Effects of oxygen on the structure and reactivity of char during steam gasification of Shengli brown coal
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摘要: 为了研究氧气对半焦的结构变化和反应性的影响,采用不锈钢模拟气流床反应器,在8种不同气氛,800和900 ℃条件下,进行了胜利褐煤水蒸气气化实验。利用拉曼光谱和热重分析仪分别表征了半焦的结构和本征反应性。结果表明,在800和900 ℃条件下,添加的氧气对半焦结构变化的影响方式不同;半焦结构的变化是影响碱金属和碱土金属(AAEM)挥发的主要因素。在不同温度下,添加的氧气对Na挥发的影响和对结构的作用类似,H2O/O2混合气氛促使气化所得半焦的反应性进一步降低。半焦的反应活性指数与拉曼光谱谱带比值 I (GR+VL+VR)/ID具有很好的相关性。Abstract: The effects of oxygen on changes in char structure and reactivity during steam gasification of Shengli brown coal were examined. A stainless steel simulated entrained-flow reactor was employed to carry out gasification at 800 and 900 ℃ in 8 atmospheres: pure N2, 15% H2O, 25%H2O and 35%H2O balanced with N2; and 1%O2, 15%H2O+1%O2, 25%H2O+1%O2 and 35%H2O+1% O2 balanced with N2. The structure of chars was measured by Raman spectrum, and the intrinsic reactivity of chars with air was measured using a thermogravimetric analyzer (TGA) at low temperature (300 ℃). The results show that the effects of oxygen on char structure are different at high temperature (900 ℃) and low temperature (800 ℃) in brown coal steam gasification. The volatilization of alkali and alkaline earth metallic (AAEM) is strongly influenced by char structure. The presence of O2 during steam gasification has a similar effect on the volatilization of Na to the evolution of structure at different temperatures. Experimental data provided evidence that a mixed H2O/O2 atmosphere could promote a decrease in subsequent char reactivity in air at 300 ℃, and that char reactivity could correlate well with the band area ratio, I(GR+VL+VR)/ID.
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Key words:
- brown coal /
- gasification /
- char structure /
- char reactivity /
- simulated entrained-flow reactor
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TREMEL A, SPLIETHOFF H. Gasification kinetics during entrained flow gasification-Part I: Devolatilisation and char deactivation[J]. Fuel, 2013, 103: 663-671. QUYN D M, WU H W, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part I. Volatilisation of Na and Cl from a set of NaCl-loaded samples[J]. Fuel, 2002, 81(2): 143-149. TAY H L, KAJITANI S, ZHANG S, LI C Z. Effects of gasifying agent on the evolution of char structure during the gasification of Victorian brown coal[J]. Fuel, 2013, 103: 22-28. BAYARSAIKHAN B, SONOYAMA N, HOSOKAI S, SHIMADA T, HAYASHI J I, LI C Z, CHIBA T. Inhibition of steam gasification of char by volatiles in a fluidized bed under continuous feeding of a brown coal[J]. Fuel, 2006, 85(3): 340-349. ZHANG L X, MATSUHARA T, KUDO S, HAYASHI J I, NORINAGA K. Rapid pyrolysis of brown coal in a drop-tube reactor with co-feeding of char as a promoter of in situ tar reforming[J]. Fuel, 2013, 112: 681-686. YE D P, AGNEW J B, ZHANG D K. Gasification of a south Australian low-rank coal with carbon dioxide and steam: Kinetics and reactivity studies[J]. Fuel, 1998, 77(11): 1209-1219. ZHANG S, MIN Z H, TAY H L, ASADULLAH M, LI C Z. Effects of volatile-char interactions on the evolution of char structure during the gasification of Victorian brown coal in steam[J]. Fuel, 2011, 90(4): 1529-1535. LI C Z. Importance of volatile-char interactions during the pyrolysis and gasification of low-rank fuels-A review[J]. Fuel, 2013, 112: 609-623. WU H W, LI X J, HAYASHI J I, CHIBA T, LI C Z. Effects of volatile-char interactions on the reactivity of chars from NaCl-loaded Loy Yang brown coal[J]. Fuel, 2005, 84(10): 1221-1228. KAJITANI S, TAY H L, ZHANG S, LI C Z. Mechanisms and kinetic modelling of steam gasification of brown coal in the presence of volatile-char interactions[J]. Fuel, 2013, 103: 7-13. WU H W, QUYN D M, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part III. The importance of the interactions between volatiles and char at high temperature[J]. Fuel, 2002, 81(8): 1033-1039. LI X J, WU H W, HAYASHI J I, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part VI. Further investigation into the effects of volatile-char interactions[J]. Fuel, 2004, 83(10): 1273-1279. ZHANG S, HAYASHI J I, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part IX. Effects of volatile-char interactions on char-H2O and char-O2 reactivities[J]. Fuel, 2011, 90(4): 1655-1661. TAY H L, LI C Z. Changes in char reactivity and structure during the gasification of a Victorian brown coal: comparison between gasification in O2 and CO2[J]. Fuel Process Technol, 2010, 91(8): 800-804. QUYN D M, HAYASHI J I, LI C Z. Volatilisation of alkali and alkaline earth metallic species during the gasification of a Victorian brown coal in CO2[J]. Fuel Process Technol, 2005, 86(12/13): 1241-1251. LI X J, HAYASHI J I, LI C Z. FT-Raman spectroscopic study of the evolution of char structure during the pyrolysis of a Victorian brown coal[J]. Fuel, 2006, 85(12/13): 1700-1707. TAY H L, KAJITANI S, ZHANG S, LI C Z. Inhibiting and other effects of hydrogen during gasification: Further insights from FT-Raman spectroscopy[J]. Fuel, 2014, 116: 1-6. TAY H L, KAJITANI S, WANG S, LI C Z. A preliminary Raman spectroscopic perspective for the roles of catalysts during char gasification[J]. Fuel, 2014, 121: 165-172. LI X J, HAYASHI J I, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal.Part VII. Raman spectroscopic study on the changes in char structure during the catalytic gasification in air[J]. Fuel, 2006, 85(10/11): 1509-1517. LI X J, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal.Part VIII. Catalysis and changes in char structure during gasification in steam[J]. Fuel, 2006, 85(10/11): 1518-1525. QUYN D M, WU H W, HAYASHI J I, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part IV. Catalytic effects of NaCl and ion-exchangeable Na in coal on char reactivity[J]. Fuel, 2003, 82(5): 587-593. LI C Z, SATHE C, KERSHAW J R, PANG Y. Fates and roles of alkali and alkaline earth metals during the pyrolysis of a Victorian brown coal[J]. Fuel, 2000, 79(3/4): 427-438. KEOWN D M, HAYASHI J I, LI C Z. Drastic changes in biomass char structure and reactivity upon contact with steam[J]. Fuel, 2008, 87(7): 1127-1132. FUSHIMI C, WADA T, TSUTSUMI A. Inhibition of steam gasification of biomass char by hydrogen and tar[J]. Biomass Bioenergy, 2011, 35(1): 179-185. LUSSIER M G, ZHANG Z, MILLER D J. Characterizing rate inhibition in steam/hydrogen gasification via analysis of adsorbed hydrogen[J]. Carbon, 1998, 36(9): 1361-1369. JOCHEN S, TORE M. Reduction of a detailed reaction mechanism for hydrogen combustion under gas turbine conditions[J]. Combust Flame, 2006, 144(3): 545-557. QUYN D M, WU H W, P.BHATTACHARYA S, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part II. Effects of chemical form and valence[J]. Fuel, 2002, 81(2): 151-158. LI C Z. Some recent advances in the understanding of the pyrolysis and gasification behaviour of Victorian brown coal[J]. Fuel, 2007, 86(12/13): 1664-1683. WU H W, HAYASHI J I, CHIBA T, TAKARADA T, LI C Z. Volatilisation and catalytic effects of alkali and alkaline earth metallic species during the pyrolysis and gasification of Victorian brown coal. Part V. Combined effects of Na concentration and char structure on char reactivity[J]. Fuel, 2004, 83(1): 23-30.
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