Sulfur-containing pollutants are released during coal thermal conversion processes and must be controlled to satisfy the requirements of industrial production and protect the environments. This study investigated the release behaviors of sulfur species in Zhundong (ZD) coal during combustion and gasification. H2O-washed ZD coal and Shenmu (SM) coal were also investigated as reference samples to compare with ZD coal and to obtain general release properties. The experiments were carried out using online thermogravimetric analysis coupled with mass spectrometry. Theoretical calculation of the released gas was obtained by a novel method and equivalent characteristic spectrum analysis. The mass flow rate, the release proportion and the release temperature range of individual sulfur-containing pollutant were evaluated. The results show that water washing process did not change the combustion reactivity and the sulfur release temperature ranges of ZD coal, but the maximum gasification rate and the SO2 release rate were decreased. H2S, COS and SO2 were observed in gasification of the coals, while COS and SO2 were observed in combustion. SO2 was always the main sulfur-containing gaseous product in both combustion and gasification. Some sulfur starts to release as SO2 at high temperature (at about 1000 °C for ZD coal and H2O-washed ZD coal, and at about 1100 °C for SM coal) due to the decomposition of sulfate, at which temperature carbon had already burned out in combustion, and the coal conversion in gasification reached about 90%. With combustion temperature lower than 1000 °C, the release of SO2 from ZD coal, H2O-washed ZD coal and SM coal can be decreased by 46.14%, 38.95% and 4.36%, respectively. With gasification temperature lower than 1000 °C, few SO2 from ZD coal and H2O-washed ZD coal and SM coal can be released. It was observed that the releases of sulfur species were related to their occurrence, reaction evolution, temperature and atmosphere. Controlling the temperature is helpful in reducing the release of SO2 in both combustion and gasification. This work also shows that it is possible to achieve high carbon conversion of ZD coal gasification at a moderate temperature and simultaneously reduce the release of sulfur.
This is a preview of subscription content, log in to check access.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Hook M, Tang X. Depletion of fossil fuels and anthropogenic climate change—a review. Energy Policy. 2013;52:797–809. https://doi.org/10.1016/j.enpol.2012.10.046.
Frigge L, Stroehle J, Epple B. Release of sulfur and chlorine gas species during coal combustion and pyrolysis in an entrained flow reactor. Fuel. 2017;201:105–10. https://doi.org/10.1016/j.fuel.2016.11.037.
Wang Z, Li Q, Lin Z, Whiddon R, Qiu K, Kuang M, et al. Transformation of nitrogen and sulphur impurities during hydrothermal upgrading of low quality coals. Fuel. 2016;164:254–61. https://doi.org/10.1016/j.fuel.2015.10.015.
Blaesing M, Melchior T, Mueller M. Influence of temperature on the release of inorganic species during high temperature gasification of Rhenish lignite. Fuel Process Technol. 2011;92(3):511–6. https://doi.org/10.1016/j.fuproc.2010.11.005.
Krishnamoorthy V, Pisupati SV. Fate of sulfur during entrained-flow gasification of Pittsburgh no. 8 coal: influence of particle size, sulfur forms, and temperature. Energy Fuels. 2016;30(4):3241–50. https://doi.org/10.1021/acs.energyfuels.5b02691.
Zhang HX, Zhang YK, Zhu ZP, Lu QG. Circulating fluidized bed gasification of low rank coal: influence of O2/C molar ratio on gasification performance and sulphur transformation. J Therm Sci. 2016;25(4):363–71. https://doi.org/10.1007/s11630-016-0872-9.
Li Y, Lin Y, Xu Z, Wang B, Zhu T. Oxidation mechanisms of H2S by oxygen and oxygen-containing functional groups on activated carbon. Fuel Process Technol. 2019;189:110–9. https://doi.org/10.1016/j.fuproc.2019.03.006.
Chu X, Li W, Li B, Chen H. Sulfur transfers from pyrolysis and gasification of direct liquefaction residue of Shenhua coal. Fuel. 2008;87(2):211–5.
Duan Y, Duan L, Wang J, Anthony EJ. Observation of simultaneously low CO, NOx and SO2 emission during oxy-coal combustion in a pressurized fluidized bed. Fuel. 2019;242:374–81. https://doi.org/10.1016/j.fuel.2019.01.048.
Chen L, Wang C, Yan G, Zhao F, Anthony EJ. The simultaneous calcination/sulfation reaction of limestone under oxy-fuel CFB conditions. Fuel. 2019;237:812–22. https://doi.org/10.1016/j.fuel.2018.10.060.
Fang P, Gong Z, Wang Z, Wang Z, Meng F. Study on combustion and emission characteristics of microalgae and its extraction residue with TG-MS. Renew Energy. 2019;140:884–94. https://doi.org/10.1016/j.renene.2019.03.114.
Rodilla I, Contreras ML, Bahillo A. Thermogravimetric and mass spectrometric (TG-MS) analysis of sub-bituminous coal-energy crops blends in N2, air and CO2/O2 atmospheres. Fuel. 2018;215:506–14. https://doi.org/10.1016/j.fuel.2017.09.102.
Guo H, Wu H, Yang N, Fu Q, Liu F, Zhang H, et al. XAS combined with TG–DTG study on synergic effect on sulfur transformation during co-pyrolysis of sawdust and lignite. J Therm Anal Calorim. 2019;135(4):2475–80. https://doi.org/10.1007/s10973-018-7259-y.
Zhao B, Jin J, Li S, Liu D, Zhang R, Yang H. Co-pyrolysis characteristics of sludge mixed with Zhundong coal and sulphur contaminant release regularity. J Therm Anal Calorim. 2019. https://doi.org/10.1007/s10973-019-08300-x.
Cheng H, Liu Q, Zhang S, Wang S, Frost RL. Evolved gas analysis of coal-derived pyrite/marcasite. J Therm Anal Calorim. 2014;116(2):887–94. https://doi.org/10.1007/s10973-013-3595-0.
Zhou J, Zhuang X, Alastuey A, Querol X, Li J. Geochemistry and mineralogy of coal in the recently explored Zhundong large coal field in the Junggar basin, Xinjiang province, China. Int J Coal Geol. 2010;82(1–2):51–67. https://doi.org/10.1016/j.coal.2009.12.015.
Wang X, Xu Z, Wei B, Zhang L, Tan H, Yang T, et al. The ash deposition mechanism in boilers burning Zhundong coal with high contents of sodium and calcium: a study from ash evaporating to condensing. Appl Therm Eng. 2015;80:150–9. https://doi.org/10.1016/j.applthermaleng.2015.01.051.
Qi X, Song G, Song W, Yang S, Lu Q. Combustion performance and slagging characteristics during co-combustion of Zhundong coal and sludge. J Energy Inst. 2018;91(3):397–410. https://doi.org/10.1016/j.joei.2017.02.002.
Zhang H, Guo X, Zhu Z. Effect of temperature on gasification performance and sodium transformation of Zhundong coal. Fuel. 2017;189:301–11. https://doi.org/10.1016/j.fuel.2016.10.097.
Guo X, Zhang H, Zhu Z. The effect of O2/C ratio on gasification performance and sodium transformation of Zhundong coal. Fuel Process Technol. 2019;193:31–8. https://doi.org/10.1016/j.fuproc.2019.04.015.
Gao Q, Li S, Yuan Y, Zhang Y, Yao Q. Ultrafine particulate matter formation in the early stage of pulverized coal combustion of high-sodium lignite. Fuel. 2015;158:224–31. https://doi.org/10.1016/j.fuel.2015.05.028.
Liu Y, Cheng L, Zhao Y, Ji J, Wang Q, Luo Z, et al. Transformation behavior of alkali metals in high-alkali coals. Fuel Process Technol. 2018;169:288–94. https://doi.org/10.1016/j.fuproc.2017.09.013.
Ruan R, Tan H, Wang X, Li Y, Hu Z, Wei B, et al. Characteristics of fine particulate matter formation during combustion of lignite riched in AAEM (alkali and alkaline earth metals) and sulfur. Fuel. 2018;211:206–13. https://doi.org/10.1016/j.fuel.2017.08.114.
Lyu Q, Yu K, Liu W, Sun Y, Zhang H, Sun Y et al. Development and operation of large scale circulating fluidized bed coal gasification. In: Proceedings of the 12th international conference on fluidized bed technology. 2017 825–30.
Huang Q, Wei K, Xia H. A novel perspective of dolomite decomposition: elementary reactions analysis by thermogravimetric mass spectrometry. Thermochim Acta. 2019;676:47–51. https://doi.org/10.1016/j.tca.2019.03.042.
Li R, Chen Q, Xia H. Study on pyrolysis characteristics of pretreated highsodium (Na) Zhundong coal by skimmer-type interfaced TG-DTA-EI/PI-MS system. Fuel Process Technol. 2018;170:79–87. https://doi.org/10.1016/j.fuproc.2017.10.023.
Xia H, Wei K. Equivalent characteristic spectrum analysis in TG-MS system. Thermochim Acta. 2015;602:15–21. https://doi.org/10.1016/j.tca.2014.12.019.
Duan Y, Duan L, Anthony EJ, Zhao C. Nitrogen and sulfur conversion during pressurized pyrolysis under CO2 atmosphere in fluidized bed. Fuel. 2017;189:98–106. https://doi.org/10.1016/j.fuel.2016.10.080.
Song G, Song W, Qi X, Lu Q. Transformation characteristics of sodium of Zhundong coal combustion/gasification in circulating fluidized bed. Energy Fuels. 2016;30(4):3473–8. https://doi.org/10.1021/acs.energyfuels.6b00028.
Yan J, Yang J, Liu Z. SH radical: the key intermediate in sulfur transformation during thermal processing of coal. Environ Sci Technol. 2005;39(13):5043–51. https://doi.org/10.1021/es048398c.
Zhang Y, Wang M, Qin Z, Yang Y, Fu C, Feng L, et al. Effect of the interactions between volatiles and char on sulfur transformation during brown coal upgrade by pyrolysis. Fuel. 2013;103:915–22. https://doi.org/10.1016/j.fuel.2012.09.061.
Wang X, Guo H, Liu F, Hua R, Wang M. Effects of CO2 on sulfur removal and its release behavior during coal pyrolysis. Fuel. 2016;165:484–9. https://doi.org/10.1016/j.fuel.2015.10.047.
Jia X, Wang QH, Cen KF, Chen LM. An experimental study of CaSO4 decomposition during coal pyrolysis. Fuel. 2016;163:157–65. https://doi.org/10.1016/j.fuel.2015.09.054.
This work was financially supported by the National Key Research and Development Program of China (No. 2017YFB0602302) and the Beijing Municipal Science and Technology Commission (No. Z181100005118006).
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Zhang, H., Xian, S., Zhu, Z. et al. Release behaviors of sulfur-containing pollutants during combustion and gasification of coals by TG-MS. J Therm Anal Calorim 143, 377–386 (2021). https://doi.org/10.1007/s10973-019-09251-z
- Release behavior