Crosslinking acrylamide with EDTA-intercalated layered double hydroxide for enhanced recovery of Cr(VI) and Congo red: Adsorptive and mechanistic study

Highlights

• Functional groups of AM and EDTA in composite increased removal of Cr(VI) and CR.

• Removal process reached equilibrium within 30 min and was minimally affected by pH.

• Elimination of Cr(VI) was promoted by coexisting CR.

• Adsorption process of CR was less influenced by the presence of Cr(VI).

• Mechanisms were electrostatic attraction, surface complexation and anion exchange.

Abstract

We prepared ethylenediaminetetraacetic acid (EDTA)-intercalated MgAl-layered double hydroxide (LDH-EDTA), then grafted acrylamide (AM) to the LDH-EDTA by a cross-linking method to yield a LDH-EDTA-AM composite; we then evaluated its adsorptive ability for Congo red (CR) and hexavalent chromium (Cr(VI)) in single and binary adsorption systems. The adsorption process on LDH-EDTA-AM for CR and Cr(VI) achieved equilibrium quickly, and the removal efficiencies were minimally affected by initial pH. The maximum uptake quantities of CR and Cr(VI) on LDH-EDTA-AM were 632.9 and 48.47 mg/g, respectively. In mixed systems, chromate removal was stimulated by the presence of CR, while the adsorption efficiency of CR was almost not influenced by coexisting Cr(VI). The mechanisms involved electrostatic attraction, surface complexation, and anion exchange for the adsorption of both hazardous pollutants. In the Cr(VI) adsorption process, reduction also took place. The removal efficiencies in real contaminated water were all higher than those in the laboratory solutions.

Graphical abstract

Keywords

Chromate / Dye adsorption / Simultaneous removal / Cross-linking method / Amino functionalization

References

[1] Asiabi H, Yamini Y, Shamsayei M (2017). Highly selective and efficient removal of arsenic(V), chromium(VI) and selenium(VI) oxyanions by layered double hydroxide intercalated with zwitterionic glycine. Journal of Hazardous Materials, 339: 239–247

[2] Chen B, Zhao H N, Chen S J, Long F X, Huang B, Yang B Q, Pan X J (2019). A magnetically recyclable chitosan composite adsorbent functionalized with EDTA for simultaneous capture of anionic dye and heavy metals in complex wastewater. Chemical Engineering Journal, 356: 69–80

[3] Chen H, Lin J H, Zhang N, Chen L Z, Zhong S P, Wang Y, Zhang W G, Ling Q D (2018). Preparation of MgAl-EDTA-LDH based electrospun nanofiber membrane and its adsorption properties of copper(II) from wastewater. Journal of Hazardous Materials, 345: 1–9

[4] Chen J, Yan L G, Yu H Q, Li S, Qin L L, Liu G Q, Li Y F, Du B (2016). Efficient removal of phosphate by facile prepared magnetic diatomite and illite clay from aqueous solution. Chemical Engineering Journal, 287: 162–172

[5] Cui L M, Wang Y G, Gao L, Hu L H, Yan L G, Wei Q, Du B (2015). EDTA functionalized magnetic graphene oxide for removal of Pb(II), Hg(II) and Cu(II) in water treatment: Adsorption mechanism and separation property. Chemical Engineering Journal, 281: 1–10

[6] Das N N, Konar J, Mohanta M K, Srivastava S C (2004). Adsorption of Cr(VI) and Se(IV) from their aqueous solutions onto Zr⁴⁺-substituted ZnAl/MgAl-layered double hydroxides: Effect of Zr⁴⁺ substitution in the layer. Journal of Colloid and Interface Science, 270(1): 1–8

[7] Deng L, Zeng H X, Shi Z, Zhang W, Luo J M (2018). Sodium dodecyl sulfate intercalated and acrylamide anchored layered double hydroxides: A multifunctional adsorbent for highly efficient removal of Congo red. Journal of Colloid and Interface Science, 521: 172–182

[8] Dhal B, Thatoi H N, Das N N, Pandey B D (2013). Chemical and microbial remediation of hexavalent chromium from contaminated soil and mining/metallurgical solid waste: A review. Journal of Hazardous Materials, 250–251: 272–291

[9] Gao Z S, Sasaki K K, Qiu X H (2018). Structural memory effect of Mg–Al and Zn–Al layered double hydroxides in the presence of different natural humic acids: Process and mechanism. Langmuir, 34(19): 5386–5395

[10] Guo X X, Zhang F Z, Peng Q, Xu S L, Lei X D, Evans D G, Duan X (2011). Layered double hydroxide/eggshell membrane: An inorganic biocomposite membrane as an efficient adsorbent for Cr(VI) removal. Chemical Engineering Journal, 166(1): 81–87

[11] Guo X Y, Du B, Wei Q, Yang J, Hu L H, Yan L G, Xu W Y (2014). Synthesis of amino functionalized magnetic graphenes composite material and its application to remove Cr(VI), Pb(II), Hg(II), Cd(II) and Ni(II) from contaminated water. Journal of Hazardous Materials, 278: 211–220

[12] Li B, Zhang Y X, Zhou X B, Liu Z L, Liu Q Z, Li X H (2016a). Different dye removal mechanisms between monodispersed and uniform hexagonal thin plate-like MgAl-CO₃^2–-LDH and its calcined product in efficient removal of Congo red from water. Journal of Alloys and Compounds, 673: 265–271

[13] Li J, Fan Q H, Wu Y J, Wang X X, Chen C L, Tang Z Y, Wang X K (2016b). Magnetic polydopamine decorated with Mg-Al LDH nanoflakes as a novel bio-based adsorbent for simultaneous removal of potentially toxic metals and anionic dyes. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 4(5): 1737–1746

[14] Li Y J, Gao B Y, Wu T, Sun D J, Li X, Wang B, Lu F J (2009). Hexavalent chromium removal from aqueous solution by adsorption on aluminum magnesium mixed hydroxide. Water Research, 43(12): 3067–3075

[15] Liu X L, Ma R, Wang X X, Ma Y, Yang Y P, Zhuang L, Zhang S, Jehan R, Chen J R, Wang X K (2019). Graphene oxide-based materials for efficient removal of heavy metal ions from aqueous solution: A review. Environmental Pollution, 252: 62–73

[16] Lu Y, Jiang B, Fang L, Ling F L, Gao J M, Wu F, Zhang X H (2016). High performance NiFe layered double hydroxide for methyl orange dye and Cr(VI) adsorption. Chemosphere, 152: 415–422

[17] Pang H W, Wu Y H, Wang X X, Hu B W, Wang X K (2019). Recent advances in composites of graphene and layered double hydroxides for water remediation: A review. Chemistry, an Asian Journal, 14(15): 2542–2552

[18] Qiu X H, Sasaki K K, Xu S, Zhao J W (2019). Double-edged effect of humic acid on multiple sorption modes of calcined layered double hydroxides: Inhibition and promotion. Langmuir, 35(19): 6267–6278

[19] Shan R R, Yan L G, Yang K, Yu S J, Hao Y F, Yu H Q, Du B (2014). Magnetic Fe₃O₄/MgAl-LDH composite for effective removal of three red dyes from aqueous solution. Chemical Engineering Journal, 252: 38–46

[20] Shan R R, Yan L G, Yang Y M, Yang K, Yu S J, Yu H Q, Zhu B C, Du B (2015). Highly efficient removal of three red dyes by adsorption onto Mg-Al-layered double hydroxide. Journal of Industrial and Engineering Chemistry, 21: 561–568

[21] Wang S F, Li X, Liu Y G, Zhang C, Tan X F, Zeng G M, Song B, Jiang L H (2018). Nitrogen-containing amino compounds functionalized graphene oxide: Synthesis, characterization and application for the removal of pollutants from wastewater: A review. Journal of Hazardous Materials, 342: 177–191

[22] Xing H T, Chen J H, Sun X, Huang Y H, Su Z B, Hu S R, Weng W, Li S X, Guo H X, Wu W B, He Y S, Li F M, Huang Y (2015). NH₂-rich polymer/graphene oxide use as a novel adsorbent for removal of Cu(II) from aqueous solution. Chemical Engineering Journal, 263: 280–289

[23] Xu S, Zhao J W, Yu Q Q, Qiu X H, Sasaki K K (2019a). Effect of natural organic matter model compounds on the structure memory effect of different layered double hydroxides. ACS Earth & Space Chemistry, 3(10): 2175–2189

[24] Xu S, Zhao J W, Yu Q Q, Qiu X H, Sasaki K K (2019b). Understanding how specific functional groups in humic acid affect the sorption mechanisms of different calcinated layered double hydroxides. Chemical Engineering Journal: 123633

[25] Xue L, Lu Z P, Cheng Y Z, Sun X Y, Lin H T, Xiao X L, Liu X F, Zhuo S P (2018). Three-dimensional layered double hydroxide membranes: fabrication technique, growth mechanism, and enhanced photocatalytic activity. Chemical Communications, 54(61): 8494–8497

[26] Yan L G, Yang K, Shan R R, Yu H Q, Du B (2015). Calcined ZnAl- and Fe₃O₄/ZnAl–layered double hydroxides for efficient removal of Cr(VI) from aqueous solution. RSC Advances, 5(117): 96495–96503

[27] Yang S Y, Li Q, Chen L, Chen Z S, Hu B W, Wang H H, Wang X K (2020). Synergistic removal and reduction of U(VI) and Cr(VI) by Fe₃S₄ micro-crystal. Chemical Engineering Journal, 385: 123909

[28] Yang S Y, Li Q, Chen L, Chen Z S, Pu Z X, Wang H H, Yu S J, Hu B W, Chen J R, Wang X K (2019). Ultrahigh sorption and reduction of Cr(VI) by two novel core-shell composites combined with Fe₃O₄ and MoS₂. Journal of Hazardous Materials, 379: 120797

[29] Yao W, Yu S J, Wang J, Zou Y D, Lu S S, Ai Y J, Alharbi N S, Alsaedi A, Hayat T, Wang X K (2017). Enhanced removal of methyl orange on calcined glycerol-modified nanocrystallined Mg/Al layered double hydroxides. Chemical Engineering Journal, 307: 476–486

[30] Yin L, Hu B W, Zhuang L, Fu D, Li J X, Hayat T, Alsaedi A, Wang X K (2020). Synthesis of flexible cross-linked cryptomelane-type manganese oxide nanowire membranes and their application for U(VI) and Eu(III) elimination from solutions. Chemical Engineering Journal, 381: 122744

[31] Yu S J, Wang X X, Chen Z S, Wang J, Wang S H, Hayat T, Wang X K (2017). Layered double hydroxide intercalated with aromatic acid anions for the efficient capture of aniline from aqueous solution. Journal of Hazardous Materials, 321: 111–120

[32] Yuan X Y, Wang Y F, Wang J, Zhou C, Tang Q, Rao X B (2013). Calcined graphene/MgAl-layered double hydroxides for enhanced Cr(VI) removal. Chemical Engineering Journal, 221: 204–213

[33] Zhang J, Li Y, Zhou J Z, Chen D, Qian G R (2012). Chromium (VI) and zinc (II) waste water co-treatment by forming layered double hydroxides: Mechanism discussion via two different processes and application in real plating water. Journal of Hazardous Materials, 205–206: 111–117

[34] Zhang L, Fu F L, Tang B (2019). Adsorption and redox conversion behaviors of Cr(VI) on goethite/carbon microspheres and akaganeite/carbon microspheres composites. Chemical Engineering Journal, 356: 151–160

[35] Zhao J Q, Zhang X F, He X, Xiao M J, Zhang W, Lu C H (2015). A super biosorbent from dendrimer poly(amidoamine)-grafted cellulose nanofibril aerogels for effective removal of Cr(VI). Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 3(28): 14703–14711

Acknowledgement

This work was supported by the National Natural Science Foundation of China (Grant No. 21577048).

RIGHTS & PERMISSIONS

2020 Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature