Functionalization of sawdust biochar using Mg-Fe-LDH and sodium dodecyl sulfonate enhanced its stability and immobilization capacity for Cd and Pb in contaminated water and soil

Abstract

The increased contamination of potentially toxic element (PTE) has posed remarkable ecological risks to environment. Application of functionalized biochar for the remediation of PTE contaminated water and soils are of great concern, and effective strategies are urgently needed to enhance the removal capacity of biochar for PTE. As a novel surface modification technology, the effect of layered double hydroxides (LDH) and sodium dodecyl sulfonate (SDS) on the remediation capacity of biochar for PTE polluted soils and water remains unclear. Sawdust biochar (SB) was coated with Mg and Fe to synthesize the Mg-Fe-LDH functionalized biochar (MFB); thereafter, the MFB was mixed with SDS solution to synthesize the organic-Mg-Fe-LDH biochar (MSB). The potential of SB, MFB, and MSB for remediation of Cd and Pb contaminated soil and water was evaluated in terms of adsorption capacity, immobilization efficiency, and stability. Loading of Mg-Fe-LDH into SB, along with SDS treatment created a regular micro-nano hierarchical structure and enhanced the surface roughness, aromaticity, and hydrophobicity of MSB as compared to SB. MSB exhibited a significantly higher maximum adsorption capacity (mg g⁻¹) for water Pb (405.2) and Cd (673.0) than MFB (335.9 for Pb and 209.0 for Cd) and SB (178.2 for Pb and 186.1 for Cd). MSB altered the soluble fraction of Cd/Pb to the residual fraction and thus significantly decreased their mobilization in soil. The higher removal/immobilization efficiency of MSB could be attributed to its alkalinity, and the enhanced synergistic interactions including surface precipitation, ion exchange, complexation, and hydrogen bonding. The resistance to carbon loss by H₂O₂, thermal recalcitrance index R ₅₀, and degree of graphitization in MSB were significantly improved compared to SB, indicating a more stable carbon fraction sequestered in MSB following aging in soil. These results indicate that MSB could be used for remediation of Cd and Pb contaminated soil and water.

References

[1] Abbas T, Rizwan M, Ali S, Zia-ur-Rehman M, Qayyum MF, Abbas F, Hannan F, Rinklebe J, Ok YS. Effect of biochar on cadmium bioavailability and uptake in wheat (Triticum aestivum L.) grown in a soil with aged contamination. Ecotox Environ Safety, 2017, 140: 37-47

[2] Aytekin M, Haykiri-Acma H, Yaman S. Hydrophobic and oleophilic carbon fiber aerogel for oil/water separation. Biomass Conv Biorefinery, 2023

[3] Azhar U, Ahmad H, Shafqat H, Babar M, Munir HMS, Sagir M, Arif M, Hassan A, Rachmadona N, Rajendran S. Remediation techniques for elimination of heavy metal pollutants from soil: a review. Environ Res, 2022, 214: 113918

[4] Bandara T, Franks A, Xu J, Bolan N, Wang H, Tang C. Chemical and biological immobilization mechanisms of potentially toxic elements in biochar-amended soils. Crit Rev Environ Sci Technol, 2020, 50(9): 903-978

[5] Boostani HR, Hardie AG, Najafi-Ghiri M, Khalili D. The effect of soil moisture regime and biochar application on lead (Pb) stabilization in a contaminated soil. Ecotoxicol Environ Saf, 2021, 208: 111626

[6] Cairns S, Chaudhuri S, Sigmund G, Robertson I, Hawkins N, Dunlop T, Hofmann T. Wood ash amended biochar for the removal of lead, copper, zinc and cadmium from aqueous solution. Environ Technol Innov, 2021, 24: 101961

[7] Cao Y, Xiao W, Shen G, Ji G, Zhang Y, Gao C, Han L. Carbonization and ball milling on the enhancement of Pb (II) adsorption by wheat straw: competitive effects of ion exchange and precipitation. Biores Technol, 2019, 273: 70-76

[8] Chen J, Wang P, Ding L, Yu T, Leng S, Chen J, Fan L, Li J, Wei L, Li J. The comparison study of multiple biochar stability assessment methods. J Anal Appl Pyrol, 2021, 156: 105070

[9] Chen S, Yang Q, Shi J, Ying Y, Liu Y. Porous biomass skeleton/Ni-Co LDH composite nanomaterials electrode with high rate capability for advanced supercapacitors. Colloids Surf, A, 2022, 635: 128078

[10] Das A, Jana A, Das D, Biswas S, Sheshadri H, Rao M, De S. Surfactant assisted APTES functionalization of graphene oxide intercalated layered double hydroxide (LDH) for uranium adsorption from alkaline leach liquor. J Clean Prod, 2023, 390: 136058

[11] Deng L, Zeng H, Shi Z, Zhang W, Luo J. Sodium dodecyl sulfate intercalated and acrylamide anchored layered double hydroxides: a multifunctional adsorbent for highly efficient removal of Congo red. J Colloid Interface Sci, 2018, 521: 172-182

[12] Deng S, Ke T, Wu Y, Zhang C, Hu Z, Yin H, Guo L, Chen L, Zhang D. Heavy metal exposure alters the uptake behavior of 16 priority polycyclic aromatic hydrocarbons (PAHs) by Pak Choi ( Brassica chinensis L.). Environ Sci Technol, 2018, 52(22): 13457-13468

[13] dos Santos GEDS, dos Santos Lins PV, de Magalhães Oliveira LMT, da Silva EO, Anastopoulos I, Erto A, Giannakoudakis DA, de Almeida ARF, da Silva Duarte JL, Meili L. Layered double hydroxides/biochar composites as adsorbents for water remediation applications: recent trends and perspectives. J Clean Prod, 2021, 284: 124755

[14] Eltaweil AS, Gaber NM, El-Subruiti GM, Omer AM. Dandelion-like Cu-Ni LDH-decorated biochar/aminated chitosan composite for boosting Fenton-like degradation of doxycycline: insights into performance and mechanism. J Mol Liq, 2024, 394: 123716

[15] Fan J, Cai C, Chi H, Reid BJ, Coulon F, Zhang Y, Hou Y. Remediation of cadmium and lead polluted soil using thiol-modified biochar. J Hazard Mater, 2020, 388: 122037

[16] Fang Q, Ye S, Yang H, Yang K, Zhou J, Gao Y, Lin Q, Tan X, Yang Z. Application of layered double hydroxide-biochar composites in wastewater treatment: recent trends, modification strategies, and outlook. J Hazard Mater, 2021, 420: 126569

[17] Feng X, Long R, Wang L, Liu C, Bai Z, Liu X. A review on heavy metal ions adsorption from water by layered double hydroxide and its composites. Sep Purif Technol, 2022, 284: 120099

[18] Feng X, Li X, Su B. Photocatalytic degradation performance of antibiotics by peanut shell biochar anchored NiCr-LDH nanocomposites fabricated by one-pot hydrothermal protocol. Colloids Surf, A, 2023, 666: 131337

[19] Gao X, Peng Y, Guo L, Wang Q, Guan C-Y, Yang F, Chen Q. Arsenic adsorption on layered double hydroxides biochars and their amended red and calcareous soils. J Environ Manage, 2020, 271: 111045

[20] Gholizadeh M, Hu X. Removal of heavy metals from soil with biochar composite: a critical review of the mechanism. J Environ Chem Eng, 2021, 9(5): 105830

[21] Gong H, Zhao L, Rui X, Hu J, Zhu N. A review of pristine and modified biochar immobilizing typical heavy metals in soil: applications and challenges. J Hazard Mater, 2022, 432: 128668

[22] He X, Zhong P, Qiu X. Remediation of hexavalent chromium in contaminated soil by Fe (II)-Al layered double hydroxide. Chemosphere, 2018, 210: 1157-1166

[23] Hu Y, Zhang S, Luo C, Wan L, Wu S, Baig SA, Xu X. Enhanced removal of Sb (V) from aqueous solutions using layered double hydroxide modified with sodium dodecyl sulfate. J Environ Chem Eng, 2022, 10(3): 107776

[24] Huang Z, Wang T, Shen M, Huang Z, Chong Y, Cui L. Coagulation treatment of swine wastewater by the method of in-situ forming layered double hydroxides and sludge recycling for preparation of biochar composite catalyst. Chem Eng J, 2019, 369: 784-792

[25] Hudcová B, Fein JB, Tsang DC, Komárek M. Mg-Fe LDH-coated biochars for metal (loid) removal: surface complexation modeling and structural change investigations. Chem Eng J, 2022, 432: 134360

[26] Jansson JK, Wu R. Soil viral diversity, ecology and climate change. Nat Rev Microbiol, 2023, 21(5): 296-311

[27] Ji X, Wan J, Wang X, Peng C, Wang G, Liang W, Zhang W. Mixed bacteria-loaded biochar for the immobilization of arsenic, lead, and cadmium in a polluted soil system: effects and mechanisms. Sci Total Environ, 2022, 811: 152112

[28] Ji Y, Zhang C, Zhang X, Xie P, Wu C, Jiang L. A high adsorption capacity bamboo biochar for CO₂ capture for low temperature heat utilization. Sep Purif Technol, 2022, 293: 121131

[29] Jia Y, Zhang Y, Fu J, Yuan L, Li Z, Liu C, Zhao D, Wang X. A novel magnetic biochar/MgFe-layered double hydroxides composite removing Pb²⁺ from aqueous solution: isotherms, kinetics and thermodynamics. Colloids Surf, A, 2019, 567: 278-287

[30] Jin X, Liu R, Wang H, Han L, Qiu M, Hu B. Functionalized porous nanoscale Fe₃O₄ particles supported biochar from peanut shell for Pb (II) ions removal from landscape wastewater. Environ Sci Pollut Res, 2022

[31] Kim P, Johnson A, Edmunds CW, Radosevich M, Vogt F, Rials TG, Labbé N. Surface functionality and carbon structures in lignocellulosic-derived biochars produced by fast pyrolysis. Energy Fuels, 2011, 25(10): 4693-4703

[32] Kim H-S, Kim K-R, Kim H-J, Yoon J-H, Yang JE, Ok YS, Owens G, Kim K-H. Effect of biochar on heavy metal immobilization and uptake by lettuce (Lactuca sativa L.) in agricultural soil. Environ Earth Sci, 2015, 74: 1249-1259

[33] Klasson KT. Biochar characterization and a method for estimating biochar quality from proximate analysis results. Biomass Bioenerg, 2017, 96: 50-58

[34] Kołodyńska D, Wnętrzak R, Leahy J, Hayes M, Kwapiński W, Hubicki Z. Kinetic and adsorptive characterization of biochar in metal ions removal. Chem Eng J, 2012, 197: 295-305

[35] Lawrinenko M, Laird DA, Johnson RL, Jing D. Accelerated aging of biochars: impact on anion exchange capacity. Carbon, 2016, 103: 217-227

[36] Lehmann J, Gaunt J, Rondon M. Bio-char sequestration in terrestrial ecosystems–a review. Mitig Adapt Strat Glob Change, 2006, 11: 403-427

[37] Leng L, Huang H, Li H, Li J, Zhou W. Biochar stability assessment methods: a review. Sci Total Environ, 2019, 647: 210-222

[38] Li Y, Yu H, Liu L, Yu H. Application of co-pyrolysis biochar for the adsorption and immobilization of heavy metals in contaminated environmental substrates. J Hazard Mater, 2021, 420: 126655

[39] Liang X, Su Y, Wang X, Liang C, Tang C, Wei J, Liu K, Ma J, Yu F, Li Y. Insights into the heavy metal adsorption and immobilization mechanisms of CaFe-layered double hydroxide corn straw biochar: synthesis and application in a combined heavy metal-contaminated environment. Chemosphere, 2023, 313: 137467

[40] Lin L, Li Z, Liu X, Qiu W, Song Z. Effects of Fe-Mn modified biochar composite treatment on the properties of As-polluted paddy soil. Environ Pollut, 2019, 244: 600-607

[41] Liu W-J, Jiang H, Yu H-Q. Development of biochar-based functional materials: toward a sustainable platform carbon material. Chem Rev, 2015, 115(22): 12251-12285

[42] Liu G, Zheng H, Jiang Z, Zhao J, Wang Z, Pan B, Xing B. Formation and physicochemical characteristics of nano biochar: insight into chemical and colloidal stability. Environ Sci Technol, 2018, 52(18): 10369-10379

[43] Liu R, Zhang Y, Hu B, Wang H. Improved Pb (II) removal in aqueous solution by sulfide@ biochar and polysaccharose-FeS@ biochar composites: efficiencies and mechanisms. Chemosphere, 2022, 287: 132087

[44] Liu Z, Xu Z, Xu L, Buyong F, Chay TC, Li Z, Cai Y, Hu B, Zhu Y, Wang X. Modified biochar: synthesis and mechanism for removal of environmental heavy metals. Carbon Res, 2022, 1(1): 8

[45] Liu G, Zhang X, Liu H, He Z, Show PL, Vasseghian Y, Wang C. Biochar/layered double hydroxides composites as catalysts for treatment of organic wastewater by advanced oxidation processes: a review. Environ Res, 2023

[46] Luo X, Chen W, Liu Q, Wang X, Miao J, Liu L, Zheng H, Liu R, Li F. Corn straw biochar addition elevated phosphorus availability in a coastal salt-affected soil under the conditions of different halophyte litter input and moisture contents. Sci Total Environ, 2024, 908: 168355

[47] Luo Y, He Y, Zhou D, Pan L, Wu Y. Organic amendment application affects the release behaviour, bioavailability, and speciation of heavy metals in zinc smelting slag: Insight into dissolved organic matter. J Hazard Mater, 2024, 465: 133105

[48] Lyu H, Zhao H, Tang J, Gong Y, Huang Y, Wu Q, Gao B. Immobilization of hexavalent chromium in contaminated soils using biochar supported nanoscale iron sulfide composite. Chemosphere, 2018, 194: 360-369

[49] Ma R, Yan X, Mi X, Wu Y, Qian J, Zhang Q, Chen G-H. Enhanced catalytic degradation of aqueous doxycycline (DOX) in Mg-Fe-LDH@ biochar composite-activated peroxymonosulfate system: performances, degradation pathways, mechanisms and environmental implications. Chem Eng J, 2021, 425: 131457

[50] Nguyen T-B, Truong Q-M, Chen C-W, Doong R-A, Chen W-H, Dong C-D. Mesoporous and adsorption behavior of algal biochar prepared via sequential hydrothermal carbonization and ZnCl₂ activation. Biores Technol, 2022, 346: 126351

[51] Palansooriya KN, Li J, Dissanayake PD, Suvarna M, Li L, Yuan X, Sarkar B, Tsang DC, Rinklebe Jr, Wang X. Prediction of soil heavy metal immobilization by biochar using machine learning. Environ Sci Technol, 2022, 56(7): 4187-4198

[52] Pan X, Shi M, Chen X, Kuang S, Ullah H, Lu H, Riaz L. An investigation into biochar, acid-modified biochar, and wood vinegar on the remediation of saline-alkali soil and the growth of strawberries. Front Environ Sci, 2022, 10: 1057384

[53] Pan X, Wang X, Liu L, Kuang S, Zheng H. CO₂ and H₂O as sweep gases elevated carbon stability and decreased phytotoxicity of biochars. Chem Eng J, 2023, 472: 145035

[54] Qi X, Yin H, Zhu M, Yu X, Shao P, Dang Z. MgO-loaded nitrogen and phosphorus self-doped biochar: High-efficient adsorption of aquatic Cu²⁺, Cd²⁺, and Pb²⁺ and its remediation efficiency on heavy metal contaminated soil. Chemosphere, 2022, 294: 133733

[55] Qiu M, Liu L, Ling Q, Cai Y, Yu S, Wang S, Fu D, Hu B, Wang X. Biochar for the removal of contaminants from soil and water: a review. Biochar, 2022, 4(1): 19

[56] Rahman S, Navarathna CM, Das NK, Alchouron J, Reneau P, Stokes S, Thirumalai RV, Perez F, Hassan EB, Mohan D. High capacity aqueous phosphate reclamation using Fe/Mg-layered double hydroxide (LDH) dispersed on biochar. J Colloid Interface Sci, 2021, 597: 182-195

[57] Rauret G, López-Sánchez J, Sahuquillo A, Rubio R, Davidson C, Ure A, Quevauviller P. Improvement of the BCR three step sequential extraction procedure prior to the certification of new sediment and soil reference materials. J Environ Monit, 1999, 1(1): 57-61

[58] Ren S, Song C, Ye S, Cheng C, Gao P. The spatiotemporal variation in heavy metals in China’s farmland soil over the past 20 years: a meta-analysis. Sci Total Environ, 2022, 806: 150322

[59] Riaz M, Kamran M, Fang Y, Wang Q, Cao H, Yang G, Deng L, Wang Y, Zhou Y, Anastopoulos I. Arbuscular mycorrhizal fungi-induced mitigation of heavy metal phytotoxicity in metal contaminated soils: a critical review. J Hazard Mater, 2021, 402: 123919

[60] Sachdeva S, Kumar R, Sahoo PK, Nadda AK. Recent advances in biochar amendments for immobilization of heavy metals in an agricultural ecosystem: a systematic review. Environ Pollut, 2023, 319: 120937

[61] Shah V, Daverey A. Phytoremediation: a multidisciplinary approach to clean up heavy metal contaminated soil. Environ Technol Innov, 2020, 18: 100774

[62] Shao P, Yin H, Li Y, Cai Y, Yan C, Yuan Y, Dang Z. Remediation of Cu and as contaminated water and soil utilizing biochar supported layered double hydroxide: Mechanisms and soil environment altering. J Environ Sci, 2023, 126: 275-286

[63] Shearer L, Pap S, Gibb SW. Removal of pharmaceuticals from wastewater: a review of adsorptive approaches, modelling and mechanisms for metformin and macrolides. J Environ Chem Eng, 2022, 10(4): 108106

[64] Sun Y, Li H, Guo G, Semple KT, Jones KC. Soil contamination in China: current priorities, defining background levels and standards for heavy metals. J Environ Manage, 2019, 251: 109512

[65] Trakal L, Bingöl D, Pohořelý M, Hruška M, Komárek M. Geochemical and spectroscopic investigations of Cd and Pb sorption mechanisms on contrasting biochars: engineering implications. Biores Technol, 2014, 171: 442-451

[66] Vithanage M, Ashiq A, Ramanayaka S, Bhatnagar A. Implications of layered double hydroxides assembled biochar composite in adsorptive removal of contaminants: current status and future perspectives. Sci Total Environ, 2020, 737: 139718

[67] Wan X, Li C, Parikh SJ. Simultaneous removal of arsenic, cadmium, and lead from soil by iron-modified magnetic biochar. Environ Pollut, 2020, 261: 114157

[68] Wang J, Gao F, Du X, Ma X, Hao X, Ma W, Wang K, Guan G, Abudula A. A high-performance electroactive PPy/rGO/NiCo-LDH hybrid film for removal of dilute dodecyl sulfonate ions. Electrochim Acta, 2020, 331: 135288

[69] Wang S, Kwak J-H, Islam MS, Naeth MA, El-Din MG, Chang SX. Biochar surface complexation and Ni (II), Cu (II), and Cd (II) adsorption in aqueous solutions depend on feedstock type. Sci Total Environ, 2020, 712: 136538

[70] Wang D, Repo E, He F, Zhang X, Xiang H, Yang W, Min X, Zhao F. Dual functional sites strategies toward enhanced heavy metal remediation: interlayer expanded Mg-Al layered double hydroxide by intercalation with L-cysteine. J Hazard Mater, 2022, 439: 129693

[71] Wang H, Nan Q, Waqas M, Wu W. Stability of biochar in mineral soils: assessment methods, influencing factors and potential problems. Sci Total Environ, 2022, 806: 150789

[72] Wu J, Wang T, Zhang Y, Pan W-P. The distribution of Pb (II)/Cd (II) adsorption mechanisms on biochars from aqueous solution: considering the increased oxygen functional groups by HCl treatment. Biores Technol, 2019, 291: 121859

[73] Wu F, Chen L, Hu P, Zhou X, Zhou H, Wang D, Lu X, Mi B. Comparison of properties, adsorption performance and mechanisms to Cd (II) on lignin-derived biochars under different pyrolysis temperatures by microwave heating. Environ Technol Innov, 2022, 25: 102196

[74] Wu X, Liu J, Liu X, Wu X, Du Y. Fabrication of carbon doped Cu-based oxides as superior NH3-SCR catalysts via employing sodium dodecyl sulfonate intercalating CuMgAl-LDH. J Catal, 2022, 407: 265-280

[75] Xu J, Liu C, Hsu P-C, Zhao J, Wu T, Tang J, Liu K, Cui Y. Remediation of heavy metal contaminated soil by asymmetrical alternating current electrochemistry. Nat Commun, 2019, 10(1): 2440

[76] Yang X, Wan Y, Zheng Y, He F, Yu Z, Huang J, Wang H, Ok YS, Jiang Y, Gao B. Surface functional groups of carbon-based adsorbents and their roles in the removal of heavy metals from aqueous solutions: a critical review. Chem Eng J, 2019, 366: 608-621

[77] Yang Y, Tan X, Almatrafi E, Ye S, Song B, Chen Q, Yang H, Fu Q, Deng Y, Zeng Z. Alfalfa biochar supported Mg-Fe layered double hydroxide as filter media to remove trace metal (loid) s from stormwater. Sci Total Environ, 2022, 844: 156835

[78] Yuan C, Gao B, Peng Y, Gao X, Fan B, Chen Q. A meta-analysis of heavy metal bioavailability response to biochar aging: importance of soil and biochar properties. Sci Total Environ, 2021, 756: 144058

[79] Zhang M, Zhao C, Li J, Xu L, Wei F, Hou D, Sarkar B, Ok YS. Organo-layered double hydroxides for the removal of polycyclic aromatic hydrocarbons from soil washing effluents containing high concentrations of surfactants. J Hazard Mater, 2019, 373: 678-686

[80] Zhang P, Xiang M, Li P, Ouyang S, He T, Deng Q. The enhancement roles of sulfate on the adsorption of sodium dodecylsulfate by calcium-based layered double hydroxide: microstructure and thermal behaviors. Environ Sci Pollut Res, 2019, 26: 19320-19326

[81] Zhang H, Lee J-W, Nasti G, Handy R, Abate A, Grätzel M, Park N-G. Lead immobilization for environmentally sustainable perovskite solar cells. Nature, 2023, 617(7962): 687-695

[82] Zhao D, Sheng G, Hu J, Chen C, Wang X. The adsorption of Pb (II) on Mg₂Al layered double hydroxide. Chem Eng J, 2011, 171(1): 167-174

[83] Zhao M, Ma X, Liao X, Cheng S, Liu Q, Wang H, Zheng H, Li X, Luo X, Zhao J. Characteristics of algae-derived biochars and their sorption and remediation performance for sulfamethoxazole in marine environment. Chem Eng J, 2022, 430: 133092

[84] Zheng H, Feng N, Yang T, Shi M, Wang X, Zhang Q, Zhao J, Li F, Sun K, Xing B. Individual and combined applications of biochar and pyroligneous acid mitigate dissemination of antibiotic resistance genes in agricultural soil. Sci Total Environ, 2021, 796: 148962

[85] Zhou X, Zhu Y, Niu Q, Zeng G, Lai C, Liu S, Huang D, Qin L, Liu X, Li B. New notion of biochar: a review on the mechanism of biochar applications in advannced oxidation processes. Chem Eng J, 2021, 416: 129027

[86] Zong P, Wang S, Liang G, Shao M, Yan N, Xu X, Xu M, Li W, Yang Y, Chen J. Eco-friendly approach for effective removal for Congo red dye from wastewater using reusable Zn-Al layered double hydroxide anchored on multiwalled carbon nanotubes supported sodium dodecyl sulfonate composites. J Mol Liq, 2022, 349: 118468

Funding

Major Scientific and Technological Innovation Project of Shandong Province(2021CXGC011206)

RIGHTS & PERMISSIONS

The Author(s)