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煤化学链燃烧中氧诱导的元素汞氧化

Oxygen-Induced Elemental Mercury Oxidation in Chemical Looping Combustion of Coal.

作者信息

Liu Qiuqi, Liu Dunyu, Ni Mingguo, Xu Kailong, Ma Jingjing, Liu Zhuang, Jin Jing, Shi Huancong

机构信息

School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.

Shanghai Key Laboratory of Multiphase Flow and Heat Transfer in Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China.

出版信息

ACS Omega. 2022 Jun 6;7(24):20959-20967. doi: 10.1021/acsomega.2c01709. eCollection 2022 Jun 21.

DOI:10.1021/acsomega.2c01709
PMID:35755379
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9219527/
Abstract

Mercury emission is an important issue during chemical looping combustion (CLC) of coal. The aim of this work is to explore the effects of different flue gas components (e.g., HCl, NO, SO, and CO) on mercury transformation in the flue gas cooling process. A two-stage simulation method is used to reveal the reaction mechanism of these gases affecting elemental mercury (Hg) oxidation. Furthermore, using this method, Hg oxidation by eight oxygen carriers (CoO, CaSO, CeO, FeO, AlO, MnO, SiO, and CuO) commonly used in CLC are investigated and their Hg oxidation efficiencies were compared with the existing experimental results. The results show that HCl, NO, and CO promote Hg oxidation during flue gas cooling, while SO inhibits Hg oxidation. The stronger the oxygen release capacity of oxygen carriers, the higher the oxidation efficiency of Hg becomes. The order of Hg removal efficiency from high to low is CoO, CuO, MnO, CaSO, FeO, CeO, AlO, and SiO, and this sequence is in good agreement with the existing experimental results. Different flue gas components directly or indirectly affect the O content, thus affecting the content of gaseous oxidized mercury (Hg). Different oxygen carriers have different oxygen release capacities and different Hg oxidation efficiencies. Therefore, O is the core species affecting the mercury transformation in CLC.

摘要

汞排放是煤化学链燃烧(CLC)过程中的一个重要问题。本工作的目的是探讨不同烟气成分(如HCl、NO、SO和CO)在烟气冷却过程中对汞转化的影响。采用两阶段模拟方法揭示这些气体影响元素汞(Hg)氧化的反应机理。此外,利用该方法研究了CLC中常用的八种氧载体(CoO、CaSO、CeO、FeO、AlO、MnO、SiO和CuO)对Hg的氧化作用,并将它们的Hg氧化效率与现有的实验结果进行了比较。结果表明,HCl、NO和CO在烟气冷却过程中促进Hg氧化,而SO抑制Hg氧化。氧载体的氧释放能力越强,Hg的氧化效率越高。Hg脱除效率从高到低的顺序为CoO、CuO、MnO、CaSO、FeO、CeO、AlO和SiO,这一顺序与现有的实验结果吻合良好。不同的烟气成分直接或间接影响O含量,进而影响气态氧化汞(Hg)的含量。不同的氧载体具有不同的氧释放能力和不同的Hg氧化效率。因此,O是影响CLC中汞转化的核心物种。

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Oxygen-Induced Elemental Mercury Oxidation in Chemical Looping Combustion of Coal.煤化学链燃烧中氧诱导的元素汞氧化
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本文引用的文献

1
CO capturing methods: Chemical looping combustion (CLC) as a promising technique.CO 捕集方法:化学链燃烧(CLC)是一种很有前途的技术。
Sci Total Environ. 2021 Sep 20;788:147850. doi: 10.1016/j.scitotenv.2021.147850. Epub 2021 May 19.
2
Impact of gas impurities on the Hg oxidation on high iron and calcium coal ash for chemical looping combustion.气体杂质对化学链燃烧中高铁钙煤灰汞氧化的影响。
Environ Sci Pollut Res Int. 2021 Sep;28(34):46130-46146. doi: 10.1007/s11356-020-11872-z. Epub 2021 Jan 6.
3
Release characteristics of mercury in chemical looping combustion of bituminous coal.
在烟煤的化学链燃烧中汞的释放特性。
J Environ Sci (China). 2020 Aug;94:197-203. doi: 10.1016/j.jes.2020.03.017. Epub 2020 May 7.
4
Fate of Mercury in Volatiles and Char during in Situ Gasification Chemical-Looping Combustion of Coal.煤的原位气体化化学-循环燃烧过程中挥发分和炭中的汞的命运。
Environ Sci Technol. 2019 Jul 2;53(13):7887-7892. doi: 10.1021/acs.est.8b06931. Epub 2019 Jun 20.
5
A critical review on the heterogeneous catalytic oxidation of elemental mercury in flue gases.关于烟气中元素汞的多相催化氧化的批判性回顾。
Environ Sci Technol. 2013 Oct 1;47(19):10813-23. doi: 10.1021/es402495h. Epub 2013 Sep 17.