Adsorptive Removal of Aqueous Arsenic Using Nanoparticles of Iron Hydroxides

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2011 Vol.48, Issue 4 Preview Page Next Page

Adsorptive Removal of Aqueous Arsenic Using Nanoparticles of Iron Hydroxides 철수산화물 나노입자를 이용한 수용액 내 비소의 흡착처리 연구: 김현종, 전효택, 이종운, 노열
Hyun-Jong Kim, Hyo-Taek Chon, Jong-Un Lee and Yul Roh

31 August 2011. pp. 438-447

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Abstract

Adsorptive removal of aqueous As(III) and As(V) was investigated using nano-sized iron hydroxides, i.e., akaganeite (β-FeOOH) and ferrihydrite (Fe5HO8·4H2O), as adsorbents which were synthesized in laboratory. The removal efficiency was compared with that of micro-sized iron hydroxide, goethite (α-FeOOH). SEM analysis showed that the diameter of the synthesized nanoparticles ranged 10~100 nm with maximum of 150 nm. Through a potentiometric titration technique, the points of zero charge of akaganeite and ferrihydrite appeared to be 7.8 and 8.5, respectively. Akaganeite led to maximum adsorbed concentrations of As(III) and As(V) at pH 8 and pH 5, respectively, and at pH 7 and pH 3, respectively, for ferrihydrite. When pH increased over 8.5, the adsorption efficiency dropped rapidly. Both nanoparticles kinetically reached adsorption equilibrium within two hours. Nanoparticles of akaganeite and ferrihydrite resulted in higher adsorption efficiency than goethite. When As solution was amended with the nanoparticles of 3.6 g/L, most aqueous As was removed from solution.

Keywords

Nanoparticle

Akaganeite

Ferrihydrite

Goethite

Groundwater

합성한 나노크기의 철수산화물 akaganeite(β-FeOOH)와 ferrihydrite(Fe5HO8·4H2O)를 흡착제로 이용한 As(III) 및 As(V)의 제거 실험을 수행하였으며 제거효율 비교를 위해 마이크로크기의 goethite(α-FeOOH)와의 비교 실험을 수행하였다. SEM 분석 결과 합성된 나노입자는 10~100 nm의 평균 입경을 가졌고 최대 150 nm 이하로 존재하였다. 전위차 적정을 이용한 영전하점 측정 결과 akaganeite와 ferrihydrite의 영전하점은 각각 7.8과 8.5로 측정되었다. Akaganeite를 사용한 경우 As(III)는 pH 8, As(V)는 pH 5에서, ferrihydrite의 경우 As(III)는 pH 7, As(V)는 pH 3에서 가장 높은 흡착 농도를 보였으며 pH가 8.5 이상이 되면 흡착 효율이 감소하였다. 비소의 두 화학종 모두에서 나노입자를 사용한 경우가 마이크로 입자에 비하여 더 높은 흡착 효율을 보였으며, 3.6 g/L의 나노입자 투입으로 거의 모든 비소가 용액으로부터 제거되었다.

키워드

나노입자

비소

Akaganeite

Ferrihydrite

Goethite

지하수

References

고일원, 이상우, 김주용, 김경웅, 이철효, 2004, “나노크기 적철석 입자 피복 모래를 이용한 비소 3가와 비소 5가의 제거,” 지하수토양환경, 제9권 1호, pp. 63-69.
선은영, 김유미, 박병노, 노열, 2010, “금속환원미생물과 나노크기 철광물을 이용한 이온상태로 존재하는 비소의 고정,” 2010년 춘계 지질과학기술 공동학술대회 논문집, 대한자원환경지질학회․대한지질학회․한국석유지질학회, 대구, 4월 28일～30일, pp. 106-107.
이상은, Heins, U.N., 박준규, 임수길, 1994, “Utisol과 Alfisol 및 Inceptisol 토양에서 토양표면전하 측정에 사용된 이온흡착법: 전위차 적정법 및 역적정법의 비교,” 한국토양비료학회지, 제 26권 3호, pp. 160-171.
정영일, 이우춘, 조현구, 윤성택, 김순오, 2008, “비소의 two-line ferrihydrite에 대한 흡착반응,” 한국광물학회지, 제 21권 3호, pp. 227-237.
정우식, 지민규, 이상훈, Kumar, E., Bhatnagar, A., 김선준, 전병훈, 2008, “GFH(granular ferric hydroxide)를 이용한 불소 흡착연구,” 한국지구시스템공학회지, 제 45권 5호, pp. 441-447.
정현수, 2009, 비소의 철수산화물의 흡착특성 연구, 석사학위논문, 경상대학교대학원, 진주.
최영무, 2007, “나노 크기의 Mg․Fe layered double hydroxide를 이용한 5가 비소 흡착 특성 연구,” 2007년 대한환경공학회․한국대기환경학회․한국폐기물학회 환경공동학술대회 초록집, 부산, 5월 2일～4일, p. 387.
Deliyanni, E.A., Bakoyannakis, D.N., Zouboulis, A.I. and Matis, K.A., 2003, “Sorption of As(V) ions by akaganeite type nanocrystals,” Chemosphere, Vol. 50, pp. 155-163.
Deliyanni, E.A., Nalbandian, L.K. and Matis, A., 2006, “Adsorptive removal of arsenites by a nanocrystalline hybrid surfactantakaganeite sorbent,” Journal of Colloid and Interface Science, Vol. 302, No. 2, pp. 458-466.
Dousova, B., Grygar, T., Martaus, A., Fuitova, L., Kolousek, D. and Machovi, V., 2006, “Sorption of As(V) on aluminosilicate treated with Fe(II) nanoparticles,” Journal of Colloid and Interface Science, Vol. 302, No. 2, pp. 424-431.
Fendrof, S., Eick, M.J., Grossl, P. and Sparks, D.L., 1997, “Arsenate and chromate retention mechanism on goethite,” Environmental Science and Technology, Vol. 31, No. 2, pp. 315-320.
He, Y.T. and Traina, S.J., 2005, “Cr(VI) reduction and immobilization by magnetite under alkaline pH condition: the role of passivation,” Environmental Science and Technology, Vol. 31, pp. 321-326.
Hristovski, K., Baumgardener, A. and Westerhoff, P., 2007, “Selecting metal oxide nanomaterials for arsenic removal in fixed bed column,” Journal of Hazardous Materials, Vol. 147, No. 1-2, pp. 265-274.
Huang, Y.H., Hsueh, C.I., Cheng, H.P., Su, L.C. and Chen, C.Y., 2006, “Thermodynamics and kinetics of adsorption of Cu(II) onto iron oxide,” Journal of Hazardous Materials, Vol. 144, pp. 406-411.
Jain, A., Raven, K. and Leoppert, R.H., 1999, “Arsenite and arsenate adsorption on ferrihydrite,” Environmental Science and Technology, Vol. 33, pp. 1179-1184.
Johnson, B.B., 1990, “Effect of pH, temperature and concentration on the adsorption of cadmium on goethite,” Environmental Science and Technology, Vol. 24, pp. 112-118.
Kanel, S.R., Greneche, J.M. and Choi, H., 2006, “As(V) removal from groundwater using nanoscale zerovalent iron as a colloidal reactive barrier material,” Environmental Science and Technology, Vol. 40, pp. 2040-2045.
Kraepiel, A.M., Keller, K. and Morel, F., 1998, “On the acid-base chemistry of permanently charged minerals,” Environmental Science and Technology, Vol. 32, No. 19, pp. 2829-2838.
Martinson, C.A. and Reddy, K.J., 2009, “Adsorption of arsenic(III) and arsenic(V) by cupric oxide nanoparticles,” Journal of Colloid and Interface Science, Vol. 336, No. 2, pp. 406-411.
Mayo, J.T., Yavuz, C., Yean, S., Cong, L., Shipley, H., Yu, W., Faljner, J., Kan, A., Tomson, M. and Colvin, V.L., 2007, “The effect of nanocrystalline magnetite size on arsenic removal,” Science and Technology of Advanced Materials, Vol. 8, pp. 71-75.
Nowack, B., Lutzenkirchen, J., Behra, P. and Sigg, L., 1996, “Modeling the adsorption of metal-EDTA complexes onto oxides,” Environmental Science and Technology, Vol. 30, No. 7, pp. 2397-2405.
Nriagu, J.O. (Ed.), 1994, Arsenic in the Environment, John Wiley&Sons, New York, USA. Park, H., Myung, N.V., Jung, H. and Choi, H., 2009, “As(V) remediation using electrochemically synthesized maghemite nanoparticles,” The Journal of Nanoparticle Research, Vol. 11, No. 8, pp. 1981-1989.
Pena, M.E., Koratis, G.P., Patel, M., Lippincott, L. and Meng, X., 2005, “Adsorption of As(V) and As(III) by nanocrystalline titanium dioxide,” Water Research, Vol. 39, pp. 2327-2337.
Pokhrel, D. and Viraraghavan, T., 2007, “Arsenic removal in iron oxide coated fungal biomass coulmn,” Bioresources Technology, Vol. 99, No. 6, pp. 2067-2071.
Rietra, R., Hiemstra, T. and Riemsdijk, W.H., 2001, “Interaction between calcium and phosphate adsorption on goethite,” Environmental Science and Technology, Vol. 35, No. 16, pp. 3369-3374.
Schwertmann, U. and Cornell R.M., 2000, Iron Oxides in the Laboratory: Preparation and Characterization, Wiley-VCH, New York, USA, pp. 103-122.
Sharma, Y.C., Srivastava, V., Singh, K.S.N. and Weng, C.H., 2009, “Nano-adsorbents for removal of metallic pollutants from water and wastewater,” Environmental Technology, Vol. 30, pp. 583-609.
Tuutijarvi, T., Lu, J., Sillanpaa M. and Chen, G., 2009, “As(V) adsorption on maghemite nanoparticles,” Journal of Hazardous Materials, Vol. 166, No. 2-3, pp. 1415-1420.
Zhu, H., Jia, Y., Wu, X. and Wang, H., 2009, “Removal of arsenic from water by supported nano zero-valent iron on activated carbon,” Journal of Hazardous Materials, Vol. 172, No. 2-3, pp. 1591-1596.

Information

Publisher :The Korean Society of Mineral and Energy Resources Engineers
Publisher(Ko) :한국자원공학회
Journal Title :Journal of the Korean Society for Geosystem Engineering
Journal Title(Ko) :한국지구시스템공학회지
Volume : 48
No :4
Pages :438-447

[1] 고일원, 이상우, 김주용, 김경웅, 이철효, 2004, “나노크기 적철석 입자 피복 모래를 이용한 비소 3가와 비소 5가의 제거,” 지하수토양환경, 제9권 1호, pp. 63-69.

[2] 선은영, 김유미, 박병노, 노열, 2010, “금속환원미생물과 나노크기 철광물을 이용한 이온상태로 존재하는 비소의 고정,” 2010년 춘계 지질과학기술 공동학술대회 논문집, 대한자원환경지질학회․대한지질학회․한국석유지질학회, 대구, 4월 28일～30일, pp. 106-107.

[3] 이상은, Heins, U.N., 박준규, 임수길, 1994, “Utisol과 Alfisol 및 Inceptisol 토양에서 토양표면전하 측정에 사용된 이온흡착법: 전위차 적정법 및 역적정법의 비교,” 한국토양비료학회지, 제 26권 3호, pp. 160-171.

[4] 정영일, 이우춘, 조현구, 윤성택, 김순오, 2008, “비소의 two-line ferrihydrite에 대한 흡착반응,” 한국광물학회지, 제 21권 3호, pp. 227-237.

[5] 정우식, 지민규, 이상훈, Kumar, E., Bhatnagar, A., 김선준, 전병훈, 2008, “GFH(granular ferric hydroxide)를 이용한 불소 흡착연구,” 한국지구시스템공학회지, 제 45권 5호, pp. 441-447.

[6] 정현수, 2009, 비소의 철수산화물의 흡착특성 연구, 석사학위논문, 경상대학교대학원, 진주.

[7] 최영무, 2007, “나노 크기의 Mg․Fe layered double hydroxide를 이용한 5가 비소 흡착 특성 연구,” 2007년 대한환경공학회․한국대기환경학회․한국폐기물학회 환경공동학술대회 초록집, 부산, 5월 2일～4일, p. 387.

[8] Deliyanni, E.A., Bakoyannakis, D.N., Zouboulis, A.I. and Matis, K.A., 2003, “Sorption of As(V) ions by akaganeite type nanocrystals,” Chemosphere, Vol. 50, pp. 155-163.

[9] Deliyanni, E.A., Nalbandian, L.K. and Matis, A., 2006, “Adsorptive removal of arsenites by a nanocrystalline hybrid surfactantakaganeite sorbent,” Journal of Colloid and Interface Science, Vol. 302, No. 2, pp. 458-466.

[10] Dousova, B., Grygar, T., Martaus, A., Fuitova, L., Kolousek, D. and Machovi, V., 2006, “Sorption of As(V) on aluminosilicate treated with Fe(II) nanoparticles,” Journal of Colloid and Interface Science, Vol. 302, No. 2, pp. 424-431.

[11] Fendrof, S., Eick, M.J., Grossl, P. and Sparks, D.L., 1997, “Arsenate and chromate retention mechanism on goethite,” Environmental Science and Technology, Vol. 31, No. 2, pp. 315-320.

[12] He, Y.T. and Traina, S.J., 2005, “Cr(VI) reduction and immobilization by magnetite under alkaline pH condition: the role of passivation,” Environmental Science and Technology, Vol. 31, pp. 321-326.

[13] Hristovski, K., Baumgardener, A. and Westerhoff, P., 2007, “Selecting metal oxide nanomaterials for arsenic removal in fixed bed column,” Journal of Hazardous Materials, Vol. 147, No. 1-2, pp. 265-274.

[14] Huang, Y.H., Hsueh, C.I., Cheng, H.P., Su, L.C. and Chen, C.Y., 2006, “Thermodynamics and kinetics of adsorption of Cu(II) onto iron oxide,” Journal of Hazardous Materials, Vol. 144, pp. 406-411.

[15] Jain, A., Raven, K. and Leoppert, R.H., 1999, “Arsenite and arsenate adsorption on ferrihydrite,” Environmental Science and Technology, Vol. 33, pp. 1179-1184.

[16] Johnson, B.B., 1990, “Effect of pH, temperature and concentration on the adsorption of cadmium on goethite,” Environmental Science and Technology, Vol. 24, pp. 112-118.

[17] Kanel, S.R., Greneche, J.M. and Choi, H., 2006, “As(V) removal from groundwater using nanoscale zerovalent iron as a colloidal reactive barrier material,” Environmental Science and Technology, Vol. 40, pp. 2040-2045.

[18] Kraepiel, A.M., Keller, K. and Morel, F., 1998, “On the acid-base chemistry of permanently charged minerals,” Environmental Science and Technology, Vol. 32, No. 19, pp. 2829-2838.

[19] Martinson, C.A. and Reddy, K.J., 2009, “Adsorption of arsenic(III) and arsenic(V) by cupric oxide nanoparticles,” Journal of Colloid and Interface Science, Vol. 336, No. 2, pp. 406-411.

[20] Mayo, J.T., Yavuz, C., Yean, S., Cong, L., Shipley, H., Yu, W., Faljner, J., Kan, A., Tomson, M. and Colvin, V.L., 2007, “The effect of nanocrystalline magnetite size on arsenic removal,” Science and Technology of Advanced Materials, Vol. 8, pp. 71-75.

[21] Nowack, B., Lutzenkirchen, J., Behra, P. and Sigg, L., 1996, “Modeling the adsorption of metal-EDTA complexes onto oxides,” Environmental Science and Technology, Vol. 30, No. 7, pp. 2397-2405.

[22] Nriagu, J.O. (Ed.), 1994, Arsenic in the Environment, John Wiley&Sons, New York, USA. Park, H., Myung, N.V., Jung, H. and Choi, H., 2009, “As(V) remediation using electrochemically synthesized maghemite nanoparticles,” The Journal of Nanoparticle Research, Vol. 11, No. 8, pp. 1981-1989.

[23] Pena, M.E., Koratis, G.P., Patel, M., Lippincott, L. and Meng, X., 2005, “Adsorption of As(V) and As(III) by nanocrystalline titanium dioxide,” Water Research, Vol. 39, pp. 2327-2337.

[24] Pokhrel, D. and Viraraghavan, T., 2007, “Arsenic removal in iron oxide coated fungal biomass coulmn,” Bioresources Technology, Vol. 99, No. 6, pp. 2067-2071.

[25] Rietra, R., Hiemstra, T. and Riemsdijk, W.H., 2001, “Interaction between calcium and phosphate adsorption on goethite,” Environmental Science and Technology, Vol. 35, No. 16, pp. 3369-3374.

[26] Schwertmann, U. and Cornell R.M., 2000, Iron Oxides in the Laboratory: Preparation and Characterization, Wiley-VCH, New York, USA, pp. 103-122.

[27] Sharma, Y.C., Srivastava, V., Singh, K.S.N. and Weng, C.H., 2009, “Nano-adsorbents for removal of metallic pollutants from water and wastewater,” Environmental Technology, Vol. 30, pp. 583-609.

[28] Tuutijarvi, T., Lu, J., Sillanpaa M. and Chen, G., 2009, “As(V) adsorption on maghemite nanoparticles,” Journal of Hazardous Materials, Vol. 166, No. 2-3, pp. 1415-1420.

[29] Zhu, H., Jia, Y., Wu, X. and Wang, H., 2009, “Removal of arsenic from water by supported nano zero-valent iron on activated carbon,” Journal of Hazardous Materials, Vol. 172, No. 2-3, pp. 1591-1596.

Journal of the Korean Society of Mineral and Energy Resources Engineers ISSN:2288-0291(Print) 2288-2790(Online) 한국자원공학회지

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