A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface...A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface chemistry were carried out with the aim to improve the benzene adsorption capacity of activated carbon. The influences of KOH and activation process parameters including activation temperature, activation time and steam flow rate on porosity of activated carbon were evaluated, and the effect of modification methods on surface chemistry was investigated. Also, the relationship between benzene adsorption capacity and porosity and surface chemistry was analyzed. Results show that activation temperature is the dominant factor in the activation process; the introduction of KOH into the raw material can enhance the reactivity of char in activation process, meanwhile it shows a negative effect on the porosity development, especially on the mesopore development. Results of FTIR analysis indicate that anthracite-based activated carbon with condensed aromatics and chemically inert oxygen does not present the nature to be surface modified. Besides, benzene adsorption capacity has an approximate linear relationship with surface area and in our preparation, benzene adsorption capacity and surface area of activated carbon are up to 1210 m 2 /g and 423 mg/g, respectively.展开更多
Alkaline hydrazine liquid fuel cells(AHFC) have been highlighted in terms of high power performance with non-precious metal catalysts.Although Fe-N-C is a promising non-Pt electrocatalyst for oxygen reduction reaction...Alkaline hydrazine liquid fuel cells(AHFC) have been highlighted in terms of high power performance with non-precious metal catalysts.Although Fe-N-C is a promising non-Pt electrocatalyst for oxygen reduction reaction(ORR),the surface density of the active site is very low and the catalyst layer should be thick to acquire the necessary number of catalytic active sites.With this thick catalyst layer,it is important to have an optimum pore structure for effective reactant conveyance to active sites and an interface structure for faster charge transfer.Herein,we prepare a Fe-N-C catalyst with magnetite particles and hierarchical pore structure by steam activation.The steam activation process significantly improves the power performance of the AHFC as indicated by the lower IR and activation voltage losses.Based on a systematic characterization,we found that hierarchical pore structures improve the catalyst utilization efficiency of the AHFCs,and magnetite nanoparticles act as surface modifiers to reduce the interracial resistance between the electrode and the ion-exchange membrane.展开更多
The poor-reactivity anthracite urgently needs more ways for large-scale and high-quality utilization.Due to the advantage of good fuel adaptability,the circulating fluidized bed(CFB)gasification technology has the pot...The poor-reactivity anthracite urgently needs more ways for large-scale and high-quality utilization.Due to the advantage of good fuel adaptability,the circulating fluidized bed(CFB)gasification technology has the potential of high-quality utilization of anthracite.In this paper,one kind of anthracite from Shanxi province,China,was employed to be gasified in a pilot-scale CFB gasifier.It is found that at the operating temperature of 1049℃and oxygen concentration of 60.75%,the gas with a concentration of combustibles of 66%and a low heating value of 7.93 MJ/m^(3)(at about 25℃and 101.325 kPa)was produced in the CFB gasification process.However,the overall gasification efficiency was not desired because a large amount of gasification fly ash(GFA)escaped and its yield was up to 22%.In this case,the cold gas efficiency was below 48%and the carbon conversion ratio was only 62%.Further analysis reveals that the GFA was featured with a developed pore structure and the specific surface area(S_(BET))reached 277 m^(2)/g.This indicates such GFA has a potential to use as activated carbon(AC)or AC precursor.Basis on this,steam activation experiments of the GFA produced were conducted to investigate the activation characteristics of GFA and thereby to determine its activation potential.Experimental results indicate that increasing temperature sharply accelerated the activation process,while did not impair the maximum activation effect.After activation,the S_(BET)of GFA maximumly increased by 63%,reaching452 m^(2)/g.With the progress of activation,the pore structure of GFA presents a three-stage evolution process:development,dynamic balance,and collapse.Such a process can be divided and quantified according to the carbon loss.In order to achieve an optimal activation of GFA,the carbon loss shall be controlled at~15%.This work provides a new scheme for high-quality utilization of anthracite.展开更多
Coal gasification fly ash(CGFA)is an industrial solid waste from the coal circulating fluidized bed(CFB)gasification process,and it needs to be effectively disposed to achieve sustainable development of the environmen...Coal gasification fly ash(CGFA)is an industrial solid waste from the coal circulating fluidized bed(CFB)gasification process,and it needs to be effectively disposed to achieve sustainable development of the environment.To realize the application of CGFA as a precursor of porous carbon materials,the physicochemical properties of three kinds of CGFA from industrial CFB gasifiers are analyzed.Then,the activation potential of CGFA is acquired via steam activation experiments in a tube furnace reactor.Finally,the fluidization activation technology of CGFA is practiced in a bench-scale CFB test rig,and its advantages are highlighted.The results show that CGFA is characterized by a high carbon content in the range of 54.06%–74.09%,an ultrafine particle size(d50:16.3–26.1 μm),and a relatively developed pore structure(specific surface area SSA:139.29–551.97 m^(2)·g^(-1)).The proportion of micropores in CGFA increases gradually with the coal rank.Steam activation experiments show that the pore development of CGFA mainly includes three stages:initial pore development,dynamic equilibrium between micropores and mesopores and pore collapse.The SSA of lignite fly ash(LFA),subbituminous fly ash(SBFA)and anthracite fly ash(AFA)is maximally increased by 105%,13%and 72%after steam activation;the order of the largest carbon reaction rate and decomposition ratio of steam among the three kinds of CGFA is SBFA>LFA>AFA.As the ratio of oxygen to carbon during the fluidization activation of LFA is from 0.09 to 0.19,the carbon conversion ratio increases from 14.4%to 26.8%and the cold gas efficiency increases from 6.8%to 10.2%.The SSA of LFA increases by up to 53.9%during the fluidization activation process,which is mainly due to the mesoporous development.Relative to steam activation in a tube furnace reactor,fluidization activation takes an extremely short time(seconds)to achieve the same activation effect.It is expected to further improve the activation effect of LFA by regulating the carbon conversion ratio range of 27%–35%to create pores in the initial development stage.展开更多
Oil-palm shell wastes were successfully converted into useful activated carbons in a systematic and novel approach by optimizing the pyrolysis conditions and subsequent steam activation conditions to maximize the BET ...Oil-palm shell wastes were successfully converted into useful activated carbons in a systematic and novel approach by optimizing the pyrolysis conditions and subsequent steam activation conditions to maximize the BET surface area.The optimal activation conditions were a steam flow rate of 1.13 kg/h,hold time of 1.5 h and temperature of 950℃,yielding BET areas of 1432.94 and 1382.95 m^(2)/g for nitrogen-pyrolyzed and vacuumpyrolyzed chars,respectively.In steam-chemical activation,one-step activation of oil-palm shell in steam with potassium carbonate(K_(2)CO_(3)),sodium carbonate(Na_(2)CO_(3))or potassium chloride(KCl)was conducted,resulting in BET area output order of shell/K_(2)CO_(3)(710.56 m^(2)/g)>shell/KCl(498.55 m^(2)/g)>shell(366.7 m^(2)/g)>shell/Na_(2)CO_(3)(326.62 m^(2)/g).This study reported the first use of KCl and Na_(2)CO_(3)as chemical reagents in one-step steam-chemical activation of biomass.KCl-activated carbon exhibited retardation of tar formation property,resulting in better pore development than pure steam activated carbon.Phenol adsorption of activated carbon is not only a function of the BET surface area but also the type of pyrolysis used prior to physical activation.Activated carbon(BET area of 1192.29 m^(2)/g)pyrolyzed under vacuum could adsorb 87%more phenol than that pyrolyzed in nitrogen flow which had a higher BET area of 1432.94 m^(2)/g.Phenol adsorption capacities of activated carbons are:shell pyrolyzed under vacuum(275.5 mg/g)>shell pyrolyzed in N_(2)flow(147.1 mg/g)>shell/K_(2)CO_(3)(145.7 mg/g)>shell without pyrolysis(12.1 mg/g).These activated carbons would be highly suitable in industry processes to remove phenolic contaminants.展开更多
基金the financial support by the Special Fund for Basic Scientific Research of Central Colleges (No.2009KH10)the Beijing Postdoctoral Fund (No. B148)the Green Shoots Plan of Beijing Academy of Science and Technology of China (No. B142)
文摘A series of activated carbons from Taixi anthracite were prepared by steam activation in the presence of KOH and then they were modified by different methods. The regulation of porosity and the modification of surface chemistry were carried out with the aim to improve the benzene adsorption capacity of activated carbon. The influences of KOH and activation process parameters including activation temperature, activation time and steam flow rate on porosity of activated carbon were evaluated, and the effect of modification methods on surface chemistry was investigated. Also, the relationship between benzene adsorption capacity and porosity and surface chemistry was analyzed. Results show that activation temperature is the dominant factor in the activation process; the introduction of KOH into the raw material can enhance the reactivity of char in activation process, meanwhile it shows a negative effect on the porosity development, especially on the mesopore development. Results of FTIR analysis indicate that anthracite-based activated carbon with condensed aromatics and chemically inert oxygen does not present the nature to be surface modified. Besides, benzene adsorption capacity has an approximate linear relationship with surface area and in our preparation, benzene adsorption capacity and surface area of activated carbon are up to 1210 m 2 /g and 423 mg/g, respectively.
基金supported by the GIST Research Institute(GRI)grant funded by GIST in 2021supported by the KBSI grants(C140140 and C140110)。
文摘Alkaline hydrazine liquid fuel cells(AHFC) have been highlighted in terms of high power performance with non-precious metal catalysts.Although Fe-N-C is a promising non-Pt electrocatalyst for oxygen reduction reaction(ORR),the surface density of the active site is very low and the catalyst layer should be thick to acquire the necessary number of catalytic active sites.With this thick catalyst layer,it is important to have an optimum pore structure for effective reactant conveyance to active sites and an interface structure for faster charge transfer.Herein,we prepare a Fe-N-C catalyst with magnetite particles and hierarchical pore structure by steam activation.The steam activation process significantly improves the power performance of the AHFC as indicated by the lower IR and activation voltage losses.Based on a systematic characterization,we found that hierarchical pore structures improve the catalyst utilization efficiency of the AHFCs,and magnetite nanoparticles act as surface modifiers to reduce the interracial resistance between the electrode and the ion-exchange membrane.
基金financially supported by the Special Research Assistant Project,Chinese Academy of Sciences。
文摘The poor-reactivity anthracite urgently needs more ways for large-scale and high-quality utilization.Due to the advantage of good fuel adaptability,the circulating fluidized bed(CFB)gasification technology has the potential of high-quality utilization of anthracite.In this paper,one kind of anthracite from Shanxi province,China,was employed to be gasified in a pilot-scale CFB gasifier.It is found that at the operating temperature of 1049℃and oxygen concentration of 60.75%,the gas with a concentration of combustibles of 66%and a low heating value of 7.93 MJ/m^(3)(at about 25℃and 101.325 kPa)was produced in the CFB gasification process.However,the overall gasification efficiency was not desired because a large amount of gasification fly ash(GFA)escaped and its yield was up to 22%.In this case,the cold gas efficiency was below 48%and the carbon conversion ratio was only 62%.Further analysis reveals that the GFA was featured with a developed pore structure and the specific surface area(S_(BET))reached 277 m^(2)/g.This indicates such GFA has a potential to use as activated carbon(AC)or AC precursor.Basis on this,steam activation experiments of the GFA produced were conducted to investigate the activation characteristics of GFA and thereby to determine its activation potential.Experimental results indicate that increasing temperature sharply accelerated the activation process,while did not impair the maximum activation effect.After activation,the S_(BET)of GFA maximumly increased by 63%,reaching452 m^(2)/g.With the progress of activation,the pore structure of GFA presents a three-stage evolution process:development,dynamic balance,and collapse.Such a process can be divided and quantified according to the carbon loss.In order to achieve an optimal activation of GFA,the carbon loss shall be controlled at~15%.This work provides a new scheme for high-quality utilization of anthracite.
基金financially supported by the Special Research Assistant Fund Project of Chinese Academy of Sciences.
文摘Coal gasification fly ash(CGFA)is an industrial solid waste from the coal circulating fluidized bed(CFB)gasification process,and it needs to be effectively disposed to achieve sustainable development of the environment.To realize the application of CGFA as a precursor of porous carbon materials,the physicochemical properties of three kinds of CGFA from industrial CFB gasifiers are analyzed.Then,the activation potential of CGFA is acquired via steam activation experiments in a tube furnace reactor.Finally,the fluidization activation technology of CGFA is practiced in a bench-scale CFB test rig,and its advantages are highlighted.The results show that CGFA is characterized by a high carbon content in the range of 54.06%–74.09%,an ultrafine particle size(d50:16.3–26.1 μm),and a relatively developed pore structure(specific surface area SSA:139.29–551.97 m^(2)·g^(-1)).The proportion of micropores in CGFA increases gradually with the coal rank.Steam activation experiments show that the pore development of CGFA mainly includes three stages:initial pore development,dynamic equilibrium between micropores and mesopores and pore collapse.The SSA of lignite fly ash(LFA),subbituminous fly ash(SBFA)and anthracite fly ash(AFA)is maximally increased by 105%,13%and 72%after steam activation;the order of the largest carbon reaction rate and decomposition ratio of steam among the three kinds of CGFA is SBFA>LFA>AFA.As the ratio of oxygen to carbon during the fluidization activation of LFA is from 0.09 to 0.19,the carbon conversion ratio increases from 14.4%to 26.8%and the cold gas efficiency increases from 6.8%to 10.2%.The SSA of LFA increases by up to 53.9%during the fluidization activation process,which is mainly due to the mesoporous development.Relative to steam activation in a tube furnace reactor,fluidization activation takes an extremely short time(seconds)to achieve the same activation effect.It is expected to further improve the activation effect of LFA by regulating the carbon conversion ratio range of 27%–35%to create pores in the initial development stage.
文摘Oil-palm shell wastes were successfully converted into useful activated carbons in a systematic and novel approach by optimizing the pyrolysis conditions and subsequent steam activation conditions to maximize the BET surface area.The optimal activation conditions were a steam flow rate of 1.13 kg/h,hold time of 1.5 h and temperature of 950℃,yielding BET areas of 1432.94 and 1382.95 m^(2)/g for nitrogen-pyrolyzed and vacuumpyrolyzed chars,respectively.In steam-chemical activation,one-step activation of oil-palm shell in steam with potassium carbonate(K_(2)CO_(3)),sodium carbonate(Na_(2)CO_(3))or potassium chloride(KCl)was conducted,resulting in BET area output order of shell/K_(2)CO_(3)(710.56 m^(2)/g)>shell/KCl(498.55 m^(2)/g)>shell(366.7 m^(2)/g)>shell/Na_(2)CO_(3)(326.62 m^(2)/g).This study reported the first use of KCl and Na_(2)CO_(3)as chemical reagents in one-step steam-chemical activation of biomass.KCl-activated carbon exhibited retardation of tar formation property,resulting in better pore development than pure steam activated carbon.Phenol adsorption of activated carbon is not only a function of the BET surface area but also the type of pyrolysis used prior to physical activation.Activated carbon(BET area of 1192.29 m^(2)/g)pyrolyzed under vacuum could adsorb 87%more phenol than that pyrolyzed in nitrogen flow which had a higher BET area of 1432.94 m^(2)/g.Phenol adsorption capacities of activated carbons are:shell pyrolyzed under vacuum(275.5 mg/g)>shell pyrolyzed in N_(2)flow(147.1 mg/g)>shell/K_(2)CO_(3)(145.7 mg/g)>shell without pyrolysis(12.1 mg/g).These activated carbons would be highly suitable in industry processes to remove phenolic contaminants.