Adsorption of Cr(VI) on calcined MgAl-layered double hydroxides and recycling of spent adsorbents for the removal of organic dyes

Abstract

Adsorption is considered an effective strategy for removing Cr(VI) from wastewater, but disposal of spent adsorbents is still a thorny problem. This work aims to develop an efficient adsorbent for Cr(VI) removal and recycling spent adsorbent as catalyst for the removal of organic dyes. In this study, MgAl-mixed oxides adsorbents (MgAlO) were synthesized via hydrothermal and calcination steps to effectively adsorb Cr(VI) from wastewater. The influence of initial pH and temperature on the adsorption performance of MgAlO was investigated. The maximum adsorption capacity for Cr(VI) was 95.2 mg/g at a MgAlO dosage of 1.0 g/L and a pH value of 5.5. The combination of XRD, FT-IR, and UV-vis DRS analyses revealed that CrO₄²⁻ anions were intercalated into the interlayer spaces of layered double hydroxides, and high temperatures can accelerate the reconstruction of MgAlO. The adsorption of Cr(VI) by MgAlO followed the pseudo-second-order kinetic model, which included intra-particle diffusion, film diffusion, and chemical reaction. Furthermore, the resulting spent adsorbent (Cr-MgAlO) after adsorption was reused as a catalyst for methyl orange (MO) removal after adsorption (75.6% removal rate) and showed no significant decrease in removal rate after 5 cycles. The results of this study provide insights into the reuse of spent Cr(VI) adsorbent for environmental catalytic applications, which are of great importance for the disposal of waste adsorbent.

Keywords

MgAl-mixed oxides / adsorption / Cr(VI) / recycling spent adsorbent

References

[1] ZhuZ, LiJ, LiW, et al. . Simulated-sunlight-driven Cr(vi) reduction on a type-II heterostructured Sb₂S₃/CdS photocatalyst [J]. Environmental Science: Nano, 2022, 9(5): 1738-1747

[2] WangY, LiuY, BaoS, et al. . Aminated metal-free red phosphorus nanosheets for adsorption and photocatalytic reduction of Cr(VI) from water [J]. Separation and Purification Technology, 2021, 274: 118968

[3] XiaoW, XiaoL, LvY, et al. . Lignin-derived carbon coated nanoscale zero-valent iron as a novel bifunctional material for efficient removal of Cr(VI) and organic pollutants [J]. Separation and Purification Technology, 2022, 299121689

[4] FanP, LiuC, LiQ, et al. . Microwave-assisted rapid synthesis of ovalbumin-stabilized gold nanoclusters for picric acid determination [J]. Journal of Central South University, 2023, 30(1): 74-84

[5] XuR, WangY, SunY, et al. . External sodium acetate improved Cr(VI) stabilization in a Cr-spiked soil during chemical-microbial reduction processes: Insights into Cr(VI) reduction performance, microbial community and metabolic functions [J]. Ecotoxicology and Environmental Safety, 2023, 251114566

[6] GracepavithraK, JaikumarV, KumarP S, et al. . A review on cleaner strategies for chromium industrial wastewater: Present research and future perspective [J]. Journal of Cleaner Production, 2019, 228580-593

[7] GongY, ZhaoD, WangQ-lin. An overview of field-scale studies on remediation of soil contaminated with heavy metals and metalloids: Technical progress over the last decade [J]. Water Research, 2018, 147: 440-460

[8] JobbyR, JhaP, YadavA K, et al. . Biosorption and biotransformation of hexavalent chromium[Cr(VI)]: A comprehensive review [J]. Chemosphere, 2018, 207: 255-266

[9] SunX, DingJ, HeL, et al. . Quantitative characterization of water absorption pore structure evolution in sandstone based on nitrogen adsorption and mercury intrusion [J]. Journal of Central South University, 2024, 31(1): 182-195

[10] XuD, HuangY, MaQ, et al. . A 3D porous structured cellulose nanofibrils-based hydrogel with carbon dots-enhanced synergetic effects of adsorption and photocatalysis for effective Cr(VI) removal [J]. Chemical Engineering Journal, 2023, 456: 141104

[11] ChenC, ZengH, XuS, et al. . Preparation of mesoporous material from hydrotalcite/carbon composite precursor for chromium(VI) removal [J]. Journal of the Taiwan Institute of Chemical Engineers, 2017, 70302-310

[12] GhorbaniF, KamariS, ZamaniS, et al. . Optimization and modeling of aqueous Cr(VI) adsorption onto activated carbon prepared from sugar beet bagasse agricultural waste by application of response surface methodology [J]. Surfaces and Interfaces, 2020, 18: 100444

[13] SessaregoS, RodriguesS C G, XiaoY, et al. . Phosphonium-enhanced chitosan for Cr(VI) adsorption in wastewater treatment [J]. Carbohydrate Polymers, 2019, 211249-256

[14] PanZ, ZhuX, SatpathyA, et al. . Cr(VI) adsorption on engineered iron oxide nanoparticles: Exploring complexation processes and water chemistry [J]. Environmental Science & Technology, 2019, 53(20): 11913-11921

[15] RouhaninezhadA A, HojatiS, MasirM N. Adsorption of Cr(VI) onto micro- and nanoparticles of palygorskite in aqueous solutions: Effects of pH and humic acid [J]. Ecotoxicology and Environmental Safety, 2020, 206: 111247

[16] GuanX, YuanX, ZhaoY, et al. . Application of functionalized layered double hydroxides for heavy metal removal: A review [J]. The Science of the Total Environment, 2022, 838(Pt1): 155693

[17] ZhengX, LiuD, WenJ, et al. . Nonthermal plasma-vulcanized flower-like ZnS/Zn-Al composites from Zn-Al layered double hydroxides for the adsorption-photo-reduction of Cr(VI) [J]. Separation and Purification Technology, 2021, 275117934

[18] ZhangL, HeF, MaoW, et al. . Fast and efficient removal of Cr(VI) to ppb level together with Cr(III) sequestration in water using layered double hydroxide interclated with diethyldithiocarbamate [J]. The Science of the Total Environment, 2020, 727138701

[19] LongF, NiuC, TangN, et al. . Highly efficient removal of hexavalent chromium from aqueous solution by calcined Mg/Al-layered double hydroxides/polyaniline composites [J]. Chemical Engineering Journal, 2021, 404127084

[20] DinariM, ShiraniM A, MalekiM H, et al. . Green cross-linked bionanocomposite of magnetic layered double hydroxide/guar gum polymer as an efficient adsorbent of Cr(VI) from aqueous solution [J]. Carbohydrate Polymers, 2020, 236116070

[21] ZouY, WangX, WuF, et al. . Controllable synthesis of Ca-Mg-Al layered double hydroxides and calcined layered double oxides for the efficient removal of U(VI) from wastewater solutions [J]. ACS Sustainable Chemistry & Engineering, 2017, 511173-1185

[22] BaskarA V, BolanN, HoangS A, et al. . Recovery, regeneration and sustainable management of spent adsorbents from wastewater treatment streams: A review [J]. Science of the Total Environment, 2022, 822153555

[23] HeD, ZhangL, ZhaoY, et al. . Recycling spent Cr adsorbents as catalyst for eliminating methylmercaptan [J]. Environmental Science & Technology, 2018, 52(6): 3669-3675

[24] YadavM K, SaiduluD, GhosalP S, et al. . A review on the management of arsenic-laden spent adsorbent: Insights of global practices, process criticality, and sustainable solutions [J]. Environmental Technology & Innovation, 2022, 27102500

[25] LataS, SinghP K, SamadderS R. Regeneration of adsorbents and recovery of heavy metals: A review [J]. International Journal of Environmental Science and Technology, 2015, 12(4): 1461-1478

[26] HeD, ZhangY, YangS, et al. . Development of a strategy to reuse spent Cr adsorbents as efficient catalysts: From the perspective of practical application [J]. ACS Sustainable Chemistry & Engineering, 2019, 7(3): 3251-3257

[27] LaipanM, FuH, ZhuR, et al. . Converting spent Cu/Fe layered double hydroxide into Cr(VI) reductant and porous carbon material [J]. Scientific Reports, 2017, 77277

[28] LuK, GaoM, SunB, et al. . Simultaneous removal of Cr and organic matters via coupling Cr-Fenton-like reaction with Cr flocculation: The key role of Cr flocs on coupling effect [J]. Chemosphere, 2022, 287(Pt1): 131991

[29] KawanishiS, InoueS, SanoS. Mechanism of DNA cleavage induced by sodium chromate(VI) in the presence of hydrogen peroxide [J]. The Journal of Biological Chemistry, 1986, 261135952-5958

[30] PetersJ W, BekowiesP J, WinerA M, et al. . Potassium perchromate as a source of singlet oxygen [J]. Journal of the American Chemical Society, 1975, 97(12): 3299-3306

[31] ZengH, DengX, WangY, et al. . Preparation of Mg-Al hydrotalcite by urea method and its catalytic activity for transesterification [J]. AIChE Journal, 2009, 55(5): 1229-1235

[32] XieJ, LinY, LiC, et al. . Removal and recovery of phosphate from water by activated aluminum oxide and lanthanum oxide [J]. Powder Technology, 2015, 269351-357

[33] ZhangZ, LiaoM, ZengH, et al. . Temperature effect on chromium(VI) removal by Mg/Al mixed metal oxides as adsorbents [J]. Applied Clay Science, 2014, 102: 246-253

[34] YiY, WangX, MaJ, et al. . Fe(III) modified Egeria najas driven-biochar for highly improved reduction and adsorption performance of Cr(VI) [J]. Powder Technology, 2021, 388: 485-495

[35] GuptaV K, ChandraR, TyagiI, et al. . Removal of hexavalent chromium ions using CuO nanoparticles for water purification applications [J]. Journal of Colloid and Interface Science, 2016, 478: 54-62

[36] ZhouT, LiC, JinH, et al. . Effective adsorption/reduction of Cr(VI) oxyanion by Halloysite@Polyaniline hybrid nanotubes [J]. ACS Applied Materials & Interfaces, 2017, 9(7): 6030-6043

[37] GuoL, ZhangY, ZhengJ, et al. . Synthesis and characterization of ZnNiCr-layered double hydroxides with high adsorption activities for Cr(VI) [J]. Advanced Composites and Hybrid Materials, 2021, 4(3): 819-829

[38] GuoL, ZhangY, ZhengJ, et al. . Synthesis and characterization of ZnNiCr-layered double hydroxides with high adsorption activities for Cr(VI) [J]. Advanced Composites and Hybrid Materials, 2021, 4(3): 819-829

[39] BenhitiR, Ait IchouA, AboussabekA, et al. . Efficient removal of Cr(VI) from aqueous solution using memory effect property of layered double hydroxide material [J]. Chemosphere, 2023, 341: 140127

[40] DinariM, SoltaniR, MohammadnezhadG. Kinetics and thermodynamic study on novel modified-mesoporous silica MCM-41/polymer matrix nanocomposites: Effective adsorbents for trace CrVI removal [J]. Journal of Chemical & Engineering Data, 2017, 62(8): 2316-2329

[41] SahuS, KarP, BishoyiN, et al. . Synthesis of polypyrrole-modified layered double hydroxides for efficient removal of Cr(VI) [J]. Journal of Chemical & Engineering Data, 2019, 64(10): 4357-4368

[42] LiangH, SunR, SongB, et al. . Preparation of nitrogen-doped porous carbon material by a hydrothermal-activation two-step method and its high-efficiency adsorption of Cr(VI) [J]. Journal of Hazardous Materials, 2020, 387121987

[43] ZhangY, JiaoX, LiuN, et al. . Enhanced removal of aqueous Cr(VI) by a green synthesized nanoscale zero-valent iron supported on oak wood biochar [J]. Chemosphere, 2020, 245125542

[44] YaoJ, WenJ, LiH, et al. . Surface functional groups determine adsorption of pharmaceuticals and personal care products on polypropylene microplastics [J]. Journal of Hazardous Materials, 2022, 423(PtB): 127131

[45] MartinsA C, PezotiO, CazettaA L, et al. . Removal of tetracycline by NaOH-activated carbon produced from macadamia nut shells: Kinetic and equilibrium studies [J]. Chemical Engineering Journal, 2015, 260291-299

[46] WeiH, MaJ, ShiY, et al. . Sustainable cross-linked porous corn starch adsorbents with high methyl violet adsorption [J]. ES Materials & Manufacturing, 2018, 2(3): 28-34

[47] WangY, LinN, GongY, et al. . Cu-Fe embedded cross-linked 3D hydrogel for enhanced reductive removal of Cr(VI): Characterization, performance, and mechanisms [J]. Chemosphere, 2021, 280130663

[48] CaoE, DuanW, YiL, et al. . Poly(m-phenylenediamine) functionalized Calotropis gigantea fiber for coupled adsorption reduction for Cr(VI) [J]. Journal of Molecular Liquids, 2017, 240225-232

[49] LiY, ZhangY, SuF, et al. . Adsorption behaviour of microplastics on the heavy metal Cr(VI) before and after ageing [J]. Chemosphere, 2022, 302134865

[50] SunX, XuY, BaiS, et al. . Electronic structure regulation of halogen anion-intercalated MgAl-LDH for highly selective photothermal oxidation of CH₄ [J]. Inorganic Chemistry Frontiers, 2023, 10(6): 1769-1774

[51] KimY, SonY, BaeS, et al. . Particle size and interlayer anion effect on chromate adsorption by MgAl-layered double hydroxide [J]. Applied Clay Science, 2022, 225106552

[52] MalherbeF, BesseJ P. Investigating the effects of guest-host interactions on the properties of anion-exchanged Mg-Al hydrotalcites [J]. Journal of Solid State Chemistry, 2000, 155(2): 332-341

[53] TytłakA, OleszczukP, DobrowolskiR. Sorption and desorption of Cr(VI) ions from water by biochars in different environmental conditions [J]. Environmental Science and Pollution Research, 2015, 22(8): 5985-5994

[54] HoffmannM M, DarabJ G, FultonJ L. An infrared and X-ray absorption study of the equilibria and structures of chromate, bichromate, and dichromate in ambient aqueous solutions [J]. The Journal of Physical Chemistry A, 2001, 105(10): 1772-1782

[55] XiaoL, MaW, HanM, et al. . The influence of ferric iron in calcined nano-Mg/Al hydrotalcite on adsorption of Cr(VI) from aqueous solution [J]. Journal of Hazardous Materials, 2011, 186(1): 690-698

[56] ChenY, SongY-fei. Highly selective and efficient removal of Cr(VI) and Cu(II) by the chromotropic acid-intercalated Zn-Al layered double hydroxides [J]. Industrial & Engineering Chemistry Research, 2013, 52(12): 4436-4442