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

doi:10.16085/j.issn.1000-6613.2017-1117

化工进展 ›› 2018, Vol. 37 ›› Issue (03): 1187-1193.DOI: 10.16085/j.issn.1000-6613.2017-1117

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

张志越, 毛琳, 孙佳兴, 周长松, 姜小祥, 杨宏旻

南京师范大学能源与机械工程学院, 江苏南京 210042

收稿日期:2017-06-08 修回日期:2017-07-01 出版日期:2018-03-05 发布日期:2018-03-05
通讯作者: 杨宏旻,教授,研究方向为大气污染控制。
作者简介:张志越(1992-),男,硕士研究生。
基金资助:
国家自然科学基金（51676101）及江苏省自然科学基金（BK20161558）项目。

Characterization of mercury releasing during reduction of oxygen carriers with coal in chemical looping combustion

ZHANG Zhiyue, MAO Lin, SUN Jiaxing, ZHOU Changsong, JIANG Xiaoxiang, YANG Hongmin

School of Energy and Mechanical Engineering, Nanjing Normal University, Nanjing 210042, Jiangsu, China

Received:2017-06-08 Revised:2017-07-01 Online:2018-03-05 Published:2018-03-05

摘要/Abstract

摘要： 化学链燃烧是近年来提出的一种具有高效、内分离CO₂特点的新型燃烧方式。本文在立式管式炉实验装置上研究了温度对基于Fe₂O₃载氧体的煤化学链燃烧载氧体还原过程中汞析出特性的影响，探讨了不同燃烧温度下燃料反应器（FR）出口烟气组分的变化及其对汞迁移变化的影响。结果表明：在高温条件下（≥ 800℃），煤中的汞在载氧体还原过程中基本全部析出，180s时基本达到90%，并且随着温度升高而增加；FR出口烟气中的汞主要以单质态（Hg⁰）形式存在，各工况下的单质态汞占烟气中气态总汞比例都在88%以上，随着温度的升高，烟气中Hg⁰/Hg^T略有降低；温度对烟气组分具有影响，随着温度的升高，CO、NO和SO₂浓度上升；对于汞而言，SO₂会抑制Cl及Cl₂的形成从而抑制Hg⁰向Hg²⁺转化，NO会直接或间接促进汞的氧化过程，FR烟气中以CO为主的还原性气氛不利于汞的氧化。

关键词: 煤, 还原, 化学链燃烧, 汞释放, Fe₂O₃载氧体

Abstract: Chemical looping combustion is one of the promising technologies to capture CO₂ with low cost. The effect of temperatures on mercury speciation and transport during coal chemical looping combustion based on Fe₂O₃ oxygen carriers were studied in a vertical tube furnace device. The change of flue gas components at different temperatures and the oxidation mechanism of elemental mercury on flue gas from fuel reactor were also investigated. The results showed that mercury in coal was completly released and the discharge rate reached 90% in 180s at high temperature in FR. The major mercury species was Hg⁰ and the ratio Hg⁰/Hg^T was 88%. The rate of Hg⁰/Hg^T decreased with increasing temperature. Different temperature affected the components of flue gas. The elevated temperature could cause an increase in the SO₂,NO and CO. SO₂ could inhibit the oxidation of mercury by inhibiting the formation of Cl/Cl₂. The NO could promote the oxidation of mercury,but CO had an opposite effect.

Key words: coal, reduction, chemical looping combustion, mercury release, Fe₂O₃ oxygen carriers

中图分类号:

X511

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.

ZHANG Zhiyue, MAO Lin, SUN Jiaxing, ZHOU Changsong, JIANG Xiaoxiang, YANG Hongmin. Characterization of mercury releasing during reduction of oxygen carriers with coal in chemical looping combustion[J]. Chemical Industry and Engineering Progress, 2018, 37(03): 1187-1193.

参考文献

[1] 王志,杨东晓,张晨昕,等. 分离二氧化碳膜过程技术经济分析[J]. 化工进展,2009,28(s2):409-410. WANG Zhi,YANG Dongxiao,ZHANG Chenxi,et al.Technical and economic analysis of the process of carbon dioxide separation membrane[J]. Chemical Industry and Engineering Progress,2009,28(s2):409-410.
[2] RICHTER H J,KNOCHE K F. Efficiency and costing——second law analysis of processes[J]. ACS Symp. Ser.,1983,235:71-85.
[3] GU H M,SHEN L,ZHONG Z,et al. NO release during chemical looping combustion with iron ore as an oxygen carrier[J]. Chemical Engineering Journal,2015,264:211-220.
[4] 金红光,王宝群. 化学能梯级利用机理探讨[J]. 工程热物理学报,2004,25(2):181-184. JIN Hongguang,WANG Banqun. Principle of cascading utilization of chemical energy[J]. Journal of Engineering Thermophysics,2004,25(2):181-184.
[5] 秦翠娟,沈来宏,肖军,等. 化学链燃烧技术的研究进展[J]. 锅炉技术,2008,39(5):64-73. QIN Cuijuan,SHEN Laihong,XIAO Jun,et al. Research development of chemical-looping combustion[J]. Boiler Technol.,2008,39(5):64-73.
[6] PAVLISH J H,HOLMES M J,BENSON S A,et al. Application of sorbents for mercury control for utilities burning lignite coal[J]. Fuel Processing Technology,2004,85(6/7):563-576.
[7] 郭欣,郑楚光,贾小红,等. 300MW煤粉锅炉烟钟汞形态分析的实验研究[J]. 中国电机工程学报,2004,24(6):185-188. GUO X,ZHENG C G,JIA X H,et al. Study on mercury speciation in pulverized coal fired flue gas[J]. Proceedings of the CSEE,2004,24(6):185-188.
[8] 刘玲,段钰锋,王运军,等. 两种煤在热解过程中汞的析出和形态分布实验研究[J]. 燃料化学学报,2010,38(2):134-139. LIU Ling,DUAN Yufeng,WANG Yunjun,et al. Experimental study on mercury release behavior and speciation during pyrolysis of two different coals[J]. Journal of Fuel Chemistry and Technology,2010,38(2):134-139.
[9] EOM Y,JEON S H,NGO T A,et al. Heterogeneous mercury reaction on a selective catalytic reduction (SCR) catalyst[J]. Catalysis Letters,2008,121(3):219-225.
[10] 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.
[11] JIN B,WEN L,LI C Z,et al. Influences of minerals transformation on the reactivity of high temperature char gasification[J]. Fuel Processing Technology,2010,91(4):404-409.
[12] BROWN T,SMITH D,HARGIS R,et al. Mercury measurement and its control:what we know,have learned,and need to further investigate[J]. Power System Engineering,1999,49(6):1-97.
[13] 任建莉,周劲松,骆仲泱,等. 燃煤电站汞排放分布及控制研究的进展[J]. 电站系统工程,2006,22(1):44-46. REN Jianli,ZHOU Jingsong,LUO Zhongyang,et al. Study of mercury emission during coal combustion[J]. Power System Engineering,2006,22(1):44-46.
[14] ZHOU J,LUO Z,HU Changxing,et al. Factors impacting gaseous mercury speciation in postcombustion[J]. Energy & Fuels,2006,21(2):491-495.
[15] DRANGA B A,LAZAR L,KOESER H. Oxidation catalysts for elemental mercury in flue gase——a review[J]. Catalysts,2012,2(1):139-170.
[16] 顾海明,沈来宏,吴家桦,等. 基于赤铁矿载氧体的煤化学链燃烧试验[J]. 化工学报,2011,62(1):179-185. GU Haiming,SHEN Laihong,WU Jiahua,et al. Experiments on chemical looping combustion of coal with hematite as oxygen carrier[J]. CIESC Journal,2011,62(1):179-185.
[17] WIDMER N C,WEST J. Themmochemical study of mercury oxidation in utility boiler fuel gases[C]//Proceedings of the Air and Waste Management Association's 93rd Annual Meeting. Salt Lake City:Air and Waste Management Association,2000.
[18] FERNÁNDEZ-MIRANDA N,LOPEZ-ANTON M A,DÍAZ-SOMOANO M,et al. Effect of oxy-combustion flue gas on mercury oxidation[J]. Environmental Science & Technology,2014,48(12):7164.
[19] NIKSA S,HELBLE J J,FUJIWARA N. Kinetic modeling of homogeneous mercury oxidation: the importance of NO and H₂O in predicting oxidation in coal-derived systems[J]. Environmental Science & Technology,2001,35(18):3701.

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

Characterization of mercury releasing during reduction of oxygen carriers with coal in chemical looping combustion

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]	高雨飞, 鲁金凤. 非均相催化臭氧氧化作用机理研究进展[J]. 化工进展, 2023, 42(S1): 430-438.
[2]	王乐乐, 杨万荣, 姚燕, 刘涛, 何川, 刘逍, 苏胜, 孔凡海, 朱仓海, 向军. SCR脱硝催化剂掺废特性及性能影响[J]. 化工进展, 2023, 42(S1): 489-497.
[3]	邓丽萍, 时好雨, 刘霄龙, 陈瑶姬, 严晶颖. 非贵金属改性钒钛基催化剂NH₃-SCR脱硝协同控制VOCs[J]. 化工进展, 2023, 42(S1): 542-548.
[4]	罗成, 范晓勇, 朱永红, 田丰, 崔楼伟, 杜崇鹏, 王飞利, 李冬, 郑化安. 中低温煤焦油加氢反应器不同分配器中液体分布的CFD模拟[J]. 化工进展, 2023, 42(9): 4538-4549.
[5]	赖诗妮, 江丽霞, 李军, 黄宏宇, 小林敬幸. 含碳掺氨燃料的研究进展[J]. 化工进展, 2023, 42(9): 4603-4615.
[6]	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.
[7]	王晋刚, 张剑波, 唐雪娇, 刘金鹏, 鞠美庭. 机动车尾气脱硝催化剂Cu-SSZ-13的改性研究进展[J]. 化工进展, 2023, 42(9): 4636-4648.
[8]	张启, 赵红, 荣峻峰. 质子交换膜燃料电池中氧还原反应抗毒性电催化剂研究进展[J]. 化工进展, 2023, 42(9): 4677-4691.
[9]	葛全倩, 徐迈, 梁铣, 王凤武. MOFs材料在光电催化领域应用的研究进展[J]. 化工进展, 2023, 42(9): 4692-4705.
[10]	雷伟, 姜维佳, 王玉高, 和明豪, 申峻. N、S共掺杂煤基碳量子点的电化学氧化法制备及用于Fe³⁺检测[J]. 化工进展, 2023, 42(9): 4799-4807.
[11]	宋伟涛, 宋慧平, 范朕连, 樊飙, 薛芳斌. 粉煤灰在防腐涂料中的研究进展[J]. 化工进展, 2023, 42(9): 4894-4904.
[12]	朱传强, 茹晋波, 孙亭亭, 谢兴旺, 李长明, 高士秋. 固体高分子脱硝剂选择性非催化还原NO _x 特性[J]. 化工进展, 2023, 42(9): 4939-4946.
[13]	杨莹, 侯豪杰, 黄瑞, 崔煜, 王兵, 刘健, 鲍卫仁, 常丽萍, 王建成, 韩丽娜. 利用煤焦油中酚类物质Stöber法制备碳纳米球用于CO₂吸附[J]. 化工进展, 2023, 42(9): 5011-5018.
[14]	张丽宏, 金要茹, 程芳琴. 煤气化渣资源化利用[J]. 化工进展, 2023, 42(8): 4447-4457.
[15]	王耀刚, 韩子姗, 高嘉辰, 王新宇, 李思琪, 杨全红, 翁哲. 铜基催化剂电还原二氧化碳选择性的调控策略[J]. 化工进展, 2023, 42(8): 4043-4057.