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高温气化条件下煤直接液化残渣中矿物质演化行为的研究

温海涛 ,  孔令学 ,  白进 ,  白宗庆 ,  吕冬梅 ,  李文

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引用本文: 温海涛, 孔令学, 白进, 白宗庆, 吕冬梅, 李文. 高温气化条件下煤直接液化残渣中矿物质演化行为的研究[J]. 燃料化学学报, 2015, 43(3): 257-265. shu
Citation:  WEN Hai-tao, KONG Ling-xue, BAI Jin, BAI Zong-qing, LÜ Dong-mei, LI Wen. Transformation of minerals in direct coal liquefaction residue under gasification atmosphere at high temperatures[J]. Journal of Fuel Chemistry and Technology, 2015, 43(3): 257-265. shu

高温气化条件下煤直接液化残渣中矿物质演化行为的研究

    通讯作者: 白进(1981-),男,山西太原人,博士,副研究员,主要从事煤的灰化学研究。Tel:0351-4040289;Fax:0351-4050320;E-mail:stone@sxicc.ac.cn。
  • 基金项目:

    国家自然科学基金(21476247) (21476247)

    国家自然科学基金青年基金(21406254) (21406254)

    国家自然科学基金委员会与神华集团有限责任公司联合资助项目(U1261209)。 (U1261209)

摘要: 利用XRD和FT-IR分析了高温(1 100~1 500 ℃)气化条件下液化残渣中矿物质的演变行为,并利用穆斯堡尔谱仪对残渣灰中的含铁相及铁的价态铁进行了定量分析。结果表明,煤直接液化残渣中的主要矿物质为石英、硫酸钙、紫铝铁矾、磁黄铁矿、高岭石和方解石。高温气化条件下残渣灰中主要矿物质为钙长石、钙黄长石、磁赤铁矿和磁铁矿。由于钙长石、钙黄长石等含钙化合物低温共熔作用,使得残渣灰具有较低的熔融温度。残渣灰中的含铁相主要为磁赤铁矿、磁铁矿、铁橄榄石和玻璃体,并且随温度的升高,玻璃体中的铁含量逐渐增加。同时,残渣灰中Fe2+/Fe3+出现先增加后降低再增加的变化趋势。当温度由1 100 ℃升高至1 200 ℃时,由于磁赤铁矿的还原,Fe2+/Fe3+由1.08升高至2.39;1 200 ℃以上Fe2+/Fe3+的变化不明显。另外,玻璃体中铁含量的增加是引起残渣灰液相含量随温度升高而增加的重要原因,铁含量高是导致残渣灰熔融温度低的主要原因。

English

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    1. [1] 舒歌平, 史士东, 李克健. 煤炭液化技术[M]. 北京: 煤炭工业出版社, 2003.(SHU Ge-ping, SHI Shi-dong, LI Ke-jian. Coal liquefaction technology[M]. Beijing: China Coal Industry Publishing House, 2003.)[1] 舒歌平, 史士东, 李克健. 煤炭液化技术[M]. 北京: 煤炭工业出版社, 2003.(SHU Ge-ping, SHI Shi-dong, LI Ke-jian. Coal liquefaction technology[M]. Beijing: China Coal Industry Publishing House, 2003.)

    2. [2] 罗万江, 兰新哲, 宋永辉, 付建平. 煤直接液化残渣的利用研究进展[J]. 材料导报A, 2013, 27(6): 153-157.(LUO Wan-jiang, LAN Xin-zhe, SONG Yong-hui, FU Jian-ping. Research progress on utilization of coal liquefaction residue[J]. Mater Rev A, 2013, 27(6): 153-157.)[2] 罗万江, 兰新哲, 宋永辉, 付建平. 煤直接液化残渣的利用研究进展[J]. 材料导报A, 2013, 27(6): 153-157.(LUO Wan-jiang, LAN Xin-zhe, SONG Yong-hui, FU Jian-ping. Research progress on utilization of coal liquefaction residue[J]. Mater Rev A, 2013, 27(6): 153-157.)

    3. [3] WU X J, ZHOU T, CHEN Y S, ZHANG Z X, PIAO G L, KOBAYASHI N, MORI S, YITAYA Y. Mineral melting behavior of Chinese blended coal ash under gasification condition[J]. Asia-Pac J Chem Eng, 2011, 6(2): 220-230.[3] WU X J, ZHOU T, CHEN Y S, ZHANG Z X, PIAO G L, KOBAYASHI N, MORI S, YITAYA Y. Mineral melting behavior of Chinese blended coal ash under gasification condition[J]. Asia-Pac J Chem Eng, 2011, 6(2): 220-230.

    4. [4] 芦涛, 张雷, 张晔, 丰芸, 李寒旭. 煤灰中矿物质组成对煤灰熔融温度的影响[J]. 燃料化学学报, 2010, 38(1): 23-28.(LU Tao, ZHANG Lei, ZHANG Ye, FENG Yun, LI Han-xu. Effect of mineral composition on coal ash fusion temperature[J]. J Fuel Chem Technol, 2010, 38(1): 23-28.)[4] 芦涛, 张雷, 张晔, 丰芸, 李寒旭. 煤灰中矿物质组成对煤灰熔融温度的影响[J]. 燃料化学学报, 2010, 38(1): 23-28.(LU Tao, ZHANG Lei, ZHANG Ye, FENG Yun, LI Han-xu. Effect of mineral composition on coal ash fusion temperature[J]. J Fuel Chem Technol, 2010, 38(1): 23-28.)

    5. [5] VANDYK J C, MELZER S, SOBIECKI A. Mineral matter transformation during Sasol-Lurgi fixed bed dry bottom gasification-utilization of HT-XRD and Factsage modeling[J]. Miner Eng, 2006, 19(10): 1126-1135.[5] VANDYK J C, MELZER S, SOBIECKI A. Mineral matter transformation during Sasol-Lurgi fixed bed dry bottom gasification-utilization of HT-XRD and Factsage modeling[J]. Miner Eng, 2006, 19(10): 1126-1135.

    6. [6] 白进, 李文, LI Chun-zhu, 白宗庆, 李保庆. 高温下煤中矿物质对气化反应的影响[J]. 燃料化学学报, 2009, 37(2): 134-138.(BAI Jin, LI Wen, LI Chun-zhu, BAI Zong-qing, LI Bao-qing. Influences of mineral matter on high temperature gasification of coal char[J]. J Fuel Chem Technol, 2009, 37(2): 134-138.)[6] 白进, 李文, LI Chun-zhu, 白宗庆, 李保庆. 高温下煤中矿物质对气化反应的影响[J]. 燃料化学学报, 2009, 37(2): 134-138.(BAI Jin, LI Wen, LI Chun-zhu, BAI Zong-qing, LI Bao-qing. Influences of mineral matter on high temperature gasification of coal char[J]. J Fuel Chem Technol, 2009, 37(2): 134-138.)

    7. [7] MA Z B, BAI J, LI W, BAI Z Q, KONG L X. Mineral transformation in char and its effect on coal char gasification reactivity at high temperatures, Part 1: Mineral transformation in char[J]. Energy Fuels, 2013, 27(8): 4545-4554.[7] MA Z B, BAI J, LI W, BAI Z Q, KONG L X. Mineral transformation in char and its effect on coal char gasification reactivity at high temperatures, Part 1: Mineral transformation in char[J]. Energy Fuels, 2013, 27(8): 4545-4554.

    8. [8] MA Z B, BAI J, BAI Z Q, KONG L X, GUO Z X, YAN J C, LI W. Mineral transformation in char and its effect on coal char gasification reactivity at high temperatures, Part 2: Char gasification[J]. Energy Fuels, 2014, 28(3): 1846-1853.[8] MA Z B, BAI J, BAI Z Q, KONG L X, GUO Z X, YAN J C, LI W. Mineral transformation in char and its effect on coal char gasification reactivity at high temperatures, Part 2: Char gasification[J]. Energy Fuels, 2014, 28(3): 1846-1853.

    9. [9] 世史东. 煤加氢液化工程学基础[M]. 北京: 化学工业出版社, 2012.(SHI Shi-dong. The engineering foundation of coal hydro-liquefaction[M]. Beingjing: Chemical Industry Press, 2012.)[9] 世史东. 煤加氢液化工程学基础[M]. 北京: 化学工业出版社, 2012.(SHI Shi-dong. The engineering foundation of coal hydro-liquefaction[M]. Beingjing: Chemical Industry Press, 2012.)

    10. [10] 于遵宏, 王辅臣. 煤炭气化技术[M]. 北京: 化学工业出版社, 2010.(YU Zun-hong, WANG Fu-chen. Coal gasification technology[M]. Beijing: Chemical Industry Press, 2010.)[10] 于遵宏, 王辅臣. 煤炭气化技术[M]. 北京: 化学工业出版社, 2010.(YU Zun-hong, WANG Fu-chen. Coal gasification technology[M]. Beijing: Chemical Industry Press, 2010.)

    11. [11] 杨南如, 夏元复, 陈刚, 刘荣川. 用穆斯堡尔谱效应研究粉煤灰中含铁相[J]. 燃料化学学报, 1984, 12(4): 375-381.(YANG Nan-ru, XIA Yuan-fu, CHEN Gang, LIU Rong-chuan. Mössbauer effect study of iron-bearing phases in pulverized coal ash[J]. J Fuel Chem Technol, 1984, 12(4): 375-381.)[11] 杨南如, 夏元复, 陈刚, 刘荣川. 用穆斯堡尔谱效应研究粉煤灰中含铁相[J]. 燃料化学学报, 1984, 12(4): 375-381.(YANG Nan-ru, XIA Yuan-fu, CHEN Gang, LIU Rong-chuan. Mössbauer effect study of iron-bearing phases in pulverized coal ash[J]. J Fuel Chem Technol, 1984, 12(4): 375-381.)

    12. [12] 杨南如, 张振桴, 曾燕伟. 用穆斯堡尔效应研究煤灰熔聚物中的含铁相[J]. 燃料化学学报, 1987, 15(1): 67-72.(YANG Nan-ru, ZHANG Zhen-fu, ZENG Yan-wei. Study on the iron-bearing phase in coal ash agglomerates by Mössbauer effect[J]. J Fuel Chem Technol, 1987, 15(1): 67-72.)[12] 杨南如, 张振桴, 曾燕伟. 用穆斯堡尔效应研究煤灰熔聚物中的含铁相[J]. 燃料化学学报, 1987, 15(1): 67-72.(YANG Nan-ru, ZHANG Zhen-fu, ZENG Yan-wei. Study on the iron-bearing phase in coal ash agglomerates by Mössbauer effect[J]. J Fuel Chem Technol, 1987, 15(1): 67-72.)

    13. [13] VUTHALURU H B, EENKHOORN S, HAMBURG G, HEERE P G T, KIEL J H A. Behaviour of iron-bearing minerals in the early stages of pulverised coal conversion processes[J]. Fuel Process Technol, 1998, 56(1/2): 21-31.[13] VUTHALURU H B, EENKHOORN S, HAMBURG G, HEERE P G T, KIEL J H A. Behaviour of iron-bearing minerals in the early stages of pulverised coal conversion processes[J]. Fuel Process Technol, 1998, 56(1/2): 21-31.

    14. [14] WAANDERS F B, VINKEN E, MANS A, MULABA-BAFUBIANDI A F. Iron minerals in coal, weathered coal and coal Ash-SEM and Mössbauer results[J]. Hyperfine Interact, 2003, 148/149(1/4): 21-29.[14] WAANDERS F B, VINKEN E, MANS A, MULABA-BAFUBIANDI A F. Iron minerals in coal, weathered coal and coal Ash-SEM and Mössbauer results[J]. Hyperfine Interact, 2003, 148/149(1/4): 21-29.

    15. [15] 李文, 白进. 煤的灰化学[M]. 北京: 科学出版社, 2013.(LI Wen, BAI Jin. Chemistry of ash from coal[M]. Beinjing: Science Press, 2013.)[15] 李文, 白进. 煤的灰化学[M]. 北京: 科学出版社, 2013.(LI Wen, BAI Jin. Chemistry of ash from coal[M]. Beinjing: Science Press, 2013.)

    16. [16] CHU X J, LI W, LI B Q, CHEN H K. Gasification property of direct coal liquefaction residue with steam[J]. Process Saf Environ Protect, 2006, 84(B6): 440-445.[16] CHU X J, LI W, LI B Q, CHEN H K. Gasification property of direct coal liquefaction residue with steam[J]. Process Saf Environ Protect, 2006, 84(B6): 440-445.

    17. [17] BAI J, LI W, LI B Q. Characterization of low-temperature coal ash behaviors at high temperatures under reducing atmosphere[J]. Fuel, 2008, 87(4/5): 583-591.[17] BAI J, LI W, LI B Q. Characterization of low-temperature coal ash behaviors at high temperatures under reducing atmosphere[J]. Fuel, 2008, 87(4/5): 583-591.

    18. [18] 马志斌, 白宗庆, 白进, 李文, 郭振兴. 高温弱还原气氛下高硅铝比煤灰变化行为的研究[J]. 燃料化学学报, 2012, 40(3): 279-285.(MA Zhi-bin, BAI Zong-qing, BAI Jin, LI Wen, GUO Zhen-xing. Evolution of coal ash with high Si/Al ratio under reducing atmosphere at high temperature[J]. J Fuel Chem Technol, 2012, 40(3): 279-285.)[18] 马志斌, 白宗庆, 白进, 李文, 郭振兴. 高温弱还原气氛下高硅铝比煤灰变化行为的研究[J]. 燃料化学学报, 2012, 40(3): 279-285.(MA Zhi-bin, BAI Zong-qing, BAI Jin, LI Wen, GUO Zhen-xing. Evolution of coal ash with high Si/Al ratio under reducing atmosphere at high temperature[J]. J Fuel Chem Technol, 2012, 40(3): 279-285.)

    19. [19] RAM L C, TRIPATHI P S M, MISHRA S P. Mössbauer spectroscopic studies on the transformations of iron-bearing minerals during combustion of coals: Correlation with fouling and slagging[J]. Fuel Process Technol, 1995, 42(1): 47-60.[19] RAM L C, TRIPATHI P S M, MISHRA S P. Mössbauer spectroscopic studies on the transformations of iron-bearing minerals during combustion of coals: Correlation with fouling and slagging[J]. Fuel Process Technol, 1995, 42(1): 47-60.

    20. [20] 夏元复, 刘荣川, 王述新, 许超, 潘素瑛, 程一兵. 高铁硅酸盐玻璃体系的穆斯堡尔研究[J]. 物理学报, 1984, 33(1): 132-136.(XIA Yuan-fu, LIU Rong-chuan, WANG Shu-xin, XU Chao, PAN Su-ying, CHENG Yi-bing. A Mössbauer investigation of the iron-sodium-silicate glass systems[J]. Acta Phys-Chim Sin, 1984, 33(1): 132-136.)[20] 夏元复, 刘荣川, 王述新, 许超, 潘素瑛, 程一兵. 高铁硅酸盐玻璃体系的穆斯堡尔研究[J]. 物理学报, 1984, 33(1): 132-136.(XIA Yuan-fu, LIU Rong-chuan, WANG Shu-xin, XU Chao, PAN Su-ying, CHENG Yi-bing. A Mössbauer investigation of the iron-sodium-silicate glass systems[J]. Acta Phys-Chim Sin, 1984, 33(1): 132-136.)

    21. [21] 吴新, 卓文钦, 赵长遂. 燃煤飞灰中铁磁性物质及其形成机制[J]. 燃烧科学与技术, 2010, 16(5): 422-429.(WU Xin, ZHUO Wen-xin, ZHAO Chang-sui. Ferromagnetic substance in coal-fired fly ash and its formation mechanism[J]. Process Saf Environ Protect, 2010, 16(5): 422-429.)[21] 吴新, 卓文钦, 赵长遂. 燃煤飞灰中铁磁性物质及其形成机制[J]. 燃烧科学与技术, 2010, 16(5): 422-429.(WU Xin, ZHUO Wen-xin, ZHAO Chang-sui. Ferromagnetic substance in coal-fired fly ash and its formation mechanism[J]. Process Saf Environ Protect, 2010, 16(5): 422-429.)

    22. [22] 尧德中, 俞劲炎, 刘榜华. 应用穆斯堡尔谱(Mössbauer spectroscopy)研究土壤磁性的发生机理[J]. 土壤学报, 1990, 27(4): 361-367.(YAO De-zhong, YU Jin-yan, LIU Bang-hua. The use of Mössbauer spectroscopy in study of soil magnetic genesis[J]. Acta Pedol Sin, 1990, 27(4): 361-367.)[22] 尧德中, 俞劲炎, 刘榜华. 应用穆斯堡尔谱(Mössbauer spectroscopy)研究土壤磁性的发生机理[J]. 土壤学报, 1990, 27(4): 361-367.(YAO De-zhong, YU Jin-yan, LIU Bang-hua. The use of Mössbauer spectroscopy in study of soil magnetic genesis[J]. Acta Pedol Sin, 1990, 27(4): 361-367.)

    23. [23] LOTTERMOSER W, FORCHER K, AMTHAUER G, FUESS H. Power-and single crystal Mössbauer spectroscopy on synthetic fayalite[J]. Phys Chem Minerals, 1995, 22: 259-267.[23] LOTTERMOSER W, FORCHER K, AMTHAUER G, FUESS H. Power-and single crystal Mössbauer spectroscopy on synthetic fayalite[J]. Phys Chem Minerals, 1995, 22: 259-267.

    24. [24] MYSEN B O, IRGO D. Redox equilibria, structure, and properties of Fe-bearing aluminosilicate melts: Relationships among temperature, composition, and oxygen fugacity in the system Na2O-Al2O3-SiO2-Fe-O[J]. Am Mineral, 1989, 74: 58-76.[24] MYSEN B O, IRGO D. Redox equilibria, structure, and properties of Fe-bearing aluminosilicate melts: Relationships among temperature, composition, and oxygen fugacity in the system Na2O-Al2O3-SiO2-Fe-O[J]. Am Mineral, 1989, 74: 58-76.

    25. [25] OWOK J W. Viscosity and structural state of iron in coal ash slag under gasification conditions[J]. Energy Fuels, 1995, 9(3): 534-539.[25] OWOK J W. Viscosity and structural state of iron in coal ash slag under gasification conditions[J]. Energy Fuels, 1995, 9(3): 534-539.

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