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
The purpose of this study is to investigate the catalytic effects of alkali and alkaline earth metallic species （AAEM） on char conversion during the gasification in steam and the changes in ex-situ char reactivity i...The purpose of this study is to investigate the catalytic effects of alkali and alkaline earth metallic species （AAEM） on char conversion during the gasification in steam and the changes in ex-situ char reactivity in oxygen after the gasification in steam using different forms （i.e. H-form, Na-form） of Shengli brown coal. The surface area, AAEM concentration and carbon crystallite of chars were obtained to understand the change in char reactivity. It was found that not only Na concentration and carbon structure were the main factors governing the char reactivity in the atmosphere of steam and oxygen, but also they interacted each other. The presence of Na could facilitate the formation of disordering carbon structure in char, and the amorphous carbon structure would in turn affect the distribution of Na and thus its catalytic performance. The surface area and pore volume had very little relationship with the char＇s reactivity. Addi- tionally, the morphology of chars from different forms of coals were observed using scanning electron microscope （SEM）.展开更多
The effects of the constituents of mineral matter in brown coals from different deposits of Kansk-Achinsk, Lenaand from Yallourn Basins on the structural parameters and steam gasification reactivities of respective co...The effects of the constituents of mineral matter in brown coals from different deposits of Kansk-Achinsk, Lenaand from Yallourn Basins on the structural parameters and steam gasification reactivities of respective coal chars at moderate temperature and at low and high pressure were studied in this paper. The data on how the preliminary decationization with diluted hydrochloric, acetic and sulphuric acids affect char gasification reactivities are presented. The importance of surface area and crystallinity of chars and the presence of naturally occurring metals on gasification reactivity is considered. Quantitative correlations between the calcium contents and the extents of gasification are revealed. The gasification results obtained in a flow reactor with steam stream and in an autoclave reactor at high pressure of gaseous products are compared. The catalytic effect of dispersed calcium oxide-carbonate particles produced from the naturally occurring calcium containing carboxylates was shown to be a key factor for char gasification reactivity, the effect in the flow reactor being much larger as compared to that in the autoclave reactor. This was mainly related to different forms of catalytically active calcium species and to the composition of the gaseous reaction mixture.展开更多
The steam gasification kinetics of Zhundong raw coal and the washed coal by deionized water or hydrochloric acid with/without addition of CaO were tested by thermogravimetric analyzer(TGA)at medium temperatures(650℃ ...The steam gasification kinetics of Zhundong raw coal and the washed coal by deionized water or hydrochloric acid with/without addition of CaO were tested by thermogravimetric analyzer(TGA)at medium temperatures(650℃ to 800℃).The cation contents of potassium and sodium in samples were determined by Inductively Coupled Plasma Optical Emission Spectrometer(ICP-OES).The Brunauer-Emmett-Teller(BET)surface area of the samples was tested by N2 adsorption,and the morphologies of the samples were characterized by scanning electron microscopy(SEM).Experimental results showed that the organic sodium was the main catalyst for the gasification of the pyrolysis char,and the gasification rate of the char could be enhanced further with the introduction of CaO.The inherent alkali metals in coal and the introduced CaO showed a synergistic effect that occurred obviously above 735℃.The char conversion curves with or without CaO were fitted by the modified volumetric model(MVM).The calculated results indicated that the addition of CaO increased the pre-exponential factor obviously,but made little changes on the activation energy.It was proposed that the synergistic effect was resulted from the co-melting of the sodium and CaO,which facilitated the migration of the catalyst ions and the generation of C(O)intermediates for the gasification.展开更多
Catalytic steam gasification of fine coal char particles was carried out using a self-made laboratory reactor to determine the intrinsic kinetics and external diffusion under varying pressures (0.1-0.5 MPa) and superf...Catalytic steam gasification of fine coal char particles was carried out using a self-made laboratory reactor to determine the intrinsic kinetics and external diffusion under varying pressures (0.1-0.5 MPa) and superficial gas flow velocities (GF Vs) of 13.8- 68.8 cm· s^-1. In order to estimate the in-situ gas release rate at a low GFV, the transported effect of effluent gas on the temporal gasification rate pattern was simulated by the Fluent computation and verified experimentally. The external mass transfer coefficients(kmam) and the effectiveness factors were determined at lower GF Vs, based on the intrinsic gasification rate obtained at a high GFV of 55.0 cm·s^-1. The kmamwas found to be almost invariable in a wider carbon conversion of 0.2-0.7. The variations of kmam at a median carbon conversion with GFV, temperature and pressure were found to follow a modified Chilton-Colburn correlation:Sh=0.311Re^2.83Sc1/3(P/P0)^-2.07 (0.04<Re<0.19), where P is total pressure and Po is atmospheric pressure. An intrinsic kinetics/extemal diffusion integrating model could well describe the gasification rate as a function of GFV, temperature and pressure over a whole gasification process.展开更多
A new type of mixture fuel, sludge–oil–coal agglomerate (SOCA), was catalytically gasified with steam in a thermobalance reactor under atmospheric pressure. All the four catalysts studied (K2CO3, CaO, NiO and Fe2O3)...A new type of mixture fuel, sludge–oil–coal agglomerate (SOCA), was catalytically gasified with steam in a thermobalance reactor under atmospheric pressure. All the four catalysts studied (K2CO3, CaO, NiO and Fe2O3) were found capable of enhancing the steam gasification rate and significantly increasing the conversion of carbon. The ranking of catalytic activity was found to be K2CO3 CaO > NiO > Fe2O3. A modified volumetric-reaction model in the literature was used to describe the conversion behavior of the steam gasification studied by evaluating the kinetic parameters. Expressions of the apparent gasification rates for SOCA were presented for the design of catalytic gasification processes.展开更多
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The purpose of this study is to investigate the catalytic effects of alkali and alkaline earth metallic species （AAEM） on char conversion during the gasification in steam and the changes in ex-situ char reactivity in oxygen after the gasification in steam using different forms （i.e. H-form, Na-form） of Shengli brown coal. The surface area, AAEM concentration and carbon crystallite of chars were obtained to understand the change in char reactivity. It was found that not only Na concentration and carbon structure were the main factors governing the char reactivity in the atmosphere of steam and oxygen, but also they interacted each other. The presence of Na could facilitate the formation of disordering carbon structure in char, and the amorphous carbon structure would in turn affect the distribution of Na and thus its catalytic performance. The surface area and pore volume had very little relationship with the char＇s reactivity. Addi- tionally, the morphology of chars from different forms of coals were observed using scanning electron microscope （SEM）.
文摘The effects of the constituents of mineral matter in brown coals from different deposits of Kansk-Achinsk, Lenaand from Yallourn Basins on the structural parameters and steam gasification reactivities of respective coal chars at moderate temperature and at low and high pressure were studied in this paper. The data on how the preliminary decationization with diluted hydrochloric, acetic and sulphuric acids affect char gasification reactivities are presented. The importance of surface area and crystallinity of chars and the presence of naturally occurring metals on gasification reactivity is considered. Quantitative correlations between the calcium contents and the extents of gasification are revealed. The gasification results obtained in a flow reactor with steam stream and in an autoclave reactor at high pressure of gaseous products are compared. The catalytic effect of dispersed calcium oxide-carbonate particles produced from the naturally occurring calcium containing carboxylates was shown to be a key factor for char gasification reactivity, the effect in the flow reactor being much larger as compared to that in the autoclave reactor. This was mainly related to different forms of catalytically active calcium species and to the composition of the gaseous reaction mixture.
基金financially supported by the research project“Advancing and Demonstration of the Technology of CO2 Capture,Storage and Usage”(2016YFE0102500)National Natural Science Foundation of China(51606194)。
文摘The steam gasification kinetics of Zhundong raw coal and the washed coal by deionized water or hydrochloric acid with/without addition of CaO were tested by thermogravimetric analyzer(TGA)at medium temperatures(650℃ to 800℃).The cation contents of potassium and sodium in samples were determined by Inductively Coupled Plasma Optical Emission Spectrometer(ICP-OES).The Brunauer-Emmett-Teller(BET)surface area of the samples was tested by N2 adsorption,and the morphologies of the samples were characterized by scanning electron microscopy(SEM).Experimental results showed that the organic sodium was the main catalyst for the gasification of the pyrolysis char,and the gasification rate of the char could be enhanced further with the introduction of CaO.The inherent alkali metals in coal and the introduced CaO showed a synergistic effect that occurred obviously above 735℃.The char conversion curves with or without CaO were fitted by the modified volumetric model(MVM).The calculated results indicated that the addition of CaO increased the pre-exponential factor obviously,but made little changes on the activation energy.It was proposed that the synergistic effect was resulted from the co-melting of the sodium and CaO,which facilitated the migration of the catalyst ions and the generation of C(O)intermediates for the gasification.
基金the National Natural Science Foundation of China (Grand No.21376080).
文摘Catalytic steam gasification of fine coal char particles was carried out using a self-made laboratory reactor to determine the intrinsic kinetics and external diffusion under varying pressures (0.1-0.5 MPa) and superficial gas flow velocities (GF Vs) of 13.8- 68.8 cm· s^-1. In order to estimate the in-situ gas release rate at a low GFV, the transported effect of effluent gas on the temporal gasification rate pattern was simulated by the Fluent computation and verified experimentally. The external mass transfer coefficients(kmam) and the effectiveness factors were determined at lower GF Vs, based on the intrinsic gasification rate obtained at a high GFV of 55.0 cm·s^-1. The kmamwas found to be almost invariable in a wider carbon conversion of 0.2-0.7. The variations of kmam at a median carbon conversion with GFV, temperature and pressure were found to follow a modified Chilton-Colburn correlation:Sh=0.311Re^2.83Sc1/3(P/P0)^-2.07 (0.04<Re<0.19), where P is total pressure and Po is atmospheric pressure. An intrinsic kinetics/extemal diffusion integrating model could well describe the gasification rate as a function of GFV, temperature and pressure over a whole gasification process.
基金New and Renewable Technology Development Project (2005-N-WA02-P-02-3-010-2005) under MOCIE (Ministry of Commerce, Industryand Energy)New and Renewable Energy R&D Program (2006-N-CO12-P-03-3-050) under MOCIE+2 种基金Korea Research Foundation Grant funded by the Korean Government(MOEHRD) (KRF-2007-041-D0019)KESRI (R-2005-7-072), which is funded by MOCIEThe Specialized Graduate School Program from MKE (Ministry of Knowledge Economy)
文摘A new type of mixture fuel, sludge–oil–coal agglomerate (SOCA), was catalytically gasified with steam in a thermobalance reactor under atmospheric pressure. All the four catalysts studied (K2CO3, CaO, NiO and Fe2O3) were found capable of enhancing the steam gasification rate and significantly increasing the conversion of carbon. The ranking of catalytic activity was found to be K2CO3 CaO > NiO > Fe2O3. A modified volumetric-reaction model in the literature was used to describe the conversion behavior of the steam gasification studied by evaluating the kinetic parameters. Expressions of the apparent gasification rates for SOCA were presented for the design of catalytic gasification processes.
