CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressu...CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressure. When the coal was impregnated with an appropriate quantity of Ca and BL mixture, the catalytic activity of CO2 gasification was enhanced obviously. With a loading of 8%Na-BL+2%Ca, the carbon conversion of three coal samples tested reaches up to 92.9%-99.3% at 950℃ within 30min. The continuous formation of alkali surface compounds such as ([-COM], [-CO2M]) and the presence of exchanged Ca, such as calcium phenolate and calcium carboxylates (COO)2Ca, contribute to the increase in catalytic efficiency, and using BL+Ca is more efficient than that adding BL only, The homogeneous model and shrinking-core model were applied to correlate the data of conversion with time and to estimate the reaction rate constants under different temperature. The corresponding reaction activation energy (Ea) and pre-exponential factor of three anthracites were estimated. It is found that Ea is in the range from 73.6 to 121.4kJ·mol^-1 in the case of BL+Ca, and 74.3 to 104.2kJ·mol^-1 when only BL was used as the catalyst, both of which are much less than that from 143.5 to 181.4kJ·mol^-1 if no catalyst used. It is clearly demonstrated that both of BL+Ca mixture and BL could be the source of cheap and effective catalyst for coal gasification.展开更多
The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasificati...The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.展开更多
Catalytic coal gasification is an efficient way to achieve high conversion rates at low temperatures.Catalyst loss due to the reaction between the inherent mineral matter in the coal and the catalyst is a major hurdle...Catalytic coal gasification is an efficient way to achieve high conversion rates at low temperatures.Catalyst loss due to the reaction between the inherent mineral matter in the coal and the catalyst is a major hurdle for its practical application.The problem may be overcome by removing the mineral matter from the coal before use.Two demineralizing approaches,acid-washing and solvent-extraction methods are investigated for demineralizing the coals.Elemental analysis,XRD analysis,NMR analysis,and N_(2)adsorption analysis were made to compare the demineralization efficiency,crystallographic carbon microstructure,chemical structure,and micro-porosity,respectively.Solvent-extraction method was found be more efficient for demineralization.Difference was observed in the chemical structure and micro-porosity while crystallographic carbon-microstructure was found to be similar.Non-catalytic and catalytic gasification reactivity of the chars obtained by the two methods was compared.Gas composition and gas evolution profiles were also obtained and found to be influenced by the degree of demineralization.展开更多
Catalytic coal gasification for methane production is a promising technology in the clean coal utilization field.In this review,the technologies for coal-derived natural gas production,the catalytic coal gasification ...Catalytic coal gasification for methane production is a promising technology in the clean coal utilization field.In this review,the technologies for coal-derived natural gas production,the catalytic coal gasification processes and the used reactors were compared.The compared catalysts mainly included single-component,composite,and disposable catalysts.The effects of catalyst properties included composition,preparation method,supporter and loading amount were further illustrated.The influences of coal properties included char preparation method,particle size,and ash content on catalytic performance were investigated.The effects of temperatures and pressures on gasification performance were discussed in details.The evaporation,melting,decomposition,and inactivation of catalyst under various temperatures and pressures were also analyzed.It is expected to provide comprehensive information on the researches of catalytic coal gasification for methane production.展开更多
Various process residues represent a kind of biomass resource already concentrated but containing water as much as 60 wt.%. These materials are generally treated as waste or simply combusted directly to generate heat....Various process residues represent a kind of biomass resource already concentrated but containing water as much as 60 wt.%. These materials are generally treated as waste or simply combusted directly to generate heat. Recently, we attempted to convert them into middle caloric gas to substitute for natural gas, as a chemical or a high-rank gaseous fuel for advanced combustion utilities. Such conversion is implemented through dual fluidized bed gasification (DFBG). Concerning the high water content of the fuels, DFBG was suggested to accomplish either with high-efficiency fuel drying in advance or direct decoupling of fuel drying/pyrolysis from char gasification and tar/hydrocarbon reforming. Along with fuel drying, calcium-based catalyst can be impregnated into the fuel, without much additional cost, to increase the fuel's gasification reactivity and to reduce tar formation. This article reports the Ca impregnation method and its resulting effects on gasification reactivity and tar suppression ability. Meanwhile, the principle of directly gasifying wet fuel with decoupled dual fluidized bed gasification (D-DFBG) is also highlighted.展开更多
Red mud(RM)with the high alkalinity as a catalyst was evaluated for coal pyrolysis in a fixed bed as well as CO_(2) gasification of its resultant char in a thermogravimetric analyzer(TGA).The addition of RM into coal ...Red mud(RM)with the high alkalinity as a catalyst was evaluated for coal pyrolysis in a fixed bed as well as CO_(2) gasification of its resultant char in a thermogravimetric analyzer(TGA).The addition of RM into coal could improve the quality of tar during pyrolysis and enhance the reactivity of char during gasification.For catalytic pyrolysis with 12 wt%RM at 600℃,the light fraction in tar was 72.0 wt%,which increased by 20.0%,compared with coal pyrolysis alone.The role of metal oxides in RM on coal pyrolysis was further clarified as well.After catalytic pyrolysis with RM,the specific surface area of resultant char increased,especially for mesoporous surface area,and meanwhile the sodium in RM was proved to migrate to the char surface.These positive factors contributed to the CO_(2) gasification activity of char.RM with the high alkalinity showed a promising catalyst candidate for coal pyrolysis and gasification in terms of its catalytic effects and low cost.展开更多
基金Supported by the National Natural Science Foundation of China (No.20376014) and Fujian Science and Technology Council Grant (HG99-01).
文摘CO2 gasification of Fuijian high-metamorphous anthracite with black liquor (BL) and/or mixture of BL and calcium stuff (BL+Ca) as catalyst was studied by using a thermogravimetry under 750-950℃ at ambient pressure. When the coal was impregnated with an appropriate quantity of Ca and BL mixture, the catalytic activity of CO2 gasification was enhanced obviously. With a loading of 8%Na-BL+2%Ca, the carbon conversion of three coal samples tested reaches up to 92.9%-99.3% at 950℃ within 30min. The continuous formation of alkali surface compounds such as ([-COM], [-CO2M]) and the presence of exchanged Ca, such as calcium phenolate and calcium carboxylates (COO)2Ca, contribute to the increase in catalytic efficiency, and using BL+Ca is more efficient than that adding BL only, The homogeneous model and shrinking-core model were applied to correlate the data of conversion with time and to estimate the reaction rate constants under different temperature. The corresponding reaction activation energy (Ea) and pre-exponential factor of three anthracites were estimated. It is found that Ea is in the range from 73.6 to 121.4kJ·mol^-1 in the case of BL+Ca, and 74.3 to 104.2kJ·mol^-1 when only BL was used as the catalyst, both of which are much less than that from 143.5 to 181.4kJ·mol^-1 if no catalyst used. It is clearly demonstrated that both of BL+Ca mixture and BL could be the source of cheap and effective catalyst for coal gasification.
基金The present work was supported by the National Natural Science Foundation of China (21968024)the Project of Key Research Plan of Ningxia (2019BCH01001)The authors also gratefully thank Professor Junzhuo Fang for his help in taking SEM–EDS photos.
文摘The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.
文摘Catalytic coal gasification is an efficient way to achieve high conversion rates at low temperatures.Catalyst loss due to the reaction between the inherent mineral matter in the coal and the catalyst is a major hurdle for its practical application.The problem may be overcome by removing the mineral matter from the coal before use.Two demineralizing approaches,acid-washing and solvent-extraction methods are investigated for demineralizing the coals.Elemental analysis,XRD analysis,NMR analysis,and N_(2)adsorption analysis were made to compare the demineralization efficiency,crystallographic carbon microstructure,chemical structure,and micro-porosity,respectively.Solvent-extraction method was found be more efficient for demineralization.Difference was observed in the chemical structure and micro-porosity while crystallographic carbon-microstructure was found to be similar.Non-catalytic and catalytic gasification reactivity of the chars obtained by the two methods was compared.Gas composition and gas evolution profiles were also obtained and found to be influenced by the degree of demineralization.
基金financially supported by Shangrao Natural Science Foundation(No.2020L001)Natural Science Foundation of China(No.51976226)Science Foundation of North University of China(No.XJJ201923).
文摘Catalytic coal gasification for methane production is a promising technology in the clean coal utilization field.In this review,the technologies for coal-derived natural gas production,the catalytic coal gasification processes and the used reactors were compared.The compared catalysts mainly included single-component,composite,and disposable catalysts.The effects of catalyst properties included composition,preparation method,supporter and loading amount were further illustrated.The influences of coal properties included char preparation method,particle size,and ash content on catalytic performance were investigated.The effects of temperatures and pressures on gasification performance were discussed in details.The evaporation,melting,decomposition,and inactivation of catalyst under various temperatures and pressures were also analyzed.It is expected to provide comprehensive information on the researches of catalytic coal gasification for methane production.
基金The Natural Science Foundation of China(NSFC) financed the first period of research on the decoupled dual fluidized bed gasification(20606034,20776144)
文摘Various process residues represent a kind of biomass resource already concentrated but containing water as much as 60 wt.%. These materials are generally treated as waste or simply combusted directly to generate heat. Recently, we attempted to convert them into middle caloric gas to substitute for natural gas, as a chemical or a high-rank gaseous fuel for advanced combustion utilities. Such conversion is implemented through dual fluidized bed gasification (DFBG). Concerning the high water content of the fuels, DFBG was suggested to accomplish either with high-efficiency fuel drying in advance or direct decoupling of fuel drying/pyrolysis from char gasification and tar/hydrocarbon reforming. Along with fuel drying, calcium-based catalyst can be impregnated into the fuel, without much additional cost, to increase the fuel's gasification reactivity and to reduce tar formation. This article reports the Ca impregnation method and its resulting effects on gasification reactivity and tar suppression ability. Meanwhile, the principle of directly gasifying wet fuel with decoupled dual fluidized bed gasification (D-DFBG) is also highlighted.
基金financed by the National Key Research and Development Program of China(2016YFB0600304)the National Natural Science Foundation of China(21878310).
文摘Red mud(RM)with the high alkalinity as a catalyst was evaluated for coal pyrolysis in a fixed bed as well as CO_(2) gasification of its resultant char in a thermogravimetric analyzer(TGA).The addition of RM into coal could improve the quality of tar during pyrolysis and enhance the reactivity of char during gasification.For catalytic pyrolysis with 12 wt%RM at 600℃,the light fraction in tar was 72.0 wt%,which increased by 20.0%,compared with coal pyrolysis alone.The role of metal oxides in RM on coal pyrolysis was further clarified as well.After catalytic pyrolysis with RM,the specific surface area of resultant char increased,especially for mesoporous surface area,and meanwhile the sodium in RM was proved to migrate to the char surface.These positive factors contributed to the CO_(2) gasification activity of char.RM with the high alkalinity showed a promising catalyst candidate for coal pyrolysis and gasification in terms of its catalytic effects and low cost.