Adsorption characteristics and mechanism of W(VI) from aqueous solution using MgAl layered double hydroxide and its calcined product
YUAN Xiu-juan1,2,3, ZENG Ping1,2, REN Si-li1,2, LUO Wu-hui1,2,4
1. Jiangxi Key Laboratory of Mining & Metallurgy Environmental Pollution Control, Ganzhou 341000, China; 2. School of Resources and Environmental Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, China; 3. Guangdong Fuyuan Rare Earth Co. Ltd., Meizhou 514000, China; 4. Jiangxi Academy of Eco-Environmental Sciences and Planning, Nanchang 330039, China
Abstract：A nitrate-type layered double hydroxide (LDH) with the Mg/Al molar ratio of 2:1 was prepared via microwave aging method. The adsorption characteristics of W(VI) using LDH and its calcined product (CLDH) were systematically studied, and the involved mechanisms were elucidated through the structural characterization of LDH and CLDH before and after adsorption. The adsorption kinetics of LDH and CLDH to W(VI) was well fitted with the pseudo-second order model, indicating that chemisorption was the key process determining the adsorption rate. Both LDH and CLDH showed high affinity to W(VI), showing the maximum uptakes of 176.0 and 124.5mg/g, respectively, which are far higher than the analogous LDH. The optimum pH range for W(VI) adsorption on LDH was 4.0~10.0, while the acidic condition was conducive to W(VI) adsorption by CLDH. Compared with CLDH, LDH showed the higher adsorption capacity, faster adsorption rate, and less influences on water qualities (e.g., less releases of Mg and Al and change of pH), suggesting that the original LDH is more applicable for W(VI) adsorption. The main mechanisms of W(VI) adsorption on LDH include ion exchange, outer-sphere complexation, and inner-sphere complexation, while for the case of CLDH, the intercalation of paratungstate (W7O246-) during the reconstruction of layered structure was also involved. The above results indicate that both LDH and CLDH synthesized via the microwave radiation are favorable adsorbents with the superior performance in removal of W(VI) from the polluted water.
Koutsospyros A, Braida W, Christodoulatos C, et al. A review of tungsten:From environmental obscurity to scrutiny[J]. Journal of Hazardous Materials, 2006,136(1):1-19.
[2]
Strigul N. Does speciation matter for tungsten ecotoxicology?[J]. Ecotoxicology and Environmental Safety, 2010,73(6):1099-1113.
[3]
EPA. Emerging Contaminant-Tungsten[J]. 2008.
[4]
Hallstrom L P B, Alakangas L, Martinsson O. Scheelite weathering and tungsten (W) mobility in historical oxidic-sulfidic skarn tailings at Yxsjoberg, Sweden[J]. Environmental Science and Pollution Research, 2020,27(6):6180-6192.
[5]
Bostick B C, Sun J, Landis J D, et al. Tungsten speciation and solubility in munitions-impacted soils[J]. Environmental Science & Technology, 2018,52(3):1045-1053.
[6]
刘足根,杨国华,杨帆,等.赣南钨矿区土壤重金属含量与植物富集特征[J]. 生态学杂志, 2008,27(8):1345-1350. Liu Z G, Yang G H, Yang F, et al. Soil heavy metals concentrations and their enrichment characteristics by plants in tungsten mine areas of South Jiangxi[J]. Chinese Journal of Ecology, 2008,27(8):1345-1350.
[7]
何纪力,徐光炎,朱惠民.江西省土壤环境背景值研究[M]. 北京:中国环境科学出版社, 2006. He J L, Xu G Y, Zhu H M. Background value of soil environment in Jiangxi province[M]. Beijing:China Environmental Science Press, 2006.
[8]
陈明,李凤果,师艳丽,等.赣南桃江河表层沉积物钨赋存特征及风险分析[J]. 中国环境科学, 2019,39(4):1715-1723. Chen M, Li F G, Shi Y L, et al. Occurrence characteristics and risk assessment of tungsten in surface sediments of Taojiang River in Southern Jiangxi Province[J]. China Environmental Science, 2019, 39(4):1715-1723.
[9]
Kang J, Chen C, Sun W, et al. A significant improvement of scheelite recovery using recycled flotation wastewater treated by hydrometallurgical waste acid[J]. Journal of Cleaner Production, 2017, 151:419-426.
[10]
Hsu S C, Hsieh H L, Chen C P, et al. Tungsten and other heavy metal contamination in aquatic environments receiving wastewater from semiconductor manufacturing[J]. Journal of Hazardous Materials, 2011,189(1/2):193-202.
[11]
Osterburg A R, Robinson C T, Mokashi V, et al. Oral tungstate (Na2 WO4) exposure reduces adaptive immune responses in mice after challenge[J]. Journal of Immunotoxicology, 2014,11(2):148-159.
[12]
Mccain W C, Crouse L C, Bazar M A, et al. Subchronic oral toxicity of sodium tungstate in sprague-dawley rats[J]. International Journal of Toxicology, 2015,34(4):336-345.
[13]
Sachdeva S, Kushwaha P, Flora S J. Effects of sodium tungstate on oxidative stress enzymes in rats[J]. Toxicology Mechanisms and Methods, 2013,23(7):519-527.
[14]
Gadilgereyeva B Z, Beisekova M, Kurmanbayeva A, et al. Influence of molybdenum and tungsten on the enzymatic activity of molybdenum enzymes[J]. Plant Genetics, 2019,57:75.
[15]
Preiner J, Wienkoop S, Weckwerth W, et al. Molecular mechanisms of tungsten toxicity differ for Glycine max depending on nitrogen regime[J]. Frontiers in Plant Science, 2019,10:367-390.
[16]
Dawood M F, Azooz M M. Concentration-dependent effects of tungstate on germination, growth, lignification-related enzymes, antioxidants, and reactive oxygen species in broccoli (Brassica oleracea var.italica L.)[J]. Environmental Science and Pollution Research, 2019,26(36):36441-36457.
[17]
Adamakis I S, Eleftheriou E P. Structural evidence of programmed cell death induction by tungsten in root tip cells of Pisum sativum[J]. Plants, 2019,8(3):62-79.
[18]
De Palma G, Manini P, Sarnico M, et al. Biological monitoring of tungsten (and cobalt) in workers of a hard metal alloy industry[J]. International Archives of Occupational and Environmental Health, 2010,83(2):173-181.
[19]
Coates J R E O, Watson J H. Diffuse interstitial lung disease in tungsten carbide workers[J]. Annals of Internal Medicine, 1971,75(5):709-716.
[20]
Osterburg A R, Robinson C T, Schwemberger S, et al. Sodium tungstate (Na2 WO4) exposure increases apoptosis in human peripheral blood lymphocytes[J]. Journal of Immunotoxicology, 2010,7(3):174-182.
[21]
Harris R M, Williams T D, Waring R H, et al. Molecular basis of carcinogenicity of tungsten alloy particles[J]. Toxicology and Applied Pharmacology, 2015,283(3):223-233.
[22]
James B, Zhang W, Sun P, et al. Tungsten (W) bioavailability in paddy rice soils and its accumulation in rice (Oryza sativa)[J]. International Journal of Environmental Health Research, 2017,27(6):487-497.
[23]
Lin C, Li R, Cheng H, et al. Tungsten distribution in soil and rice in the vicinity of the world's largest and longest-operating tungsten mine in China[J]. PLoS One, 2014,9(3):e91981.
[24]
Lindsay J H, Kennedy A J, Seiter-Moser J M, et al. Uptake kinetics and trophic transfer of tungsten from cabbage to a herbivorous animal model[J]. Environmental Science & Technology, 2017,51(23):13755-13762.
[25]
Sanitary Rules and Norms of Russian Federation[Z]. Moscow, 1996.
[26]
Ogi T, Makino T, Nagai S, et al. Facile and efficient removal of tungsten anions using lysine-promoted precipitation for recycling high-purity tungsten[J]. ACS Sustainable Chemistry & Engineering, 2017,5(4):3141-3147.
[27]
Makino T, Nagai S, Iskandar F, et al. Recovery and recycling of tungsten by alkaline leaching of scrap and charged amino group assisted precipitation[J]. ACS Sustainable Chemistry & Engineering, 2018,6(3):4246-4252.
[28]
Muir B, Andrunik D, Hyla J, et al. The removal of molybdates and tungstates from aqueous solution by organo-smectites[J]. Applied Clay Science, 2017,136:8-17.
[29]
Sun J, Bostick B C. Effects of tungstate polymerization on tungsten(VI) adsorption on ferrihydrite[J]. Chemical Geology, 2015,417:21-31.
[30]
Cao Y, Guo Q, Shu Z, et al. Tungstate removal from aqueous solution by nanocrystalline iowaite:An iron-bearing layered double hydroxide[J]. Environmental Pollution, 2019,247:118-127.
[31]
Luo L, Guo Q, Cao Y. Uptake of aqueous tungsten and molybdenum by a nitrate intercalated,pyroaurite-like anion exchangeable clay[J]. Applied Clay Science, 2019,180:105179.
[32]
Ogata F, Nakamura T, Ueta E, et al. Adsorption of tungsten ion with a novel Fe-Mg type hydrotalcite prepared at different Mg2+/Fe3+ ratios[J]. Journal of Environmental Chemical Engineering, 2017,5(4):3083-3090.
[33]
Rives V, Ulibarri M A A. Layered double hydroxides (LDH) intercalated with metal coordination compounds and oxometalates[J]. Coordination Chemistry Reviews, 1999,181(1):61-120.
[34]
Benito P, Herrero M, Labajos F M, et al. Effect of post-synthesis microwave-hydrothermal treatment on the properties of layered double hydroxides and related materials[J]. Applied Clay Science, 2010,48(1/2):218-227.
[35]
Qiu X, Wang W. Removal of borate by layered double hydroxides prepared through microwave-hydrothermal method[J]. Journal of Water Process Engineering, 2017,17:271-276.
[36]
胡小平,衡惠敏,卢涛,等.镁铝层状双金属氢氧化物的制备及表征[J]. 中国粉体技术, 2012,18(3):31-35. Hu X P, Heng H M, Lu T, et al. Synthesis and characterization of Mg-Al layered double hydroxides[J]. China Powder Science and Technology, 2012,18(3):31-35.
[37]
Jung K W, Lee S Y, Choi J W, et al. 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[J]. Chemical Engineering Journal, 2021,420:129775.
[38]
Yan H, Chen Q, Liu J, et al. Phosphorus recovery through adsorption by layered double hydroxide nano-composites and transfer into a struvite-like fertilizer[J]. Water Research, 2018,145:721-730.
[39]
Ho Y S, Mckay G. Pseudo-second order model for sorption processes[J]. Process Biochemistry, 1999,34(5):451-465.
[40]
Lee S H, Tanaka M, Takahashi Y, et al. Enhanced adsorption of arsenate and antimonate by calcined Mg/Al layered double hydroxide:Investigation of comparative adsorption mechanism by surface characterization[J]. Chemosphere, 2018,211:903-911.
[41]
Chen Y, An Z, Chen M. Competition mechanism study of Mg+H2O and MgO+H2O reaction[J]. IOP Conference Series:Materials Science and Engineering, 2018,394:022015.
[42]
Davantès A, Costa D, Lefèvre G. Infrared study of (poly)tungstate ions in solution and sorbed into layered double hydroxides:Vibrational calculations and in situ analysis[J]. The Journal of Physical Chemistry C, 2015,119(22):12356-12364.
[43]
Hulea V, Maciuca A L, Fajula F, et al. Catalytic oxidation of thiophenes and thioethers with hydrogen peroxide in the presence of W-containing layered double hydroxides[J]. Applied Catalysis A:General, 2006,313(2):200-207.
[44]
Blesa M A, Weisz A D, Morando P J, et al. The interaction of metal oxide surfaces with complexing agents dissolved in water[J]. Coordination Chemistry Reviews, 2000,196(1):31-63.
[45]
Jobbágy M, Regazzoni A E. Dissolution of nano-size Mg-Al-Cl hydrotalcite in aqueous media[J]. Applied Clay Science, 2011, 51(3):366-369.
[46]
Simoes M C, Hughes K J, Ingham D B, et al. Estimation of the thermochemical radii and ionic volumes of complex ions[J]. Inorganic Chemistry, 2017,56(13):7566-7573.
[47]
Xu J, Song Y, Zhao Y, et al. Chloride removal and corrosion inhibitions of nitrate,nitrite-intercalated MgAl layered double hydroxides on steel in saturated calcium hydroxide solution[J]. Applied Clay Science, 2018,163:129-136.
[48]
Li A, Zhang Y, Ge W, et al. Removal of heavy metals from wastewaters with biochar pyrolyzed from MgAl-layered double hydroxide-coated rice husk:Mechanism and application[J]. Bioresource Technology, 2022,347:126425.
[49]
Wang S L, Wang P C. In situ XRD and ATR-FTIR study on the molecular orientation of interlayer nitrate in Mg/Al-layered double hydroxides in water[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2007,292(2/3):131-138.
[50]
Fang L, Hou J, Xu C, et al. Enhanced removal of natural organic matters by calcined Mg/Al layered double hydroxide nanocrystalline particles:Adsorption, reusability and mechanism studies[J]. Applied Surface Science, 2018,442:45-53.
[51]
Wang S L, Liu C H, Wang M K, et al. Arsenate adsorption by Mg/Al-NO3 layered double hydroxides with varying the Mg/Al ratio[J]. Applied Clay Science, 2009,43(1):79-85.
[52]
Wang H, Yang Z, Zhan X, et al. NiAlZrW hydrodesulfurization catalysts derived from tungstate intercalated NiAlZr layered double hydroxides[J]. Fuel Processing Technology, 2017,160:178-184.
[53]
Hur H, Reeder R J. Formation of CoAl layered double hydroxide on the boehmite surface and its role in tungstate sorption[J]. Journal of Environmental Sciences (China), 2018,65:103-115.
[54]
Del Arco M, Carriazo D, Gutiérrez S, et al. Synthesis and characterization of new Mg2Al-paratungstate layered double hydroxides[J]. Inorganic Chemistry, 2004,43(1):375-384.
[55]
Khitous M, Salem Z, Halliche D. Removal of phosphate from industrial wastewater using uncalcined MgAl-NO3 layered double hydroxide:batch study and modeling[J]. Desalination and Water Treatment, 2016,57(34):15920-15931.
[56]
Qiu X, Sasaki K, Takaki Y, et al. Mechanism of boron uptake by hydrocalumite calcined at different temperatures[J]. Journal of Hazardous Materials, 2015,287:268-277.
[57]
Zhang P, Qian G, Cheng H, et al. Near-infrared and mid-infrared investigations of Na-dodecylbenzenesulfate intercalated into hydrocalumite chloride (CaAl-LDH-Cl)[J]. Spectrochimica Acta Part A:Molecular and Biomolecular Spectroscopy, 2011,79(3):548-553.
[58]
Xu S, Zhao J, Deng L, et al. Adsorption mechanism of borate with different calcined layered double hydroxides in a molar ratio of 3:1[J]. Desalination and Water Treatment, 2019,155:296-310.
