The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL（black liquor） catalysts and mixed 3%Ca＋5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation en...The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL（black liquor） catalysts and mixed 3%Ca＋5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation energy, relative amount of harmful pollutant like sulphur containing gases have been investigated by thermogravimetry in steam gasification under temperature 750℃ to 950℃ at ambient pressure for three high-metarnorphous anthracites （Longyan, Fenghai and Youxia coals in Fujian Province）. The mixed catalyst of 3%Ca＋5%Na-BL increases greatly the carbon conversion and gasification rate constant by accelerating the gasification reaction C＋H2O→CO＋H2 due to presence of alkali surfacecompounds [COM], [CO2M] and exchanged calcium phenolate and calcium carboxylate （-COO）2. By adding CaCO3 into BL catalyst in gasification, in addition to improving the catalyst function and enhancing the carbon conversion, the effective desulphurization is also achieved, but the better operating temperature should be below 900℃. The homogenous and shrinking core models can be successfully employed to correlate the relations between the conversion and the gasification .time .and to estimate the reaction rate constant, The reaction acUvaUon energy and pre-exponential factor are estimated and the activation energy for mixed catalyst is in a range of 98.72-166.92 kJ·mol^-1, much less than 177.50-196.46 kJ·mol^-1 for non-catalytic steam gasification for three experimental coals.展开更多
Underground coal gasification is one of the clean technologies of in-situ coal utilization.Hydrogen production from underground gasification of lignite was investigated in this study based on simulation experiments.Py...Underground coal gasification is one of the clean technologies of in-situ coal utilization.Hydrogen production from underground gasification of lignite was investigated in this study based on simulation experiments.Pyrolysis of lignite, gasification activity, oxygen-steam gasification and the effect of groundwater influx were studied.As well, the advantages of lignite for stable underground gasification were analyzed.The results indicate that lignite has a high activity for gasification.Coal pyrolysis is an important source of hydrogen emission.Under special heating conditions, hydrogen is released from coal seams at temperatures above 350 °C and reaches its maximum value between 725 and 825 °C.Gas with a hydrogen concentration of 40% to 50% can be continuously obtained by oxygen-steam injection at an optimum ratio of steam to oxygen, while lignite properties will ensure stable gasification.Groundwater influx can be utilized for hydrogen preparation under certain geological conditions through pressure control.Therefore, enhanced-hydrogen gas production through underground gasification of lignite has experimentally been proved.展开更多
The steam-gasification reaction characteristics of coal and petroleum coke （PC） were studied in the drop tube furnace （DTF）. The effects of various factors such as types of carbonaceous material, gasification temp...The steam-gasification reaction characteristics of coal and petroleum coke （PC） were studied in the drop tube furnace （DTF）. The effects of various factors such as types of carbonaceous material, gasification temperature （1100- 1400 ℃） and mass ratio of steam to char （0.4：1, 0.6：1 and 1：1 separately） on gasification gas or solid products were investigated. The results showed that for all carbonaceous materials studied, H2 content exhibited the largest part of gasification gaseous products and CH4 had the smallest part. For the two petroleum cokes, CO2 content was higher than CO, which was similar to Zun-yi char. When the steam/char ratio was constant, the carbon con- version of both Shen-fu and PC chars increased with increasing temperature. When the gasification temperature was constant, the carbon conversions of all char samples increased with increasing steam/char ratio. For all the steam/char ratios, compared to water gas shift reaction, char-H2O and char-CO2 reaction were further from the thermodynamic equilibrium due to a much lower char gasification rate than that of water gas shift reaction rate. Therefore, kinetic effects may play a more important role in a char gasification step than thermodynamic effects when the gasification reaction of char was held in DTF, The calculating method for the equilibrium shift in this study will be a worth reference for analysis of the gaseous components in industrial gasifier. The reactivity of residual cokes decreased and the crystal layer （L002/d002） numbers of residual cokes increased with increasing gasification temperature. Therefore, L002/d002, the carbon crystallite structure parameter, can be used to evaluate the reactivity of residual cokes.展开更多
基金Supported by the National Natural Science Foundation of China （20376014） and Fujian Science and Technology Council Grant （HG99-01 ）.
文摘The catalytic effects of single and mixed catalysts, i.e. single 3%Ca and 5%Na-BL（black liquor） catalysts and mixed 3%Ca＋5%Na-BL catalyst, on carbon conversion, gasification reaction rate constant and activation energy, relative amount of harmful pollutant like sulphur containing gases have been investigated by thermogravimetry in steam gasification under temperature 750℃ to 950℃ at ambient pressure for three high-metarnorphous anthracites （Longyan, Fenghai and Youxia coals in Fujian Province）. The mixed catalyst of 3%Ca＋5%Na-BL increases greatly the carbon conversion and gasification rate constant by accelerating the gasification reaction C＋H2O→CO＋H2 due to presence of alkali surfacecompounds [COM], [CO2M] and exchanged calcium phenolate and calcium carboxylate （-COO）2. By adding CaCO3 into BL catalyst in gasification, in addition to improving the catalyst function and enhancing the carbon conversion, the effective desulphurization is also achieved, but the better operating temperature should be below 900℃. The homogenous and shrinking core models can be successfully employed to correlate the relations between the conversion and the gasification .time .and to estimate the reaction rate constant, The reaction acUvaUon energy and pre-exponential factor are estimated and the activation energy for mixed catalyst is in a range of 98.72-166.92 kJ·mol^-1, much less than 177.50-196.46 kJ·mol^-1 for non-catalytic steam gasification for three experimental coals.
基金Projects 50876112 and 50674084 supported by the National Natural Science Foundation of China
文摘Underground coal gasification is one of the clean technologies of in-situ coal utilization.Hydrogen production from underground gasification of lignite was investigated in this study based on simulation experiments.Pyrolysis of lignite, gasification activity, oxygen-steam gasification and the effect of groundwater influx were studied.As well, the advantages of lignite for stable underground gasification were analyzed.The results indicate that lignite has a high activity for gasification.Coal pyrolysis is an important source of hydrogen emission.Under special heating conditions, hydrogen is released from coal seams at temperatures above 350 °C and reaches its maximum value between 725 and 825 °C.Gas with a hydrogen concentration of 40% to 50% can be continuously obtained by oxygen-steam injection at an optimum ratio of steam to oxygen, while lignite properties will ensure stable gasification.Groundwater influx can be utilized for hydrogen preparation under certain geological conditions through pressure control.Therefore, enhanced-hydrogen gas production through underground gasification of lignite has experimentally been proved.
基金Supported by the National High Technology Research and Development of China(2012AA053101,2011AA050106)the National Key State Basic Research Development Program of China(2010CB227004)the National Natural Science Foundation of China(21376081)
文摘The steam-gasification reaction characteristics of coal and petroleum coke （PC） were studied in the drop tube furnace （DTF）. The effects of various factors such as types of carbonaceous material, gasification temperature （1100- 1400 ℃） and mass ratio of steam to char （0.4：1, 0.6：1 and 1：1 separately） on gasification gas or solid products were investigated. The results showed that for all carbonaceous materials studied, H2 content exhibited the largest part of gasification gaseous products and CH4 had the smallest part. For the two petroleum cokes, CO2 content was higher than CO, which was similar to Zun-yi char. When the steam/char ratio was constant, the carbon con- version of both Shen-fu and PC chars increased with increasing temperature. When the gasification temperature was constant, the carbon conversions of all char samples increased with increasing steam/char ratio. For all the steam/char ratios, compared to water gas shift reaction, char-H2O and char-CO2 reaction were further from the thermodynamic equilibrium due to a much lower char gasification rate than that of water gas shift reaction rate. Therefore, kinetic effects may play a more important role in a char gasification step than thermodynamic effects when the gasification reaction of char was held in DTF, The calculating method for the equilibrium shift in this study will be a worth reference for analysis of the gaseous components in industrial gasifier. The reactivity of residual cokes decreased and the crystal layer （L002/d002） numbers of residual cokes increased with increasing gasification temperature. Therefore, L002/d002, the carbon crystallite structure parameter, can be used to evaluate the reactivity of residual cokes.
