Economic and Environmental Geology (자원환경지질)

The Korean Society of Economic and Environmental Geology (대한자원환경지질학회)
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Investigation on Effects of Aging on the Formation and Physicochemical Properties of Hydrothermally Synthesized Magnesium Aluminum-Layered Double Hydroxide/Rice Husk Hydrochar Nanocomposites for Effective Remediation of Arsenic-Contaminated Soil

비소 오염토양의 효과적 정화를 위한 열수합성 마그네슘알루미늄-이중층수산화물/왕겨 하이드로차 나노복합체의 형성 및 이화학적 특성에 미치는 에이징 효과 규명

  • Seon Yong Lee (Mineral Resources Division, Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Chul-Min Chon (Mineral Resources Division, Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Gil-Jae Yim (Mineral Resources Division, Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • So-Jeong Kim (Mineral Resources Division, Korea Institute of Geoscience and Mineral Resources (KIGAM)) ;
  • Sue A Kang (Department of Earth and Environmental Sciences, Korea University) ;
  • Young Jae Lee (Department of Earth and Environmental Sciences, Korea University)
  • 이선용 (한국지질자원연구원 광물자원연구본부) ;
  • 전철민 (한국지질자원연구원 광물자원연구본부) ;
  • 임길재 (한국지질자원연구원 광물자원연구본부) ;
  • 김소정 (한국지질자원연구원 광물자원연구본부) ;
  • 강수아 (고려대학교 지구환경과학과) ;
  • 이영재 (고려대학교 지구환경과학과)
  • Received : 2024.08.21
  • Accepted : 2024.09.10
  • Published : 2024.10.29
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Abstract

This study presents the synthesis and characterization of MgAl-layered double hydroxide (LDH)/rice husk hydrochar (RHH) nanocomposites (MgAl-LDH/RHHs) via an in situ one-pot hydrothermal route at 150 ℃, utilizing Mg:Al molar ratio of 2:1 for arsenic remediation. The formation of MgAl-LDH/RHHs and their physicochemical properties were evaluated under varying hydrothermal aging times systematically. Prolonging the aging period to 12 hrs significantly enhanced the crystallinity and crystal size of the LDHs, resulting in a 3D hierarchical structure with the highest specific surface area (27.98 m2/g) formed on the hydrochar surface. The hexagonal crystal structure (d003 = 0.8246 nm) was characterized by a rhombohedral unit cell with lattice parameters a = 0.3049 nm and c = 2.4738 nm, and a high positive charge density of 4.284 e/nm2. These properties were found to be favorable for the sorption of arsenic oxyanions. Batch adsorption experiments were conducted to assess the potential of MgAl-LDH/RHHs-12h for the remediation of arsenic-contaminated soils. The original soil sample (CY) was mechanically sieved into fine-grained (CYF, < 75 ㎛) and coarse-grained (CYC, 75 ㎛-2 mm) fractions. When these soil samples were reacted with deionized water, arsenate was identified as the dissolved arsenic species, with concentrations of 2.85 mg/L for CY, 4.02 mg/L for CYF, and 2.55 mg/L for CYC, respectively. Kinetic sorption experiments, conducted at pH 5.0 and 8.0 in the presence and absence of 0.1 M NaCl as a background electrolyte, revealed that arsenic sorption onto MgAl-LDH/RHHs-12h was inhibited at pH 8 in the presence of NaCl. These findings suggest that effective arsenic sorption requires low pH conditions with minimal background electrolytes in soils.

본 연구에서는 비소 정화에 활용하기 위한 마그네슘알루미늄-이중충수산화물/왕겨 하이드로차 나노복합체(MgAl-LDH/RHHs)를 150 ℃, 2:1의 Mg:Al 몰비율 조건에서 원위치 단일 열수합성을 통해 합성하고 특성화 하였다. 또한 열수조건 에이징 시간에 따른 MgAl-LDH/RHHs의 형성 및 이화학적 특성들이 체계적으로 평가되었다. 12시간까지 에이징을 연장하였을 때, LDHs의 결정도 및 결정 크기가 뚜렷하게 증가하였으며, 하이드로차 표면에는 3차원 계층 구조가 형성되어 가장 넓은 비표면적(27.98 m2/g)을 제공했다. MgAl-LDH/RHHs-12h 으로 명명된 12시간 에이징 된 시료의 LDHs 결정의 화학식은 Mg0.655Al0.345(OH)2(NO3-)0.345로서 층간 음이온으로 질산염을 가진다. 또한, 육방 결정구조(d003 = 0.8246 nm)와 능면체 단위포 격자 파라미터(a = 0.3049 nm, c = 2.4738 nm), 그리고 4.284 e/nm2의 높은 양전하밀도를 갖는다. 이러한 특성들은 비소와 같은 산소음이온 흡착에 유리한 것으로 밝혀졌다. 비소 오염토양 정화를 위한 MgAl-LDH/RHHs-12h의 잠재성을 평가하기 위하여 As(III)와 As(V)에 대한 배치 흡착실험이 수행되었다. CY로 명명된 원토양은 기계적 체질에 의해 각각 세립질(CYF, < 75 ㎛)과 조립질(CYC, 75 ㎛ ~ 2 mm)로 분리되었다. 이 토양시료들을 탈이온수와 반응시킨 결과, 용존 비소 이온종은 비산염으로 확인되었으며, 비소 농도는 CY에서 2.85 mg/L, CYF에서 4.02 mg/L, 그리고 CYC에서 2.55 mg/L로 각각 나타났다. pH 5.0과 8.0, 그리고 배경전해질 0.1 M NaCl 유무 조건에서 수행된 키네틱 흡착 실험을 통해 pH 8.0과 NaCl 존재 하에서 비소 흡착이 저해됨이 밝혀졌다. 이러한 결과들은 효과적 비소 흡착을 위해서는 토양 내(예, 토양수) pH가 낮고 배경전해질이 적은 조건이 요구됨을 시사한다.

Keywords

Acknowledgement

This study was supported by the Basic Research Project of the Korea Institute of Geoscience and Mineral Resources (KIGAM) institutional program (24-3412). This study was also supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (RS-2024-00345589).

References

  1. Basu, D., Das, A., Stockelhuber, K.W., Wagenknecht, U. and Heinrich, G. (2014) Advances in layered double hydroxide (LDH)-based elastomer composites. Progress in Polymer Science, v.39, no.3, p.594-626. doi: 10.1016/j.progpolymsci.2013.07.011
  2. Benhiti, R., Ait Ichou, A., Zaghloul, A., Aziam, R., Carja, G., Zerbet, M., Sinan, F. and Chiban, M. (2020) Synthesis, characterization, and comparative study of MgAl-LDHs prepared by standard coprecipitation and urea hydrolysis methods for phosphate removal. Environmental Science and Pollution Research, v.27, p.45767-45774. doi: 10.1007/s11356-020-10444-5
  3. Berber, M.R., Hafez, I.H., Minagawa, K., Katoh, M., Tanaka, M. and Mori, T. Control of nanoparticle size, crystal structure and growth of layered double hydroxide by hydrothermal treatment, Proceedings International Journal of Modern Physics. Conference Series2012, Volume 6, World Scientific, p.133-137. doi: 10.1142/s2010194512003066
  4. Casiot, C., Lebrun, S., Morin, G., Bruneel, O., Personne, J. and Elbaz-Poulichet, F. (2005) Sorption and redox processes controlling arsenic fate and transport in a stream impacted by acid mine drainage. Science of the Total Environment, v.347, no.1-3, p.122-130. doi: 10.1016/j.scitotenv.2004.12.039
  5. Fan, Z., Zhang, X., Li, Y., Guo, X. and Jin, Z. (2022) Construct 3D NiCo-LDH/Cu2O pn heterojunction via electrostatic self-assembly for enhanced photocatalytic hydrogen evolution. Journal of Industrial and Engineering Chemistry, v.110, p.491-502. doi: 10.1016/j.jiec.2022.03.027
  6. Goodman, B.A. (2020) Utilization of waste straw and husks from rice production: A review. Journal of Bioresources and Bioproducts, v.5, no.3, p.143-162. 10.1016/j.jobab.2020.07.001
  7. Ji, H., Wu, W., Li, F., Yu, X., Fu, J. and Jia, L. (2017) Enhanced adsorption of bromate from aqueous solutions on ordered mesoporous Mg-Al layered double hydroxides (LDHs). Journal of Hazardous Materials, v.334, p.212-222. doi: 10.1016/j.jhazmat.2017.04.014
  8. Jung, K.-W., Lee, S.Y., Choi, J.-W., Hwang, M.-J. and Shim, W.G. (2021) Synthesis of Mg-Al layered double hydroxides-functionalized hydrochar composite via an in situ one-pot hydrothermal method for arsenate and phosphate removal: Structural characterization and adsorption performance. Chemical Engineering Journal, v.420, p.129775. doi: 10.1016/j.cej.2021.129775
  9. Khorshidi, M., Asadpour, S., Sarmast, N. and Dinari, M. (2022) A review of the synthesis methods, properties, and applications of layered double hydroxides/carbon nanocomposites. Journal of Molecular Liquids, v.348, p.118399. doi: 10.1016/j.molliq.2021.118399
  10. Kim, E.J., Yoo, J.-C. and Baek, K. (2014) Arsenic speciation and bioaccessibility in arsenic-contaminated soils: sequential extraction and mineralogical investigation. Environmental Pollution, v.186, p.29-35. doi: 10.1016/j.envpol.2013.11.032
  11. Kwon, Y.-S. and Kim, E.J. (2017) Effects of Contamination Source and Particle Size on Arsenic Speciation and Bioaccessibility in Soils. Journal of Soil and Groundwater Environment, v.22, no.5, p.89-97. doi: 10.7857/JSGE.2017.22.5.089
  12. Lee, J.-H., Ko, Y.-W., Kim, K.-Y., Lim, J.-H. and Kim, K.-M. (2011) Preparation and Characterization of Graphene/Zn-Al Layered Double Hydroxide Composites. Journal of Adhesion and Interface, v.12, no.4, p.133-137. doi: 10.17702/jai.2011.12.4.133
  13. Lee, J.H., Ji, W.H., Lee, J.S., Park, S.S., Choi, K.W., Kang, C.U. and Kim, S.J. (2020) A Study of Fluoride and Arsenic Adsorption from Aqueous Solution Using Alum Sludge Based Adsorbent. Economic and Environmental Geology, v.53, no.6, p.667-675. doi: 10.9719/eeg.2021.54.6.709
  14. Lee, S.Y., Choi, J.-W., Song, K.G., Choi, K., Lee, Y.J. and Jung, K.-W. (2019a) Adsorption and mechanistic study for phosphate removal by rice husk-derived biochar functionalized with Mg/Al-calcined layered double hydroxides via co-pyrolysis. Composites Part B: Engineering, v.176, p.107209. doi: 10.1016/j.compositesb.2019.107209
  15. Lee, S.Y., Jung, K.-W., Choi, J.-W. and Lee, Y.J. (2019b) In situ synthesis of hierarchical cobalt-aluminum layered double hydroxide on boehmite surface for efficient removal of arsenate from aqueous solutions: effects of solution chemistry factors and sorption mechanism. Chemical Engineering Journal, v.368, p.914-923. doi: 10.1016/j.cej.2019.03.043
  16. Lee, S.Y., Kim, Y., Kang, S.A., Chang, B., Hur, H. and Lee, Y.J. (2023a) Characterization of arsenic (III and V) adsorption on natural schwertmannite formed in acid coal mine drainage: Batch studies and spectroscopic observations. Journal of Environmental Chemical Engineering, v.11, no.1, p.109170. doi: 10.1016/j.jece.2022.109170
  17. Lee, S.Y., Kim, Y. and Lee, Y.J. (2023b) Review of Domestic Research Trends on Layered Double Hydroxide (LDH) Materials: Based on Research Articles in Korean Citation Index (KCI). Economic and Environmental Geology, v.56, no.1, p.23-53. doi: 10.9719/eeg.2023.56.1.23
  18. Li, J., Song, Y., Wang, Y. and Zhang, H. (2019) Enhanced Heck reaction on flower-like Co (Mg or Ni) Al layered double hydroxide supported ultrafine PdCo alloy nanocluster catalysts: The promotional effect of Co. Dalton Transactions, v.48, no.48, p.17741-17751. doi: 10.1039/c9dt03663f
  19. Li, R., Wang, J.J., Zhou, B., Awasthi, M.K., Ali, A., Zhang, Z., Gaston, L.A., Lahori, A.H. and Mahar, A. (2016) Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios. Science of the Total Environment, v.559, p.121-129. doi: 10.1016/j.scitotenv.2016.03.151
  20. Okamoto, K., Iyi, N. and Sasaki, T. (2007) Factors affecting the crystal size of the MgAl-LDH (layered double hydroxide) prepared by using ammonia-releasing reagents. Applied Clay Science, v.37, no.1-2, p.23-31. doi: 10.1016/j.clay.2006.10.008
  21. Park, J.H., Kim, S.J., Nam, I.H., Ryu, J., Jung, G.Y. and Han, Y.S. (2022) Microbial mediated reaction of dimethylarsinic acid in wetland water and sediments. Water Research, v.222, 118873. doi: 10.1016/j.watres.2022.118873
  22. Pourfaraj, R., Fatemi, S.J., Kazemi, S.Y. and Biparva, P. (2017) Synthesis of hexagonal mesoporous MgAl LDH nanoplatelets adsorbent for the effective adsorption of Brilliant Yellow. Journal of Colloid and Interface Science, v.508, p.65-74. doi: 10.1016/j.jcis.2017.07.101
  23. Prasara-A, J. and Gheewala, S.H. (2017) Sustainable utilization of rice husk ash from power plants: A review. Journal of Cleaner Production, v.167, p.1020-1028. doi: 10.1016/j.jclepro.2016.11.042
  24. Rahman, M.M., Ng, J.C. and Naidu, R. (2009) Chronic exposure of arsenic via drinking water and its adverse health impacts on humans. Environmental Geochemistry and Health, v.31, p.189-200. doi: 10.1007/s10653-008-9235-0
  25. Smedley, P.L. and Kinniburgh, D.G. (2002) A review of the source, behaviour and distribution of arsenic in natural waters. Applied Geochemistry, v.17, no.5, p.517-568. doi: 10.1016/s0883-2927(02)00018-5
  26. Taher, T., Yu, Z., Melati, E.K.A., Munandar, A., Aflaha, R., Triyana, K., Wibowo, Y.G., Khairurrijal, K., Lesbani, A. and Rianjanu, A. (2024) Enabling dual-functionality material for effective anionic and cationic dye removal by using Nb2O5/MgAl-LDH nanocomposites. Journal of Hazardous Materials Letters, v.5, p.100103. doi: 10.1016/j.hazl.2024.100103
  27. Wan, D., Liu, H., Liu, R., Qu, J., Li, S. and Zhang, J. (2012) Adsorption of nitrate and nitrite from aqueous solution onto calcined (Mg-Al) hydrotalcite of different Mg/Al ratio. Chemical Engineering Journal, v.195, p.241-247. doi: 10.1016/j.cej.2012.04.088
  28. Wang, S.-L., Liu, C.H., Wang, M.K., Chuang, Y.H. and Chiang, P.N. (2009) Arsenate adsorption by Mg/Al-NO3 layered double hydroxides with varying the Mg/Al ratio. Applied Clay Science, v.43, no.1, p.79-85. doi: 10.1016/j.clay.2008.07.005
  29. Wang, Y., Xie, C., Zhang, Z., Liu, D., Chen, R. and Wang, S. (2018) In situ exfoliated, N-doped, and edge-rich ultrathin layered double hydroxides nanosheets for oxygen evolution reaction: Advanced Functional Materials, v.28, no.4, p.1703363. doi: 10.1002/adfm.201800607
  30. Zhang, F., Du, N., Song, S. and Hou, W. (2015) Mechanohydrothermal synthesis of SDS intercalated LDH nanohybrids and their removal efficiency for 2, 4-dichlorophenoxyacetic acid from aqueous solution. Materials Chemistry and Physics, v.152, p.95-103. doi: 10.1016/j.matchemphys.2014.12.019