Silica and Iron Oxide Recovery and Mineral Carbonation from Serpentine Minerals Using Acid Dissolution and pH Swing Processes

산 처리와 pH 조절을 이용한 사문석군 광물로부터 규소와 철산화물 회수 및 광물 탄산화 연구

  • Baek, Jiyeon (Department of Geological and Environmental Sciences, Chonnam National University) ;
  • Jo, Yeonu (Gwangju Science Academy for the Gifted) ;
  • Lee, Jeongheon (Gwangju Science Academy for the Gifted) ;
  • Kwon, Nayoon (Gwangju Science Academy for the Gifted) ;
  • Kim, Yeram (Gwangju Science Academy for the Gifted) ;
  • Choi, Suk (Gwangju Science Academy for the Gifted) ;
  • Kim, Sunghee (Gwangju Science Academy for the Gifted) ;
  • Roh, Yul (Department of Geological and Environmental Sciences, Chonnam National University)
  • 백지연 (전남대학교 지질환경과학과) ;
  • 조연우 (과학영재학교 광주과학고등학교) ;
  • 이정헌 (과학영재학교 광주과학고등학교) ;
  • 권나윤 (과학영재학교 광주과학고등학교) ;
  • 김예람 (과학영재학교 광주과학고등학교) ;
  • 최숙 (과학영재학교 광주과학고등학교) ;
  • 김성희 (과학영재학교 광주과학고등학교) ;
  • 노열 (전남대학교 지질환경과학과)
  • Received : 2015.12.03
  • Accepted : 2016.03.01
  • Published : 2016.02.28


The objectives of this study were to recover silica and iron oxides and $CO_2$ sequestration using serpentine via various acid dissolution and pH swing processes. Serpentine collected from Guhang-myeon in S. Korea were mainly composed of antigorite and magnetite consisting of $SiO_2$ (45.3 wt.%), MgO (41.3 wt.%), $Fe_2O_3$ (12.2 wt.%). Serpentine pulverized ($${\leq_-}75{\mu}m$$) and then dissolved in 3 different acids, HCl, $H_2SO_4$, $HNO_3$. Residues treated with acidic solution were recovered from the solution (step 1). And then the residual solution containing dissolved serpentine was titrated using $NH_4OH$. And pH of the solution increased up to pH=8.6 to obtain reddish precipitates (step 2). After recovery of the precipitates, the residual solution reacted with $CO_2$ and then pH increased up to pH=9.5 to precipitate white materials (step 3). The mineralogical characteristics of the original sample and harvested precipitates were examined by XRD, and TEM-EDS analyses. ICP-AES analysis was also used to investigate solution chemistry. The dissolved ions were Mg, Si, and Fe. The antigorite became noncrystralline silica after acid treatment (step 1). The precipitate at pH=8.6 was mainly amorphous iron oxide, of which size ranged from 2 to 10 nm and mainly consisting of Fe, O, and Si (step 2). At pH=9.5, nesquehonite [$Mg(HCO_3)(OH){\cdot}2(H_2O)$] and lasfordite [$MgCO_3{\cdot}H_2O$] were formed after reaction with $CO_2$ (step 3). The size of carbonated minerals was ranged from 1 to $6{\mu}m$. These results indicated that the acid treatment of serpentine and pH swing processes for the serpentine can be used for synthesis of other materials such as silica, iron oxides and magnesium carbonate. Also, This process may be useful for the precursor synthesis and $CO_2$ sequestration via mineral carbonation.


acid dissolution pH swing;resource recovery;$CO_2$ sequestration;antigorite


Supported by : Korea CCS R&D Center(KCRC)


  1. Faust, G.T. and Fahey, J.J. (1962) The serpentine-group minerals. US Government Printing Office, p.1-92.
  2. Fedorockova, A., Hreus, M., Paschman, P. and Suik, G. (2012) Dissolution of magnesium room calcined serpentinite in hydrochloric acid. Minerals Engineering. v.32, p.1-4.
  3. Fischbeck, R. and Mller, G. (1971) Monohydrocalcite, hydromagnesite, nesquehomite, dolomite, aragonite, and calcite in speleothems of the Frnkische schweiz, western germany. Contributions to Mineralogy and Petrology, v.33, p.87-92.
  4. Giester, G., Lengauer, C.L. and Rieck, B. (2000) The crysral structure of nesquehonite, $MgCO_3{\cdot}3H_2O$, from Lavrion, Greece. Mineralogy and Petrology, v.70, p.153-163.
  5. Hill, R.J., Canterford, J.H. and Moyle, F.J. (1982) New data for lansfordite. Mineralogical Magazine, v.46, p.453-457.
  6. Hwang, J.Y. (2002) Characteristic and Utilization of Serpentine, Journal of The Mineralogical Society of Korea, v.15, n.2, p.48-54.
  7. Jeon, C.W., Chae, S.C., Ryu, K.W., Lee, M.K. and Jang, Y.N. (2010) Activation and Acid Digestion of Discarded-Asbestos as Raw-Material for $CO_2$ Sequestration. The Korean Society of Industrial and Engineering Chemistry, v.14, n.1, p.69-72.
  8. Kloprogge, J.T., Martens, W.N., Nothdurft, L., Duong, L.V. and Webb, G.E. (2003) Low temperature synthesis and characterization of nesquehonite. Journal of Materials Science Letters, v.22, p.825-829.
  9. Kim, B.S., Yu, K.K., Kim, S.K., Kim, M.S. and Lee, J.C., (2008) Leaching Behavior of Magnesium from Serpentine in Hydrochloric Acid Solution. The Korean Society of Mineral and Energy Resources Engineers, v.45, n.6, p.627-634.
  10. Kim, D.J., Jeong, H.S., Lee, J.C., Kim, I.H. and Lee, J.H. (2000) Synthesis of zeolite A from serpentine. Journal of the Korean crystal growth and crystal technology, v.10, n.1, p.73-79.
  11. Krevor, S.C.M. and Lackner, K.S. (2011) Enhancing serpentine dissolution kinetics for mineral carbon dioxide sequestration. International Journal of Greenhouse Gas Control, v.5, p.1073-1080.
  12. Langmuir, D. (1965) Stability of carbonates in the system MgO-$CO_2$-$H_2O$. Journal of Geology, v.73, n.5, p.730-754.
  13. Lippmann, F. (1973) Sedimentary carbonate minerals. Springer-Verlag, New York, p.71-87.
  14. Maroto-Valer, M.M., Fauth, D.J., Kuchta, M.E., Zhang, Y. and Andrsen, J.M. (2005) Activation of magnesium rich minerals as carbonation feedstock materials for $CO_2$ sequestration. Fuel Processing Technology, v.86, p.1627-1645.
  15. Oelkers. E.H., Gislason. S.R. and Matter. J. (2008) Mineral carbonation of $CO_2$. Elements, v.4, p.333-337.
  16. Park, A.H.A. and Fan,L.S. (2004) $CO_2$ mineral sequestration physically activated dissolution of serpentine and pH swing process. Chemical Engineering Science, v.59, p.5241-5247.
  17. Rundsack, F.L. and Somerville, N.J. (1967) Recovery of silica, iron oxide and magnesium carbonate from the treatment of serpentine with ammonium bisulfate. US Patent 3,338,667 to ETRI, Patent and Trandemark office, Washington D. C.
  18. Teir, S., Revitzer, H., Eloneva, S., Fogelholm, C.J. and Zevenhoven, R. (2007) Dissolution of natural serpentinite in mineral and organic acids. International Journal of Mineral Processing, v.83, p.36-46.
  19. Thom, G.M., Dipple, G.M., Power, I.M. and Harrison, A.L. (2013) Chrysotile dissolution rates: Implications for carbon sequestration. Applied Geochemistry, v.35, p.244-254.
  20. Yoo, K.K., Kim, B.S., Kim, M.S., Lee, J.C. and Jeong, J. (2009) Dissolution of magnesium from serpentine mineral in sulfuric acid solution. Materials Transactions, v.50, n.5, p.1225-1230.
  21. Zhang, Q., Sugiyama, K. and Saito, F. (1997) Enhancement of acid extraction of magnesium and silicon from serpentine by mechanochemical treatment. Hydromerallurgy, v.45, p.323-331.