Activated carbon(AC)has been widely used in the removal of SO_(2) from flue gas owing to its well-developed pore structure and abundant functional groups.Herein,the effect of alkali/alkaline earth metals on sulfur mig...Activated carbon(AC)has been widely used in the removal of SO_(2) from flue gas owing to its well-developed pore structure and abundant functional groups.Herein,the effect of alkali/alkaline earth metals on sulfur migration was investigated based on the dynamic adsorption and temperature programmed desorption experiment.The adsorption and desorption properties of six types of AC(three commercial and three laboratory-made)were carried out on a fixed-bed experimental device,and the physical and chemical properties of samples were determined by X-ray fluorescence,X-ray diffraction,scanning electron microscopy/energy dispersive X-ray,and X-ray photoelectron spectroscopy analysis.The experimental results showed that the adsorbed SO_(2) cannot be completely desorbed by increasing the regeneration temperature(350-850℃),while the SO_(2) fixed in the AC combines with the Ca-based minerals in the ash to form a stable sulfate.For different samples,higher ash content,higher CaO content in the ash and a more developed pore structure lead to a higher SO_(2) fixation rate.Moreover,the multiple adsorption-desorption cycles experiment showed that the effect of SO_(2) fixation is mainly reflected in the first cycle,after which the adsorption and desorption amount are approximately the same.This study elucidates the effect of alkali/alkaline earth metals on the adsorption-desorption cycle of AC,which provides a deeper understanding of sulfur migration in the AC flue gas desulfurization process.展开更多
The Al-pillared montmorillonite-supported alkaline earth metal 5M/Al-PILC(PILC = pillared clay, M = Mg, Ca, Sr, and Ba) and x Mg/Al-PILC( x = 1, 3, 5, and 7 wt.%) samples were prepared using an impregnation method. Ph...The Al-pillared montmorillonite-supported alkaline earth metal 5M/Al-PILC(PILC = pillared clay, M = Mg, Ca, Sr, and Ba) and x Mg/Al-PILC( x = 1, 3, 5, and 7 wt.%) samples were prepared using an impregnation method. Physical properties of the materials were determined by means of X-ray diffraction(XRD) and N2 adsorption-desorption, and their CO2 adsorption behaviors were investigated using the thermogravimetric analyzer(TG), CO2 temperatureprogrammed desorption(CO2-TPD), and in situ diffuse reflectance infrared transform spectroscopy(in situ-DRIFTS) techniques. It is shown that 5 Mg/Al-PILC possessed the highest CO2 adsorption capacity(2.559 mmol/g). The characterization results indicate that Alpillaring increased the specific surface area of montmorillonite, which was beneficial for the adsorption of CO2. The CO2 adsorption process on the sample was mainly chemical adsorption, and alkalinity was the main factor influencing its adsorption capacity. The alkalinity of the sample was enhanced by loading an appropriate amount of alkaline earth metal, and the adsorbed CO2 was present in the form of bicarbonate and carbonate. In addition, the 5Mg/Al-PILC sample exhibited an excellent regeneration efficiency. We believe that the outcome of this research would provide a good option for developing highly effective CO2 adsorption materials.展开更多
Development of active and non-noble metal-based catalyst for H2 production via NH3 decomposition is crucial for the implementation of NH3 as a H2 carrier.Co-based catalysts have received increasing attention because o...Development of active and non-noble metal-based catalyst for H2 production via NH3 decomposition is crucial for the implementation of NH3 as a H2 carrier.Co-based catalysts have received increasing attention because of its high intrinsic activity and moderate cost.In this work,we examined the effect of BaNH,CaNH and Mg3 N2 on the catalytic activity of Co in the NH3 decomposition reaction.The H2 formation rate ranks the order as Co-BaNH>Co-CaNH>Co-Mg3 N2≈Co/CNTs within a reaction temperature range of 300-550℃.It is worth pointing out that the H2 formation rate of Co-BaNH at 500℃reaches20 mmolH2 gcat-1 min-1,which is comparable to those of the active Ru/Al2 O3(ca.17 mmolH2 gcat-1 min1)and Ru/AC(21 mmolH2 gcat-1 min-1)catalysts under the similar reaction conditions.In-depth research shows that Co-BaNH exhibits an obviously higher intrinsic activity and much lower Ea(46.2 kJ mol-1)than other Co-based catalysts,suggesting that BaNH may play a different role from CaNH,Mg3 N2 and CNTs during the catalytic process.Combined results of XRD,Ar-TPD and XAS show that a[Co-N-Ba]-like intermediate species is likely formed at the interface of Co metal and BaNH,which may lead to a more energy-efficient reaction pathway than that of neat Co metal for NH3 decomposition.展开更多
To improve the removal capacity of NO + O_(2) effectively, the alkaline earth metal-doped order mesoporous carbon(A-C-FDU-15(0.001)(A = Mg, Ca, Sr and Ba)) and Mg-C-FDU-15( x)( x = 0.001-0.003) samples were prepared, ...To improve the removal capacity of NO + O_(2) effectively, the alkaline earth metal-doped order mesoporous carbon(A-C-FDU-15(0.001)(A = Mg, Ca, Sr and Ba)) and Mg-C-FDU-15( x)( x = 0.001-0.003) samples were prepared, and their physicochemical and NO + O_(2) adsorption properties were determined by means of various techniques. The results show that the sequence in(NO + O_(2)) adsorption performance was as follows: Mg-C-FDU-15(0.001)(93.2 mg/g) > Ca-C-FDU-15(0.001)(82.2 mg/g) > Sr-C-FDU-15(0.001)(76.1 mg/g) > Ba-C-FDU-15(0.001)(72.9 mg/g) > C-FDU-15(67.1 mg/g). Among all of the A-C-FDU-15(0.001) samples, Mg-C-FDU-15(0.001) possessed the highest(NO + O_(2)) adsorption capacity(106.2 mg/g). The species of alkaline earth metals and basic sites were important factors determining the adsorption of NO + O_(2) on the A-C-FDU-15( x) samples, and(NO + O_(2)) adsorption on the samples was mainly chemical adsorption. Combined with the results of(NO + O_(2))-temperatureprogrammed desorption((NO + O_(2))-TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS) characterization, we deduced that there were two main pathways of(NO + O_(2)) adsorption: one was first the conversion of NO and O_(2) to NO_(2) and then part of NO_(2) was converted to NO_(2)^(-) and NO_(3)^(-);and the other was the direct oxidation of NO to NO-2 and NO_(3)^(-).展开更多
Combustion of agricultural organic solid waste(AOSW)was an ideal solution for their resource utilization in view of their massive annual production and great potential for reduction of fossil fuel utilization.However,...Combustion of agricultural organic solid waste(AOSW)was an ideal solution for their resource utilization in view of their massive annual production and great potential for reduction of fossil fuel utilization.However,high alkali and alkaline earth metals(AAEMs)content in the feedstock can arose severe fouling and slagging issues and thus prohibiting its vast utilization.In this study,a semi-continuous water washing method was proposed to preliminarily remove AAEMs from agricultural organic solid waste and its effects on the combustion behaviors of washed solid product were investigated.Results showed that the combustion index S were improved to 2.63×10-6,over 68%of the total ashes were removed from the cotton stalk,and 96.3%,89.0%and 74.7%of K,Na and Mg were effectively removed,respectively.Moreover,the softening temperature of low temperature ash from the washed sample was as high as 1450◦C,538◦C higher than the low temperature ash from the original sample;the base acid ratio and fouling index were improved from high slagging and fouling risk(1.7 and 90.8)of the original organic solid waste to low and medium risk(0.4 and 3.5),respectively.All these results signified the contributing effect of proposed semi-continuous water washing method on the combustion of agricultural organic solid waste.In a word,this study provided a promising method for fouling and slagging inhibition during the agricultural organic solid waste combustion.展开更多
基金the National Key R&D Program of China(No.2017YFB0602901)。
文摘Activated carbon(AC)has been widely used in the removal of SO_(2) from flue gas owing to its well-developed pore structure and abundant functional groups.Herein,the effect of alkali/alkaline earth metals on sulfur migration was investigated based on the dynamic adsorption and temperature programmed desorption experiment.The adsorption and desorption properties of six types of AC(three commercial and three laboratory-made)were carried out on a fixed-bed experimental device,and the physical and chemical properties of samples were determined by X-ray fluorescence,X-ray diffraction,scanning electron microscopy/energy dispersive X-ray,and X-ray photoelectron spectroscopy analysis.The experimental results showed that the adsorbed SO_(2) cannot be completely desorbed by increasing the regeneration temperature(350-850℃),while the SO_(2) fixed in the AC combines with the Ca-based minerals in the ash to form a stable sulfate.For different samples,higher ash content,higher CaO content in the ash and a more developed pore structure lead to a higher SO_(2) fixation rate.Moreover,the multiple adsorption-desorption cycles experiment showed that the effect of SO_(2) fixation is mainly reflected in the first cycle,after which the adsorption and desorption amount are approximately the same.This study elucidates the effect of alkali/alkaline earth metals on the adsorption-desorption cycle of AC,which provides a deeper understanding of sulfur migration in the AC flue gas desulfurization process.
基金supported by the National Natural Science Foundation of China (Nos. 21277008 and 20777005)the National Key Research and Development Program of China (No. 2017YFC0209905)。
文摘The Al-pillared montmorillonite-supported alkaline earth metal 5M/Al-PILC(PILC = pillared clay, M = Mg, Ca, Sr, and Ba) and x Mg/Al-PILC( x = 1, 3, 5, and 7 wt.%) samples were prepared using an impregnation method. Physical properties of the materials were determined by means of X-ray diffraction(XRD) and N2 adsorption-desorption, and their CO2 adsorption behaviors were investigated using the thermogravimetric analyzer(TG), CO2 temperatureprogrammed desorption(CO2-TPD), and in situ diffuse reflectance infrared transform spectroscopy(in situ-DRIFTS) techniques. It is shown that 5 Mg/Al-PILC possessed the highest CO2 adsorption capacity(2.559 mmol/g). The characterization results indicate that Alpillaring increased the specific surface area of montmorillonite, which was beneficial for the adsorption of CO2. The CO2 adsorption process on the sample was mainly chemical adsorption, and alkalinity was the main factor influencing its adsorption capacity. The alkalinity of the sample was enhanced by loading an appropriate amount of alkaline earth metal, and the adsorbed CO2 was present in the form of bicarbonate and carbonate. In addition, the 5Mg/Al-PILC sample exhibited an excellent regeneration efficiency. We believe that the outcome of this research would provide a good option for developing highly effective CO2 adsorption materials.
基金financial supports from the Project of the National Natural Science Foundation of China(Grant Nos.21633011and 21872137)“Transformational Technologies for Clean Energy and Demonstration”+2 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA21000000)Youth Innovation Promotion Association CAS(No.2018213)the Shanghai Synchrotron Radiation Facility(SSRF)for providing the beam time。
文摘Development of active and non-noble metal-based catalyst for H2 production via NH3 decomposition is crucial for the implementation of NH3 as a H2 carrier.Co-based catalysts have received increasing attention because of its high intrinsic activity and moderate cost.In this work,we examined the effect of BaNH,CaNH and Mg3 N2 on the catalytic activity of Co in the NH3 decomposition reaction.The H2 formation rate ranks the order as Co-BaNH>Co-CaNH>Co-Mg3 N2≈Co/CNTs within a reaction temperature range of 300-550℃.It is worth pointing out that the H2 formation rate of Co-BaNH at 500℃reaches20 mmolH2 gcat-1 min-1,which is comparable to those of the active Ru/Al2 O3(ca.17 mmolH2 gcat-1 min1)and Ru/AC(21 mmolH2 gcat-1 min-1)catalysts under the similar reaction conditions.In-depth research shows that Co-BaNH exhibits an obviously higher intrinsic activity and much lower Ea(46.2 kJ mol-1)than other Co-based catalysts,suggesting that BaNH may play a different role from CaNH,Mg3 N2 and CNTs during the catalytic process.Combined results of XRD,Ar-TPD and XAS show that a[Co-N-Ba]-like intermediate species is likely formed at the interface of Co metal and BaNH,which may lead to a more energy-efficient reaction pathway than that of neat Co metal for NH3 decomposition.
基金supported by the National Natural Science Foundation of China(Nos.21277008 and 20777005)the National Key Research and Development Program of China(No.2017YFC0209905)。
文摘To improve the removal capacity of NO + O_(2) effectively, the alkaline earth metal-doped order mesoporous carbon(A-C-FDU-15(0.001)(A = Mg, Ca, Sr and Ba)) and Mg-C-FDU-15( x)( x = 0.001-0.003) samples were prepared, and their physicochemical and NO + O_(2) adsorption properties were determined by means of various techniques. The results show that the sequence in(NO + O_(2)) adsorption performance was as follows: Mg-C-FDU-15(0.001)(93.2 mg/g) > Ca-C-FDU-15(0.001)(82.2 mg/g) > Sr-C-FDU-15(0.001)(76.1 mg/g) > Ba-C-FDU-15(0.001)(72.9 mg/g) > C-FDU-15(67.1 mg/g). Among all of the A-C-FDU-15(0.001) samples, Mg-C-FDU-15(0.001) possessed the highest(NO + O_(2)) adsorption capacity(106.2 mg/g). The species of alkaline earth metals and basic sites were important factors determining the adsorption of NO + O_(2) on the A-C-FDU-15( x) samples, and(NO + O_(2)) adsorption on the samples was mainly chemical adsorption. Combined with the results of(NO + O_(2))-temperatureprogrammed desorption((NO + O_(2))-TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS) characterization, we deduced that there were two main pathways of(NO + O_(2)) adsorption: one was first the conversion of NO and O_(2) to NO_(2) and then part of NO_(2) was converted to NO_(2)^(-) and NO_(3)^(-);and the other was the direct oxidation of NO to NO-2 and NO_(3)^(-).
基金the financial supports provided by the National Key Research and Development Program of China(2019YFC190252).
文摘Combustion of agricultural organic solid waste(AOSW)was an ideal solution for their resource utilization in view of their massive annual production and great potential for reduction of fossil fuel utilization.However,high alkali and alkaline earth metals(AAEMs)content in the feedstock can arose severe fouling and slagging issues and thus prohibiting its vast utilization.In this study,a semi-continuous water washing method was proposed to preliminarily remove AAEMs from agricultural organic solid waste and its effects on the combustion behaviors of washed solid product were investigated.Results showed that the combustion index S were improved to 2.63×10-6,over 68%of the total ashes were removed from the cotton stalk,and 96.3%,89.0%and 74.7%of K,Na and Mg were effectively removed,respectively.Moreover,the softening temperature of low temperature ash from the washed sample was as high as 1450◦C,538◦C higher than the low temperature ash from the original sample;the base acid ratio and fouling index were improved from high slagging and fouling risk(1.7 and 90.8)of the original organic solid waste to low and medium risk(0.4 and 3.5),respectively.All these results signified the contributing effect of proposed semi-continuous water washing method on the combustion of agricultural organic solid waste.In a word,this study provided a promising method for fouling and slagging inhibition during the agricultural organic solid waste combustion.
