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Ranking Oxygen Carriers for Elemental Mercury Oxidation in Coal-Fired Chemical-Looping Combustion: A Thermodynamic Approach

  • Mingguo Ni
    Mingguo Ni
    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
    More by Mingguo Ni
  • Dunyu Liu*
    Dunyu Liu
    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
    *E-mail: [email protected]
    More by Dunyu Liu
  • Jing Jin
    Jing Jin
    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
    More by Jing Jin
  • Liang Feng
    Liang Feng
    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
    More by Liang Feng
  • , and 
  • Zhuang Liu
    Zhuang Liu
    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
    More by Zhuang Liu
Cite this: Energy Fuels 2020, 34, 2, 2355–2365
Publication Date (Web):January 14, 2020
https://doi.org/10.1021/acs.energyfuels.9b03829
Copyright © 2020 American Chemical Society

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    Abstract

    Oxygen carriers in coal-fired chemical looping combustion can oxidize elemental mercury, but there are still no specific criteria to rank the efficiencies of Hg0 oxidation by classification of different oxygen carriers. Both an experimental approach and thermodynamic modeling were adopted to evaluate the Hg0 oxidation efficiencies in the case of eight commonly used oxygen carriers, applying a temperature range from 800 to 1000 °C. The efficiency of the Hg0 oxidation process in experiments within this temperature range was found to correspond well with the amounts of Cl/Cl2 in the calculated reaction products. Results have shown that the sequence of the amounts of Cl/Cl2 for different oxygen carriers was as follows: CaSO4 > Co3O4 (Mn2O3) > Fe2O3 > CuO (CeO2) > SiO2 (Al2O3). This sequence was in agreement with the simulations of the experiments investigating the efficiency of Hg0 oxidation. According to thermodynamic calculations, the oxidation mechanism of Hg0 can be classified into two categories: MxOy-based mechanisms (Fe2O3, CuO, Co3O4, Mn2O3, CeO2, Al2O3, and SiO2) and CaSO4-based processes. Hg0 oxidation by MxOy follows three reaction pathways. In the first instance, Hg0 can be oxidized by Cl2 to form HgCl2; in the second reaction pathway, Hg0 can be oxidized by Cl to form HgCl, which is oxidized afterward by Cl/Cl2 to HgCl2. In the third reaction pathway, Hg0 is oxidized by oxygen atoms to HgO, which is then oxidized by Cl2O to form HgCl2. In comparison, the oxidation of Hg0 by CaSO4 is different from that of other oxygen carriers with existing additional reaction pathways. Hg0 is converted first to HgS before being oxidized to HgCl2. The approach in this study may be used for choosing the optimum oxygen carriers for Hg0 oxidation in coal-fired chemical-looping combustion processes.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.energyfuels.9b03829.

    • The amount of Cl/Cl2 generated in “fresh oxygen carriers + HCl + Hg0” and “reduced oxygen carriers + HCl + Hg0” systems, reduction of oxygen carriers by different amounts of H2 at 900 °C, contribution ratios of oxygen uncoupling abilities of different oxygen carriers to Cl/Cl2 generation in the system, the 670 detailed reactions in this paper, bond energies of metal chlorides, and thermal dissociation temperatures corresponding to the pure mercury compounds (PDF)

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    Cited By

    This article is cited by 17 publications.

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    2. Chaoran Wang, Dunyu Liu, Kailong Xu, Jing Jin, Jingjing Ma. Enhancement of Elemental Mercury Oxidation by Core–Shell CuCo2O4@SiO2 Oxygen Carrier with Strong Oxygen Release and Weak Adsorption Capacity in Chemical-Looping Combustion. Energy & Fuels 2023, 37 (24) , 19664-19679. https://doi.org/10.1021/acs.energyfuels.3c02821
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    6. Zhuang Liu, Jinsong Zhou, Lingtao Zhou, Bohao Li, Tang Wang, Haoyun Liu. A review on mercury removal in chemical looping combustion of coal. Separation and Purification Technology 2024, 337 , 126352. https://doi.org/10.1016/j.seppur.2024.126352
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    8. Zhuang Liu, Jinsong Zhou, Qixin Zhou, Lingtao Zhou, Yang Lu, Bohao Li, Tang Wang. Inhibition of insoluble HgS and HgO generation and promotion of easy-soluble HgCl2 production for the solution washing regeneration of mercury adsorbent in syngas. Separation and Purification Technology 2023, 325 , 124640. https://doi.org/10.1016/j.seppur.2023.124640
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    10. Mei An, Qingjie Guo, Xianyong Wei. Reaction mechanism of H2S with Hg0 on CuFe2O4 oxygen carrier with oxygen vacancy structure during coal chemical looping gasification. Fuel 2023, 333 , 126477. https://doi.org/10.1016/j.fuel.2022.126477
    11. Amr Abdalla, Mohanned Mohamedali, Nader Mahinpey. Recent progress in the development of synthetic oxygen carriers for chemical looping combustion applications. Catalysis Today 2023, 407 , 21-51. https://doi.org/10.1016/j.cattod.2022.05.046
    12. Dunyu Liu, Kailong Xu, Jingjing Ma, Qiuqi Liu, Yunpei Fan, Chaoran Wang, Xudong Wang, Jing Jin, Huancong Shi. Advances in rational design of catalysts for efficient Hg0 removal. Fuel 2023, 331 , 125922. https://doi.org/10.1016/j.fuel.2022.125922
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    14. Alhadi Ishag, Yanxue Yue, Jingting Xiao, Xinshui Huang, Yubing Sun. Recent advances on the adsorption and oxidation of mercury from coal-fired flue gas: A review. Journal of Cleaner Production 2022, 367 , 133111. https://doi.org/10.1016/j.jclepro.2022.133111
    15. Hongming Jiang, Ruiqiang Huo, Zhen Zhang, Yan Lin, Zengli Zhao, Zhen Huang, Yitian Fang, Haibin Li. Removal of pollution from the chemical looping process: A mini review. Fuel Processing Technology 2021, 221 , 106937. https://doi.org/10.1016/j.fuproc.2021.106937
    16. Zhuang Liu, Dunyu Liu, Jing Jin, Liang Feng, Mingguo Ni, Bingtao Zhao, Xiaojiang Wu. Impact of gas impurities on the Hg0 oxidation on high iron and calcium coal ash for chemical looping combustion. Environmental Science and Pollution Research 2021, 28 (34) , 46130-46146. https://doi.org/10.1007/s11356-020-11872-z
    17. Jinchen Ma, Xin Tian, Bo Zhao, Xiaoshan Li, Yongchun Zhao, Haibo Zhao, Chuguang Zheng. Behavior of mercury in chemical looping with oxygen uncoupling of coal. Fuel Processing Technology 2021, 216 , 106747. https://doi.org/10.1016/j.fuproc.2021.106747

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