Resources Recycling (자원리싸이클링)

The Korean Institute of Resources Recycling (한국자원리싸이클링학회)
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Carbon Dioxide Storage and Calcium Carbonate Production through Indirect Carbonation Using Paper Sludge Ash and Chelating Reagents

제지슬러지소각재 및 킬레이트제 활용 간접탄산화 방법을 통한 이산화탄소 저장 및 탄산칼슘 생성

  • Jeon, Junhyeok (Department of Convergence Study on the Ocean Science and Technology, Korea Maritime and Ocean University) ;
  • Kim, Myoung-Jin (Department of Environmental Engineering, Korea Maritime and Ocean University)
  • 전준혁 (한국해양대학교 해양과학기술융합학과) ;
  • 김명진 (한국해양대학교 환경공학과)
  • Received : 2019.04.12
  • Accepted : 2019.05.28
  • Published : 2019.06.30
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Abstract

In this study, we conducted experiments to store $CO_2$ and produce $CaCO_3$ through indirect carbonation using paper sludge ash (PSA) and three chelating reagents (fumarate, IDA and EDTA). Fumarate and IDA used as solvents could facilitate the indirect carbonation reaction to store more $CO_2$ than water. When 0.1 M fumarate and IDA were used, $CO_2$ storage was 63 and $89kg-CO_2/ton-PSA$, respectively, and $CaCO_3$ yield was 144 and $202kg-CaCO_3/ton-PSA$. For the case of EDTA, however, the carbonation was hardly progressed. As either the concentration or Ca-ligand stabilization constant of each chelating reagent increased, the calcium extraction efficiency from PSA increased. In addition, the carbonation efficiency was influenced by the Ca-ligand stabilization constant. As the Ca-ligand stabilization constant increased, more calcium could be extracted from the PSA. With the constant larger than that of $CaCO_3$ ($10^{8.35}$), however, the carbonation reaction was not proceeded.

본 연구에서는 제지슬러지소각재(PSA)와 세 가지 킬레이트제(fumarate, IDA, EDTA)를 가지고 간접탄산화에 의해 이산화탄소를 저장하고 탄산칼슘을 생성하는 실험을 진행하였다. Fumarate와 IDA를 용제로 사용하면 간접탄산화반응이 촉진되어 물을 사용했을 때보다 더 많은 양의 이산화탄소를 저장하였다. 0.1 M 농도의 fumarate와 IDA를 사용했을 때, 이산화탄소 저장량은 각각 63, $89kg-CO_2/ton-PSA$이었고, 탄산칼슘 생성량은 각각 144, $202kg-CaCO_3/ton-PSA$이었다. 그러나 EDTA를 용제로 사용한 경우에는 탄산화반응이 거의 진행되지 않았다. PSA로부터 칼슘용출효율은 킬레이트제의 농도가 높고 Ca-ligand 안정화상수가 클수록 증가하였다. 또한 탄산화효율도 Ca-ligand 안정화상수의 영향을 받았다. Ca-ligand 안정화상수가 클수록 P SA로부터 더 많은 칼슘이 용출되었지만, 이 값이 탄산칼슘의 안정화상수($10^{8.35}$)보다 크면 탄산화반응이 진행되기 어려웠다.

Keywords

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Fig. 1. Constitutional formulas of three ligands: (a) fumarate, (b) IDA, and (c) EDTA.

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Fig. 2. Schematic diagram of the carbonation reactor: 1. CO2 gas cylinder, 2. gas regulator, 3. needle valve, 4. digital mass flow meter, 5. fine control valve, 6. pH meter, 7. pH electrode, 8. electrical stirrer, 9. CO2 outlet.

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Fig. 3. Variations of the (a) calcium and (b) hydroxide ion concentration of eluent with the solvent concentration.

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Fig. 4. Variations of the monitored pH and its time derivative with the carbonation time: (a) 0.1 M fumarate, (b) 0.1 M IDA, (c) 0.1 M EDTA, and (d) water (–●– : monitored pH, —: pH derivative curve).

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Fig. 5. XRD analysis of the solids obtained by using three chelating reagents and water as solvents: (a) 0.1 M fumarate, (b) 0.1 M IDA, (c) 0.1 M EDTA, (d) water, (e) calcite reference, and (f) vaterite reference.

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Fig. 6. SEM analysis of the solids obtained by using three chelating reagents and water as solvents: (a) 0.1 M fumarate, (b) 0.1 M IDA, (c) 0.1 M EDTA, and (d) water.

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Fig. 7. TGA results of the solids obtained by using three chelating reagents and water as solvents: (a) 0.1 M fumarate, (b) 0.1 M IDA, (c) 0.1 M EDTA, and (d) water.

Table 1. Comparison of the calcium extraction efficiency, carbonation efficiency, CO2 storage, CaCO3 yield, and CaCO3 characteristics (morphology, particle size, and purity) among the three chelating reagents and water used as solvents

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