铁基载氧体对煤中汞释放行为的影响

doi:10.16085/j.issn.1000-6613.2019-0212

化工进展 ›› 2019, Vol. 38 ›› Issue (s1): 240-246.DOI: 10.16085/j.issn.1000-6613.2019-0212

铁基载氧体对煤中汞释放行为的影响

高明刚, 刘永卓, 张欣涛, 宋鸣航, 郭庆杰

青岛科技大学化工学院, 山东省高等学校清洁化工重点实验室, 山东青岛 266042

收稿日期:2019-02-11 修回日期:2019-05-14 出版日期:2019-11-16 发布日期:2019-11-16
通讯作者: 刘永卓,博士,副教授,硕士生导师,研究方向为煤/生物质化学链清洁高效转化、多相反应流的数值模拟、流化床反应器设计与优化等。
作者简介:高明刚(1992-),男,硕士研究生,研究方向为污染物排放与控制。E-mail:724138364@qq.com。
基金资助:
国家自然科学基金青年基金（51506105）；山东省重点研发计划（2017GSF16101）；青岛市源头创新计划（17-1-1-37-jch）。

Effects of Fe-based oxygen carriers on mercury release behavior from coal

GAO Minggang, LIU Yongzhuo, ZHANG Xintao, SONG Minghang, GUO Qingjie

College of Chemical Engineering, Qingdao University of Science&Technology, Key Laboratory of Clean Chemical Engineering in Universities of Shandong, Qingdao 266042, Shandong, China

Received:2019-02-11 Revised:2019-05-14 Online:2019-11-16 Published:2019-11-16

摘要/Abstract

摘要： 采用Ontario-Hydro方法，在管式炉中考察了煤化学链燃烧/气化过程中Fe₄Al₆载氧体对煤中汞释放率、气态汞形态分布及汞在两反应器内释放行为的影响。结果表明，载氧体对煤中汞释放率具有显著的影响，在500~700℃，与无载氧体相比，化学链燃烧过程煤中汞释放率减少，化学链气化过程煤中汞释放率增大，而在900℃时，无论化学链燃烧过程还是化学链气化过程，煤中汞释放率均减小。Fe₄Al₆载氧体能够显著增加燃料反应器出口气态Hg²⁺的相对含量，其含量随温度的升高而逐渐升高。燃料反应器的温度也是影响煤中汞在两反应器中的分布以及空气反应器中不同价态汞百分含量的重要因素。此外，相同条件下不同煤种的汞释放率不同，主要与煤的组成不同有关。该研究对揭示载氧体对煤中汞迁移的影响机理以及煤化学链转化过程汞的控制提供了实验依据。

关键词: 化学链燃烧, 化学链气化, 汞释放, 载氧体, 形态分布

Abstract: Effects of Fe₄Al₆ oxygen carriers on mercury release rate, gaseous mercury distribution and mercury release behavior in two reactors in coal chemical looping combustion/gasification process were investigated by Ontario-Hydro method in a tubular furnace. The result showed that Fe₄Al₆ oxygen carriers could affect the mercury release rate significantly. Compared with the traditional coal pyrolysis, mercury release rate in CLC decreased, while that in CLG increased in 500-700℃. However, mercury release rate in both CLC and CLG was more than that without oxygen carriers at 900℃. Fe₄Al₆ oxygen carriers can significantly increase the relative content of Hg²⁺ from fuel reactor (FR) outlet. The relative content of Hg²⁺ increased with the increasing temperature. Besides the content of oxygen carrier, FR temperature was the primary influence factor on the distribution of mercury from fuel reactor and air reactor as well as the percentage of gaseous mercury speciation in the air reactor. In addition, the mercury release rate was different from types of coal under the same condition, which related mainly to the composition of coal. This study will provide experimental evidence for revealing the influence mechanism of oxygen carriers on mercury migration in the coal and for the control of mercury in coal chemical looping conversion processes.

Key words: chemical looping combustion, chemical looping gasification, mercury release, oxygen carriers, species distribution

中图分类号:

TQ534.9

高明刚, 刘永卓, 张欣涛, 宋鸣航, 郭庆杰. 铁基载氧体对煤中汞释放行为的影响[J]. 化工进展, 2019, 38(s1): 240-246.

GAO Minggang, LIU Yongzhuo, ZHANG Xintao, SONG Minghang, GUO Qingjie. Effects of Fe-based oxygen carriers on mercury release behavior from coal[J]. Chemical Industry and Engineering Progress, 2019, 38(s1): 240-246.

参考文献

[1] EVAN J Granite, HENRY W Pennline. Constance senior. Mercury control for coal-derived gas streams[M]. Frankfurt:Wiley-VCH Verlag GmbH & Co. KGaA, 2015:51-66.
[2] 王泉海. 煤燃烧过程中汞排放及其控制的实验及机理研究[D]. 武汉:华中科技大学, 2006. WANG Quanhai. Experimental and mechanism study on mercury emission and control during coal combustion[D]. Wuhan:Huazhong University of Science & Technology, 2006.
[3] 刘永卓, 郭庆杰, 田红景. 煤化学链转化技术研究进展[J]. 化工进展, 2014, 33(6):1357-1364. LIU Yongzhuo, GUO Qingjie, TIAN Hongjing. Advance in the coal chemical-looping conversion technology[J]. Chemical Industry and Engineering Progress, 2014, 33(6):1357-1364.
[4] 程煜. 铁基载氧体/煤化学链气化反应及动力学研究[D]. 青岛:青岛科技大学, 2013. CHENG Yu. Chemical-looping gasification reaction characteristics and kinetic studies of coal and Fe-based oxygen carriers[D]. Qingdao:Qingdao University of Science & Technology, 2013.
[5] JUAN Adanez, ALBERTO Abad, FRANCISCO Garcia-Labiano, et al. Progress in chemical-looping combustion and reforming technologies[J]. Progress in Energy and Combustion Science, 2012, 38(2):215-282.
[6] YANG Hongqun, XU Zhenghe, FAN Maohong, et al. Progress in carbon dioxide separation and capture:a review[J]. Journal of Environmental Sciences, 2008, 20(1):14-27.
[7] FAN Liangshi, ZENG Liang, WANG William, et al. Chemical looping processes for CO₂ capture and carbonaceous fuel conversion prospect and opportunity[J]. Energy Environ & Science, 2012, 5:7254-7280.
[8] 史晓斐, 杨思宇, 钱宇. 化学链技术在煤炭清洁高效利用中的研究进展[J]. 化工学报, 2018, 69(12):4931-4946. SHI Xiaofei, YANG Siyu, QIAN Yu. Chemical looping technology for clean and highly efficient coal processes[J]. CIESC Journal, 2018, 69(12):4931-4946.
[9] MENDIARA T, IZQUIERDO M T, ABAD A, et al. Mercury release and speciation in chemical looping combustion of coal[J]. Energy & Fuels, 2014, 28(4):2786-2794.
[10] 张志越, 毛琳, 孙佳兴, 等. 温度对载氧体还原过程中汞的析出特性及形态分布的影响[J]. 化工进展, 2018, 37(3):1187-1193. ZHANG Zhiyue, MAO Lin, SUN Jiaxing, et al. Characterization of mercury releasing during reduction of oxygen carriers with coal in chemical looping combustion[J]. Chemical Industry and Engineering Progress, 2018, 37(3):1187-1193.
[11] PéREZ Vega Raúl, ADáNEZ Rubio Inaki, GAYáN Pilar, et al. Sulphur, nitrogen and mercury emissions from coal combustion with CO₂ capture in chemical looping with oxygen uncoupling (CLOU)[J]. International Journal of Greenhouse Gas Control, 2016, 46:28-38.
[12] LI Jihong, LIN Changfeng, QIN Wu, et al. Synergetic effect of mercury adsorption on the catalytic decomposition of CO over perfect and reduced Fe₂O₃
[001] Surface[J]. Acta Physico-Chimica Sinica, 2016, 32(11):2717-2723.
[13] ZHANG Junjiao, QIN Wu, DONG Changqing, et al. Density functional theory study of elemental mercury adsorption on Fe₂O₃
[104] and it's effect on carbon deposit during chemical looping combustion[J]. Energy & Fuels, 2016, 30(4):3413-3418.
[14] GUO Pan, GUO Xin, ZHENG Chuguang. Roles of γ-Fe₂O₃ in fly ash for mercury removal:results of density functional theory study[J]. Applied Surface Science, 2010, 256(3):6991-6996.
[15] JUNG Ji Eun, GEATCHES Lesley Dawn, LEE Kyoungjin, et al. First-principles investigation of mercury adsorption on the α-Fe₂O₃(1102) surface[J]. The Journal of Physical Chemistry C, 2015, 119(47):26512-26518.
[16] GALBREATH Kevin C, ZYGRLICKE Christopher J, TIBBETTS James E, et al. Effects of NO_x, α-Fe₂O₃, γ-Fe₂O₃, and HCl on mercury transformations in a 7-kW coal combustion system[J]. Fuel Processing Technology, 2005, 86(4):429-448.
[17] 万奇顺. 煤灰对载氧体的煤焦化学链气化反应特性及形貌结构影响研究[D]. 青岛:青岛科技大学, 2017. WAN Qishun. Study of the effect of coal ash on the reaction characteristic and morphology structure of oxygen carrier in chemical looping gasification with coal char[D]. Qingdao:Qingdao University of Science & Technology, 2017.
[18] U. S. EPA. Standard test method for mercury from coal-fired stationary sources (ontario hydro method):ASTM D6784-02[S]. Philadelphia:American Society for Testing and Materials International, 1999.

铁基载氧体对煤中汞释放行为的影响

Effects of Fe-based oxygen carriers on mercury release behavior from coal

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	朱杰, 金晶, 丁正浩, 杨会盼, 侯封校. 化学链气化中准东煤灰对CaSO₄载氧体改性及其作用机理[J]. 化工进展, 2023, 42(9): 4628-4635.
[2]	王保文, 刘同庆, 张港, 李炜光, 林德顺, 王梦家, 马晶晶. CuFe₂O₄改性脱硫渣氧载体与褐煤的反应特性[J]. 化工进展, 2023, 42(6): 2884-2894.
[3]	龚陈俊, 梅道锋. 钨修饰对镍载氧体的沼气化学链重整制氢性能影响[J]. 化工进展, 2023, 42(4): 2130-2141.
[4]	范昀培, 金晶, 刘敦禹, 王静杰, 刘秋祺, 许开龙. CaSO₄载氧体在煤气化化学链燃烧中的脱汞[J]. 化工进展, 2023, 42(3): 1638-1648.
[5]	沈天绪, 沈来宏. 基于3kW塔式串行流化床差异燃料的化学链燃烧解析[J]. 化工进展, 2023, 42(1): 138-147.
[6]	安阳, 袁思杰, 高振东, 吴曼, 王凌云, 郭庆杰. Mg修饰Fe/Al载氧体煤化学链制氢[J]. 化工进展, 2022, 41(2): 648-654.
[7]	韩丹华, 郭雪岩, 王志远. 化学链重整制氢NiO-CeO₂/γ-Al₂O₃复合载氧体的性能[J]. 化工进展, 2022, 41(1): 192-200.
[8]	朱晓, 沈来宏, 沈天绪, 闫景春. 塔式化学链燃烧反应器系统的气固流动特性[J]. 化工进展, 2021, 40(8): 4144-4151.
[9]	李彦坤,马晶晶,常国璋,胡修德,郭庆杰. 基于铁基载氧体的煤化学链气化还原过程中氮元素迁移行为[J]. 化工进展, 2019, 38(08): 3631-3639.
[10]	吴健, 沈来宏, 蒋守席, 闫景春, 沈天绪. 基于双级燃料反应器的污泥化学链燃烧特性[J]. 化工进展, 2018, 37(07): 2830-2836.
[11]	王博, 郭庆杰. CuO修饰的赤泥载氧体废弃活性炭化学链燃烧[J]. 化工进展, 2018, 37(07): 2837-2845.
[12]	张志越, 毛琳, 孙佳兴, 周长松, 姜小祥, 杨宏旻. 温度对载氧体还原过程中汞的析出特性及形态分布的影响[J]. 化工进展, 2018, 37(03): 1187-1193.
[13]	胡晓雨, 金保昇, 王晓佳, 王旭东, 朱小明. 草木灰水溶液改性的天然贫铁矿载氧体的反应性能[J]. 化工进展, 2017, 36(11): 4022-4029.
[14]	王晨平, 段钰锋, 赵士林, 李雅宁, 朱纯, 佘敏, 刘猛, 韦红旗, 王双群. 燃烧温度对煤中汞析出特性及形态分布的影响[J]. 化工进展, 2017, 36(05): 1899-1905.
[15]	李雅宁, 段钰锋, 王卉, 薛源, 朱纯, 周强, 张君, 佘敏, 刘猛. O₂/CO₂气氛下煤中汞的释放特性[J]. 化工进展, 2017, 36(01): 372-377.