn2 Si O4 content profiles could be fitted into the zero order equation, from which the apparent rate constant k and the activation energy E a were calculated. The matrix P greatly raised the E a of Zn2 Si O4 formation due to the less bridged hydroxyl silanol groups on its surface, which accounted for the high stability of Ni/Zn O-P. The desulfurization performance of the fresh and aged sorbents showed that the overall average sulfur conversion of Ni/Zn O-P(aged) was 92%, which was close to that of fresh sorbents(95%), and was higher than that of Ni/Zn O-M(aged)(86%) and Ni/Zn O-H(aged)(90%). Based on these findings, the application of Ni/Zn O-P can greatly improve the long-term running stability of the industrial unit.
基金the support of this work at Penn State by the U.S.Department of Energy,National Energy Technology Laboratorythe financial support by the China Scholarship Council,the Natural Science Foundation of China(No.51176034)the Open Fund of Key Laboratory of Coal-Based CO2 Capture and Geological Storage of Jiangsu Province(2016A05)
文摘The objective of this work is to study the influences of silica supports and PEG additive on the sorption performance of molecular basket sorbent(MBS) for COcapture consisting of polyethylenimine and one of the following supports: SBA-15(2-D structure), TUD-1(3-D sponge-like structure) and fumed silica HS-5(3-D disordered structure). Effects of the supports regarding pore structures and pore properties, the PEI loading amount as well as the sorption temperature were examined. Furthermore, polyethylene glycol(PEG) was introduced as an additive into the sorbents and its effect was investigated at different PEI loadings and sorption temperatures. The results suggest that the pore properties of MBS(after PEI loading) play a more important role in the COsorption capacity, rather than those of the supports alone.MBS with 3D pore structure exhibits higher COsorption capacity and amine efficiency than those with 2D-structured support. Among the sorbents studied, fumed silica(HS-5) based MBS showed the highest COsorption capacity in the temperature range of 30-95 °C, probably due to its unique interstitial pores formed by the aggregation of polymer-loaded SiOparticles. It was found that the temperature dependence is directly related to the PEI surface coverage layers. The more PEI surface coverage layers, the higher diffusion barrier for COand the stronger temperature dependence of COcapacity. 3D MBS exceeds 2D MBS at the same PEI coverage layers due to lower diffusion barrier. Adding PEG can significantly enhance the COsorption capacity and improve amine efficiency of all MBS, most likely by alleviating the diffusion barrier within PEI bulk layers through the inter-molecular interaction between PEI and PEG.
文摘By combining thermodynamic database mining with first principles density functional theory and phonon lattice dynamics calculations, a theoretical screening methodology to identify the most promising CO2 sorbent candidates from the vast array of possible solid materials has been proposed and validated. The ab initio thermodynamic technique has the advantage of allowing identification of thermodynamic properties of CO2 capture reactions without any experimental input beyond crystallographic structural information of the solid phases involved. For a given solid, the first step is to attempt to extract thermodynamic properties from thermodynamic databases and the available literatures. If the thermodynamic properties of the compound of interest are unknown, an ab initio thermodynamic approach is used to calculate them. These properties expressed conveniently as chemical potentials and heat of reactions, which obtained either from databases or from calculations, are further used for computing the thermodynamic reaction equilibrium properties of the CO2 absorption/desorption cycles. Only those solid materials for which lower capture energy costs are predicted at the desired process conditions are selected as CO2 sorbent candidates and are further considered for ex- perimental validations. Solid sorbents containing alkali and alkaline earth metals have been reported in several previous studies to be good candidates for CO2 sorbent applications due to their high CO2 absorption capacity at moderate work- ing temperatures. In addition to introducing our computational screening procedure, in this presentation we will sum- marize our results for solid systems composed by alkali and alkaline earth metal oxides, hydroxides, and carbonates/bicarbonates to validate our methodology. Additionally, applications of our computational method to mixed solid systems of Li2O with SiO2/ZrO2 with different mixing ratios, our preliminary results showed that increasing the Li2O/SiO2 ratio in lithium silicates increases their corresponding turnover temperatures for CO2 capture reactions. Overall these theoretical predictions are found to be in good agreement with available experimental findings.
文摘In this paper, study on the effect of preparation conditions of K2CO3/Al2O3 sorbent was done. Box-Behnken design was applied to study the influence of four parameters involve initial solution concentration, impregnation time and calcination step temperature and time. A quadratic model was used to correlate the sorbent capture capacity. The model was used to calculate the optimum conditions for preparing sorbent. From the analysis of variance (ANOVA), the most influential factor on each experimental design response was identified. The potassium-based sorbents used in this study were prepared by impregnating K2CO3 on Al2O3 support. The CO2 capture capacity was measured in the presence of H2O in a fixed-bed reactor at CO2 capture temperature of 60°C using breakthrough curves. The optimum sorbent prepared by this method showed CO2 capture capacity of 77.21 mg CO2/g sorbent. It was observed that the experimental values obtained were in good agreement with the values predicted by the model, with relatively small errors between the predicted and the actual values. The results obtained in this study can be used as basic data for study on design and operating condition optimization of CO2 capture process using these sorbents.
基金the support given by the National Key Research and Development Program of China(2018YFC1901203)Natural Science Foundation of Guangdong Province,China(2021A1515010497)+1 种基金Guangzhou Science and Technology Innovation Development Special FundFundamental Research Funds for the Central Universities(2019MS017)。
文摘High-temperature pyrolysis technology can effectively solve the problem of municipal solid waste pollution.However,the pyrolysis gas contains a large amount of CO_(2),which would adversely affect the subsequent utilization.To address this problem,a novel method of co-precipitation modification with Ca,Mg and Zr metals was proposed to improve the CO_(2)capture performance.X-ray diffraction(XRD)patterns and energy dispersive X-ray spectroscopy analysis showed that the two inert supports MgO and CaZrO_(3)were uniformly distributed in the modified calcium-based sorbents.In addition,the XRD results indicated that CaZrO_(3)was produced by the reaction of ZrO_(2)and CaO at high temperatures.The effects of doping ratios,adsorption temperature,calcination temperature,CO_(2)concentration and calcination atmosphere on the adsorption capacity and cycle stability of the modified calcium-based sorbent were studied.The modified calcium-based sorbent achieved the best CO_(2)capture performance when the doping ratio was 10:1:1 with carbonation at 700℃ under 20%CO_(2)/80%N_(2)atmosphere and calcination at 900℃ under100%N_(2)atmosphere.After ten cycles,the average carbonation conversion rate of Ca-10 sorbent was 72%.Finally,the modified calcium-based sorbents successfully reduced the CO_(2)concentration of the pyrolysis gas from 37%to 5%.
基金This work was supported by National Key R&D Program of China(2016YFB0600604)National Natural Science Foundation of China(52006083)Fundamental Research Funds for the Central Universities(2019kfyRCPY021).
文摘CuMn_(2)O_(4)spinel has been regarded as a highly efficient sorbent for Hg^(0)capture from flue gas.The regenerability and recyclability of CuMn_(2)O_(4)sorbent are mainly associated with the mercury speciation adsorbed on its surface.However,the effect mechanism of HCl on Hg^(0)transformation over CuMn_(2)O_(4)sorbent is still elusive.Experiments were conducted to understand the effect of HCl on Hg^(0)transformation over CuMn_(2)O_(4)sorbent.The results indicate thatCuMn_(2)O_(4)sorbent is a mesoporousmaterial and possesses a good thermal stability.CuMn_(2)O_(4)shows>95%Hg^(0)removal efficiency in a wide temperature window of 50-350℃.The favorable electron-transfer environment caused by the mixed valence states of Cu and Mn cations is responsible for the excellent Hg^(0)removal performance of CuMn_(2)O_(4)sorbent.CuMn_(2)O_(4)shows a higherHg^(0)adsorption capacity of 4774.57μg/g.Hg^(0)adsorption process over CuMn_(2)O_(4)sorbent can bewell described by the developed kinetic model.Hg^(0)removal efficiency of CuMn_(2)O_(4)sorbent does not depend on the presence of HCl.Mercury species adsorbed on the CuMn_(2)O_(4)sorbent in the presence of HCl mainly exist in the forms of Hg^(O)and HgCl_(2)O_(8)·H_(2)O.HCl shows a significant effect on mercury speciation over CuMn_(2)O_(4)sorbent.Most of Hg^(O)species will be transformed into HgCl_(2)O_(8)·H_(2)O in the presence of HCl.
基金the financial support from National Natural Science Foundation of China(21868015,51802135)the Applied Basic Research Programs of Yunnan Province(140520210057)+1 种基金Taif University Researchers Supporting Project number(TURSP-2020/163)Taif University,Taif,Saudi Arabia。
文摘In this paper,a low-cost and environmental-friendly leaching agent citric acid(C_(6)H_(8)O_(7))was used to treat the sediment of Dianchi Lake(SDL)to synthesize lithium silicate(Li_(4)SiO_(4))based CO_(2)sorbent.The results were compared with that treated with strong acid.Moreover,the effects of preparation conditions,sorption conditions and desorption conditions on the CO_(2)sorption performance of prepared Li_(4)SiO_(4)were systematically studied.Under optimal conditions,the Li_(4)SiO_(4)sorbent was successfully synthesized and its CO_(2)sorption capacity reached 31.37%(mass),which is much higher than that synthesized from SDL treated with strong acid.It is speculated that the presence of some elements after C_(6)H_(8)O_(7)treatment may promote the sorption of synthetic Li_(4)SiO_(4)to CO_(2).In addition,after doping with K_(2)CO_(3),the CO_(2)uptake increases from the original 12.02%and 22.12%to 23.96%and 32.41%(mass)under the 20%and 50%CO_(2)partial pressure,respectively.More importantly,after doping K_(2)CO_(3),the synthesized Li_(4)SiO_(4)has a high cyclic stability under the low CO_(2)partial pressure.
文摘The H2S removal characteristics of Taxada lime tinder the high temperature of 600-900℃ have been investigated. The test results indicated that this kind of sorbent almost was inert to H2S When temperature lowered down to 600℃,while its reactivity increased with increased temperature and the equilibrium conversion reached up to over 60% at temperatLlre of 900℃.However, side reactions of H2S in conjunction with high-temperature decomposition and mineral catalysis to elemental sulfur and sulfur dioxide were testified.