Abstract
In this paper, waste gypsum from wet flue gas desulfurization (WFGD) mixed with NH3·H2O was applied for CO2 absorption in the solid-liquid-gas phase system. The effects of operation temperature, CO2 flow rates, and ammonia-to-gypsum ratio on carbonation process were discussed. Meanwhile, a model for CO2 absorption in the suspension of WFGD gypsum and ammonia was established. The results indicate that higher temperature favors the reaction, and WFGD gypsum conversion can be achieved above 90% even at lower ammonia-to-gypsum ratio, while CO2 conversion reaches 90% and ammonia utilization is up to 83.69%. The model fits well with the experimental results at various CO2 flow rates and predicts the concentration distribution of the main species, including CO2 absorbed, NH2COO−, and HCO3 −.
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Abbreviations
- A, B :
-
Decbye–Hückel constants
- CO2T :
-
Total CO2 concentration (mol L−1)
- D :
-
Diffusion coefficient (m2 s−1)
- e0 :
-
Unit charge (C)
- F :
-
Faraday constant (C mol−1)
- I :
-
Ionic strength (mol L−1)
- K b :
-
Chemical equilibrium constant of ammonia hydrolysis reaction
- K N :
-
Chemical equilibrium constant of CO2 absorption reaction
- K 1 :
-
Chemical equilibrium constant of reaction (14*)
- K sp :
-
Solubility product
- k 1 :
-
Kinetics parameter of the elementary reaction (9*) (L mol s−1)
- k OH :
-
Kinetics parameter of the elementary reaction (14*) (mol L s−1)
- \( {m}_{0,\ {\mathrm{CaCO}}_3} \) :
-
Initial mass of calcium carbonate in the gypsum (g)
- NH3T :
-
Total ammonia concentration (mol L−1)
- p :
-
Ambient pressure (Pa)
- \( {\mathrm{P}}_{{\mathrm{CaCO}}_3} \) :
-
Calcium carbonate content (%)
- PC :
-
Carbon content (%)
- \( {\mathrm{P}}_{{\mathrm{CaSO}}_4} \) :
-
Calcium sulfate content (%)
- R :
-
Gas constant (J mol K−1)
- R a :
-
Reaction rate of fast CO2 absorption (mol L s−1)
- R d :
-
Reaction rate of gypsum dissolution (mol L s−1)
- R h :
-
Reaction rate of ammonium carbamate hydrolysis (mol L s−1)
- r a :
-
Linearized reaction rate of CO2 absorption (mol L s−1)
- r d :
-
Linearized reaction rate of gypsum dissolution (mol L s−1)
- r h :
-
Linearized reaction rate of ammonium carbamate hydrolysis (mol L s−1)
- T :
-
Ambient temperature (K)
- t :
-
Contact time (min)
- \( {\mathrm{V}}_{{\mathrm{CO}}_2} \) :
-
Amount of CO2 uptake (mol)
- v :
-
Flow rate (mL min−1)
- y a, y b, y c, y d., y e :
-
Molar concentration of CO2, NH3, NH2COO−, NH4 +, and HCO3 − (mol L−1)
- z :
-
Charge number
- \( {\eta}_{{\mathrm{CO}}_2} \) :
-
CO2 conversion (%)
- NH3(aq) :
-
Aqueous ammonia conversion (%)
- η gyp :
-
Gypsum conversion (%)
- γ :
-
The activity coefficients for ionics
- ε :
-
Dielectric constants (F m−1)
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Acknowledgements
This work was supported by the National Natural Science Funds of China (grants no. 51678291 and no. 21207064) and Scientific Research Project of Environmental Protection Department of Jiangsu Province (2015015). Also, the authors thank Qing Lan Project of Jiangsu Province for funds provided.
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Tan, W., Zhang, Z., Li, H. et al. Carbonation of gypsum from wet flue gas desulfurization process: experiments and modeling. Environ Sci Pollut Res 24, 8602–8608 (2017). https://doi.org/10.1007/s11356-017-8480-0
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DOI: https://doi.org/10.1007/s11356-017-8480-0