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The fate of sulphur in the Cu-based Chemical Looping with Oxygen Uncoupling (CLOU) Process

Author

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  • Adánez-Rubio, Iñaki
  • Abad, Alberto
  • Gayán, Pilar
  • García-Labiano, Francisco
  • de Diego, Luis F.
  • Adánez, Juan

Abstract

The Chemical Looping with Oxygen Uncoupling (CLOU) process is a type of Chemical Looping Combustion (CLC) technology that allows the combustion of solid fuels with air, as with conventional combustion, through the use of oxygen carriers that release gaseous oxygen inside the fuel reactor. The aim of this work was to study the behaviour of the sulphur present in fuel during CLOU combustion. Experiments using lignite as fuel were carried out in a continuously operated 1.5kWth CLOU unit during more than 15h. Particles containing 60wt.% CuO on MgAl2O4, prepared by spray drying, were used as the oxygen carrier in the CLOU process. The temperature in the fuel reactor varied between 900 and 935°C. CO2 capture, combustion efficiency and the sulphur split between fuel and air reactor streams in the process were analysed. Complete combustion of the fuel to CO2 and H2O was found in all experiments. Most of the sulphur introduced with the fuel exited as SO2 at the fuel reactor outlet, although a small amount of SO2 was measured at the air reactor outlet. The SO2 concentration in the air reactor exit flow decreased as the temperature in the fuel reactor increased. A carbon capture efficiency of 97.6% was achieved at 935°C, with 87.9wt.% of the total sulphur exiting as SO2 in the fuel reactor. Both the reactivity and oxygen transport capacity of the oxygen carrier were unaffected during operation with a high sulphur content fuel, and agglomeration problems did not occur. Predictions were calculated regarding the use of a carbon separation system in the CLOU process in order to reduce sulphur emissions. Coals with high sulphur content, such as lignite and anthracite, would require a carbon separation system in order to comply with legislation governing sulphur-limits. In conclusion, coals with a high sulphur content can be burnt in a CLOU process using Cu-based material to obtain high carbon capture efficiencies.

Suggested Citation

  • Adánez-Rubio, Iñaki & Abad, Alberto & Gayán, Pilar & García-Labiano, Francisco & de Diego, Luis F. & Adánez, Juan, 2014. "The fate of sulphur in the Cu-based Chemical Looping with Oxygen Uncoupling (CLOU) Process," Applied Energy, Elsevier, vol. 113(C), pages 1855-1862.
  • Handle: RePEc:eee:appene:v:113:y:2014:i:c:p:1855-1862
    DOI: 10.1016/j.apenergy.2013.06.022
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    1. Abad, Alberto & Pérez-Vega, Raúl & de Diego, Luis F. & García-Labiano, Francisco & Gayán, Pilar & Adánez, Juan, 2015. "Design and operation of a 50kWth Chemical Looping Combustion (CLC) unit for solid fuels," Applied Energy, Elsevier, vol. 157(C), pages 295-303.
    2. Samuel C. Bayham & Andrew Tong & Mandar Kathe & Liang-Shih Fan, 2016. "Chemical looping technology for energy and chemical production," Wiley Interdisciplinary Reviews: Energy and Environment, Wiley Blackwell, vol. 5(2), pages 216-241, March.
    3. Chung, Cheng & Pottimurthy, Yaswanth & Xu, Mingyuan & Hsieh, Tien-Lin & Xu, Dikai & Zhang, Yitao & Chen, Yu-Yen & He, Pengfei & Pickarts, Marshall & Fan, Liang-Shih & Tong, Andrew, 2017. "Fate of sulfur in coal-direct chemical looping systems," Applied Energy, Elsevier, vol. 208(C), pages 678-690.
    4. Hamers, H.P. & Romano, M.C. & Spallina, V. & Chiesa, P. & Gallucci, F. & van Sint Annaland, M., 2015. "Boosting the IGCLC process efficiency by optimizing the desulfurization step," Applied Energy, Elsevier, vol. 157(C), pages 422-432.
    5. Wang, Zhe & Fan, Weiyu & Zhang, Guangqing & Dong, Shuang, 2016. "Exergy analysis of methane cracking thermally coupled with chemical looping combustion for hydrogen production," Applied Energy, Elsevier, vol. 168(C), pages 1-12.
    6. Abad, Alberto & Adánez, Juan & Gayán, Pilar & de Diego, Luis F. & García-Labiano, Francisco & Sprachmann, Gerald, 2015. "Conceptual design of a 100MWth CLC unit for solid fuel combustion," Applied Energy, Elsevier, vol. 157(C), pages 462-474.
    7. Bayham, Samuel & McGiveron, Omar & Tong, Andrew & Chung, Elena & Kathe, Mandar & Wang, Dawei & Zeng, Liang & Fan, Liang-Shih, 2015. "Parametric and dynamic studies of an iron-based 25-kWth coal direct chemical looping unit using sub-bituminous coal," Applied Energy, Elsevier, vol. 145(C), pages 354-363.
    8. García-Labiano, F. & de Diego, L.F. & Gayán, P. & Abad, A. & Cabello, A. & Adánez, J. & Sprachmann, G., 2014. "Energy exploitation of acid gas with high H2S content by means of a chemical looping combustion system," Applied Energy, Elsevier, vol. 136(C), pages 242-249.
    9. Adánez-Rubio, Iñaki & Abad, Alberto & Gayán, Pilar & García-Labiano, Francisco & de Diego, Luis F. & Adánez, Juan, 2017. "Coal combustion with a spray granulated Cu-Mn mixed oxide for the Chemical Looping with Oxygen Uncoupling (CLOU) process," Applied Energy, Elsevier, vol. 208(C), pages 561-570.
    10. Zhang, Yongliang & Jin, Bo & Zou, Xixian & Zhao, Haibo, 2016. "A clean coal utilization technology based on coal pyrolysis and chemical looping with oxygen uncoupling: Principle and experimental validation," Energy, Elsevier, vol. 98(C), pages 181-189.
    11. Imtiaz, Qasim & Broda, Marcin & Müller, Christoph R., 2014. "Structure–property relationship of co-precipitated Cu-rich, Al2O3- or MgAl2O4-stabilized oxygen carriers for chemical looping with oxygen uncoupling (CLOU)," Applied Energy, Elsevier, vol. 119(C), pages 557-565.

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    Keywords

    CO2 capture; Cu-based oxygen carrier; CLOU; Coal; Sulphur;
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