Effect of precipitation pH and coexisting magnesium ion on phosphate adsorption onto hydrous zirconium oxide
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摘要
To understand the effect of precipitation pH and coexisting Mg~(2+) on phosphate adsorption onto zirconium oxide(ZrO_2), ZrO_2 particles precipitated at pH 5.3, 7.1 and 10.5, i.e., ZrO_2(5.3), ZrO_2(7.1)and ZrO_2(10.5), respectively were prepared and characterized, then their adsorption performance and mechanism in the absence and presence of Mg~(2+) were comparatively investigated in this study. The results showed that the Elovich, pseudo-second-order and Langmuir isotherm models correlated with the experimental data well. The adsorption mechanism involved the complexation between phosphate and zirconium. Coexisting Mg~(2+) slightly inhibited the adsorption of phosphate on ZrO_2(5.3), including the adsorption capacity and rate, but coexisting Mg~(2+) greatly increased the adsorption capacity and rate for ZrO_2(7.1)and ZrO_2(10.5). The enhanced adsorption of phosphate on ZrO_2(7.1) and ZrO_2(10.5) in the presence of Mg~(2+) was mainly due to the formation of Mg~(2+)-HPO_4~(2-) ion pair(MgHPO_4~0) in the solution and then the adsorption of MgHPO_4~0 on the adsorbent surface, forming the phosphatebridged ternary complex Zr(OPO_3H)Mg. In the absence of Mg~(2+) , the maximum phosphate adsorption capacity at pH 7 calculated from the Langmuir isotherm model decreased in the order of ZrO 2(7.1)(67.3 mg/g) > ZrO_2(5.3)(53.6 mg/g) ≈ ZrO_2(10.5)(53.1 mg/g), but it followed the order of Zr O2(7.1)(97.0 mg/g) > ZrO_2(10.5)(79.7 mg/g) > ZrO_2(5.3)(51.3 mg/g) in the presence of Mg~(2+) . The results of this work suggest that ZrO_2(7.1) is more suitable for use as an adsorbent for the effective removal of phosphate from municipal wastewater than ZrO_2(5.3) and ZrO_2(10.5),because Mg~(2+) is generally present in this wastewater.
To understand the effect of precipitation pH and coexisting Mg~(2+) on phosphate adsorption onto zirconium oxide(ZrO_2), ZrO_2 particles precipitated at pH 5.3, 7.1 and 10.5, i.e., ZrO_2(5.3), ZrO_2(7.1)and ZrO_2(10.5), respectively were prepared and characterized, then their adsorption performance and mechanism in the absence and presence of Mg~(2+) were comparatively investigated in this study. The results showed that the Elovich, pseudo-second-order and Langmuir isotherm models correlated with the experimental data well. The adsorption mechanism involved the complexation between phosphate and zirconium. Coexisting Mg~(2+) slightly inhibited the adsorption of phosphate on ZrO_2(5.3), including the adsorption capacity and rate, but coexisting Mg~(2+) greatly increased the adsorption capacity and rate for ZrO_2(7.1)and ZrO_2(10.5). The enhanced adsorption of phosphate on ZrO_2(7.1) and ZrO_2(10.5) in the presence of Mg~(2+) was mainly due to the formation of Mg~(2+)-HPO_4~(2-) ion pair(MgHPO_4~0) in the solution and then the adsorption of MgHPO_4~0 on the adsorbent surface, forming the phosphatebridged ternary complex Zr(OPO_3H)Mg. In the absence of Mg~(2+) , the maximum phosphate adsorption capacity at pH 7 calculated from the Langmuir isotherm model decreased in the order of ZrO 2(7.1)(67.3 mg/g) > ZrO_2(5.3)(53.6 mg/g) ≈ ZrO_2(10.5)(53.1 mg/g), but it followed the order of Zr O2(7.1)(97.0 mg/g) > ZrO_2(10.5)(79.7 mg/g) > ZrO_2(5.3)(51.3 mg/g) in the presence of Mg~(2+) . The results of this work suggest that ZrO_2(7.1) is more suitable for use as an adsorbent for the effective removal of phosphate from municipal wastewater than ZrO_2(5.3) and ZrO_2(10.5),because Mg~(2+) is generally present in this wastewater.
To understand the effect of precipitation pH and coexisting Mg~(2+) on phosphate adsorption onto zirconium oxide(ZrO_2), ZrO_2 particles precipitated at pH 5.3, 7.1 and 10.5, i.e., ZrO_2(5.3), ZrO_2(7.1)and ZrO_2(10.5), respectively were prepared and characterized, then their adsorption performance and mechanism in the absence and presence of Mg~(2+) were comparatively investigated in this study. The results showed that the Elovich, pseudo-second-order and Langmuir isotherm models correlated with the experimental data well. The adsorption mechanism involved the complexation between phosphate and zirconium. Coexisting Mg~(2+) slightly inhibited the adsorption of phosphate on ZrO_2(5.3), including the adsorption capacity and rate, but coexisting Mg~(2+) greatly increased the adsorption capacity and rate for ZrO_2(7.1)and ZrO_2(10.5). The enhanced adsorption of phosphate on ZrO_2(7.1) and ZrO_2(10.5) in the presence of Mg~(2+) was mainly due to the formation of Mg~(2+)-HPO_4~(2-) ion pair(MgHPO_4~0) in the solution and then the adsorption of MgHPO_4~0 on the adsorbent surface, forming the phosphatebridged ternary complex Zr(OPO_3H)Mg. In the absence of Mg~(2+) , the maximum phosphate adsorption capacity at pH 7 calculated from the Langmuir isotherm model decreased in the order of ZrO 2(7.1)(67.3 mg/g) > ZrO_2(5.3)(53.6 mg/g) ≈ ZrO_2(10.5)(53.1 mg/g), but it followed the order of Zr O2(7.1)(97.0 mg/g) > ZrO_2(10.5)(79.7 mg/g) > ZrO_2(5.3)(51.3 mg/g) in the presence of Mg~(2+) . The results of this work suggest that ZrO_2(7.1) is more suitable for use as an adsorbent for the effective removal of phosphate from municipal wastewater than ZrO_2(5.3) and ZrO_2(10.5),because Mg~(2+) is generally present in this wastewater.
引文
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Du,X.L.,Han,Q.,Li,J.Q.,Li,H.Y.,2017.The behavior of phosphate adsorption and its reactions on the surfaces of Fe-Mn oxide adsorbent.J.Taiwan Inst.Chem.Eng.76,167-175.
Fang,L.P.,Wu,B.L.,Lo,I.M.C.,2017.Fabrication of silica-free superparamagnetic ZrO2@Fe3O4with enhanced phosphate recovery from sewage:performance and adsorption mechanism.Chem.Eng.J.319,258-267.
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Fu,D.D.,He,Z.Q.,Su,S.S.,Xu,B.,Liu,Y.L.,Zhao,Y.P.,2017.Fabrication ofα-FeOOH decorated graphene oxide-carbon nanotubes aerogel and its application in adsorption of arsenic species.J.Colloid Interface Sci.505,105-114.
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Hu,P.,Liu,Q.,Wang,J.,Huang,R.H.,2017.Phosphate removal by Ce(III)-impregnated crosslinked chitosan complex from aqueous solutions.Polym.Eng.Sci.57,44-51.
Huang,W.Y.,Zhang,Y.M.,Li,D.,2017.Adsorptive removal of phosphate from water using mesoporous materials:a review.J.Environ.Manag.193,470-482.
Hunger,S.,Cho,H.,Sims,J.T.,Sparks,D.L.,2004.Direct speciation of phosphorus in alum-amended poultry litter:solid-state31PNMR investigation.Environ.Sci.Technol.38,674-681.
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Ju,X.Q.,Hou,J.F.,Tang,Y.Q.,Sun,Y.B.,Zheng,S.R.,Xu,Z.Y.,2016.ZrO2nanoparticles confined in CMK-3 as highly effective sorbent for phosphate adsorption.Microporous Mesoporous Mater.230,188-195.
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Li,R.H.,Wang,J.J.,Zhou,B.Y.,Awasthi,M.K.,Ali,A.,Zhang,Z.Q.,et al.,2016a.Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios.Sci.Total Environ.559,121-129.
Li,X.,Zhang,Y.,Jing,L.,He,X.,2016b.Novel N-doped CNTs stabilized Cu2O nanoparticles as adsorbent for enhancing removal of Malachite Green and tetrabromobisphenol A.Chem.Eng.J.292,326-339.
Lin,B.,Hua,M.,Zhang,Y.Y.,Zhang,W.M.,Lv,L.,Pan,B.C.,2017a.Effects of organic acids of different molecular size on phosphate removal by HZO-201 nanocomposite.Chemosphere166,422-430.
Lin,J.W.,Zhan,Y.H.,Wang,H.,Chu,M.,Wang,C.F.,He,Y.,et al.,2017b.Effect of calcium ion on phosphate adsorption onto hydrous zirconium oxide.Chem.Eng.J.309,118-129.
Liu,X.,Zhang,L.F.,2015.Removal of phosphate anions using the modified chitosan beads:adsorption kinetic,isotherm and mechanism studies.Powder Technol.277,112-119.
Liu,H.L.,Sun,X.F.,Yin,C.Q.,Hu,C.,2008.Removal of phosphate by mesoporous ZrO2.J.Hazard.Mater.151,616-622.
Lu,H.T.,Zhu,Z.L.,Zhang,H.,Zhu,J.Y.,Qiu,Y.L.,2015.Simultaneous removal of arsenate and antimonate in simulated and practical water samples by adsorption onto Zn/Fe layered double hydroxide.Chem.Eng.J.276,365-375.
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Luo,X.G.,Liu,C.,Yuan,J.,Zhu,X.R.,Liu,S.L.,2017b.Interfacial solid-phase chemical modification with mannich reaction and Fe(III)chelation for designing lignin-based spherical nanoparticle adsorbents for highly efficient removal of low concentration phosphate from water.ACS Sustain.Chem.Eng.5,6539-6547.
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Pan,X.L.,Wang,J.L.,Zhang,D.Y.,2009.Sorption of cobalt to bone char:kinetics,competitive sorption and mechanism.Desalination 249,609-614.
Pan,S.L.,Li,J.S.,Wan,G.J.,Liu,C.,Fan,W.H.,Wang,L.J.,2016.Nanosized yolk-shell Fe3O4@Zr(OH)xspheres for efficient removal of Pb(II)from aqueous solution.J.Hazard.Mater.309,1-9.
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Chitrakar,R.,Tezuka,S.,Sonoda,A.,Sakane,K.,Ooi,K.,Hirotsu,T.,2006.Selective adsorption of phosphate from seawater and wastewater by amorphous zirconium hydroxide.J.Colloid Interface Sci.297,426-433.
D'Arcy,M.,Weiss,D.,Bluck,M.,Vilar,R.,2011.Adsorption kinetics,capacity and mechanism of arsenate and phosphate on a bifunctional TiO2-Fe2O3bi-composite.J.Colloid Interface Sci.364,205-212.
Dou,X.M.,Mohan,D.,Pittman Jr.,C.U.,Yang,S.,2012.Remediating fluoride from water using hydrous zirconium oxide.Chem.Eng.J.198-199,236-245.
Du,X.L.,Han,Q.,Li,J.Q.,Li,H.Y.,2017.The behavior of phosphate adsorption and its reactions on the surfaces of Fe-Mn oxide adsorbent.J.Taiwan Inst.Chem.Eng.76,167-175.
Fang,L.P.,Wu,B.L.,Lo,I.M.C.,2017.Fabrication of silica-free superparamagnetic ZrO2@Fe3O4with enhanced phosphate recovery from sewage:performance and adsorption mechanism.Chem.Eng.J.319,258-267.
Freundlich,H.,1926.Colloid and Capillary Chemistry.Methuen,London.
Fu,D.D.,He,Z.Q.,Su,S.S.,Xu,B.,Liu,Y.L.,Zhao,Y.P.,2017.Fabrication ofα-FeOOH decorated graphene oxide-carbon nanotubes aerogel and its application in adsorption of arsenic species.J.Colloid Interface Sci.505,105-114.
Ho,Y.S.,McKay,G.,1999.Pseudo-second order model for sorption processes.Process Biochem.34,451-465.
Hu,P.,Liu,Q.,Wang,J.,Huang,R.H.,2017.Phosphate removal by Ce(III)-impregnated crosslinked chitosan complex from aqueous solutions.Polym.Eng.Sci.57,44-51.
Huang,W.Y.,Zhang,Y.M.,Li,D.,2017.Adsorptive removal of phosphate from water using mesoporous materials:a review.J.Environ.Manag.193,470-482.
Hunger,S.,Cho,H.,Sims,J.T.,Sparks,D.L.,2004.Direct speciation of phosphorus in alum-amended poultry litter:solid-state31PNMR investigation.Environ.Sci.Technol.38,674-681.
Johir,M.A.H.,Pradhan,M.,Loganathan,P.,Kandasamy,J.,Vigneswaran,S.,2016.Phosphate adsorption from wastewater using zirconium(IV)hydroxide:kinetics,thermodynamics and membrane filtration adsorption hybrid system studies.J.Environ.Manag.167,167-174.
Ju,X.Q.,Hou,J.F.,Tang,Y.Q.,Sun,Y.B.,Zheng,S.R.,Xu,Z.Y.,2016.ZrO2nanoparticles confined in CMK-3 as highly effective sorbent for phosphate adsorption.Microporous Mesoporous Mater.230,188-195.
Kang,S.A.,Li,W.,Lee,H.E.,Phillips,B.L.,Lee,Y.J.,2011.Phosphate uptake by TiO2:batch studies and NMR spectroscopic evidence for multisite adsorption.J.Colloid Interface Sci.364,455-461.
K?iv,M.,Liira,M.,Mander,ü.,M?tlep,R.,Vohla,C.,Kirsim?e,K.,2010.Phosphorus removal using Ca-rich hydrated oil shale ash as filter material-the effect of different phosphorus loadings and wastewater compositions.Water Res.44,5232-5239.
Langmuir,I.,1916.The constitution and fundamental properties of solids and liquids Part I.Solid.J.Am.Chem.Soc.38,2221-2295.
Lee,S.H.,Yoo,B.H.,Kim,S.K.,Lim,S.J.,Kim,J.Y.,Kim,T.H.,2013.Enhancement of struvite purity by re-dissolution of calcium ions in synthetic wastewaters.J.Hazard.Mater.261,29-37.
Li,W.,Feng,X.H.,Yan,Y.P.,Sparks,D.L.,Phillips,B.L.,2013a.Solid-state NMR spectroscopic study of phosphate sorption mechanisms on aluminum(hydr)oxides.Environ.Sci.Technol.47,8308-8315.
Li,W.,Pierre-Louis,A.M.,Kwon,K.D.,Kubicki,J.D.,Strongin,D.R.,Phillips,B.L.,2013b.Molecular level investigations of phosphate sorption on corundum(α-Al2O3)by31P solid state NMR,ATR-FTIRand quantum chemical calculation.Geochim.Cosmochim.Acta107,252-266.
Li,R.H.,Wang,J.J.,Zhou,B.Y.,Awasthi,M.K.,Ali,A.,Zhang,Z.Q.,et al.,2016a.Enhancing phosphate adsorption by Mg/Al layered double hydroxide functionalized biochar with different Mg/Al ratios.Sci.Total Environ.559,121-129.
Li,X.,Zhang,Y.,Jing,L.,He,X.,2016b.Novel N-doped CNTs stabilized Cu2O nanoparticles as adsorbent for enhancing removal of Malachite Green and tetrabromobisphenol A.Chem.Eng.J.292,326-339.
Lin,B.,Hua,M.,Zhang,Y.Y.,Zhang,W.M.,Lv,L.,Pan,B.C.,2017a.Effects of organic acids of different molecular size on phosphate removal by HZO-201 nanocomposite.Chemosphere166,422-430.
Lin,J.W.,Zhan,Y.H.,Wang,H.,Chu,M.,Wang,C.F.,He,Y.,et al.,2017b.Effect of calcium ion on phosphate adsorption onto hydrous zirconium oxide.Chem.Eng.J.309,118-129.
Liu,X.,Zhang,L.F.,2015.Removal of phosphate anions using the modified chitosan beads:adsorption kinetic,isotherm and mechanism studies.Powder Technol.277,112-119.
Liu,H.L.,Sun,X.F.,Yin,C.Q.,Hu,C.,2008.Removal of phosphate by mesoporous ZrO2.J.Hazard.Mater.151,616-622.
Lu,H.T.,Zhu,Z.L.,Zhang,H.,Zhu,J.Y.,Qiu,Y.L.,2015.Simultaneous removal of arsenate and antimonate in simulated and practical water samples by adsorption onto Zn/Fe layered double hydroxide.Chem.Eng.J.276,365-375.
Luo,X.B.,Wu,X.,Reng,Z.,Min,X.Y.,Xiao,X.,Luo,J.M.,2017a.Enhancement of phosphate adsorption on zirconium hydroxide by ammonium modification.Ind.Eng.Chem.Res.56,9419-9428.
Luo,X.G.,Liu,C.,Yuan,J.,Zhu,X.R.,Liu,S.L.,2017b.Interfacial solid-phase chemical modification with mannich reaction and Fe(III)chelation for designing lignin-based spherical nanoparticle adsorbents for highly efficient removal of low concentration phosphate from water.ACS Sustain.Chem.Eng.5,6539-6547.
Lürling,M.,Waajen,G.,van Oosterhout,F.,2014.Humic substances interfere with phosphate removal by lanthanum modified clay in controlling eutrophication.Water Res.54,78-88.
Ma,Y.X.,Xing,D.,Shao,W.J.,Du,X.Y.,La,P.Q.,2017.Preparation of polyamidoamine dendrimers functionalized magnetic graphene oxide for the adsorption of Hg(II)in aqueous solution.J.Colloid Interface Sci.505,352-363.
Martins,L.R.,Rodrigues,J.A.V.,Adarme,O.F.H.,Melo,T.M.S.,Gurgel,L.V.A.,Gil,L.F.,2017.Optimization of cellulose and sugarcane bagasse oxidation:application for adsorptive removal of crystal violet and auramine-O from aqueous solution.J.Colloid Interface Sci.494,223-241.
Pan,X.L.,Wang,J.L.,Zhang,D.Y.,2009.Sorption of cobalt to bone char:kinetics,competitive sorption and mechanism.Desalination 249,609-614.
Pan,S.L.,Li,J.S.,Wan,G.J.,Liu,C.,Fan,W.H.,Wang,L.J.,2016.Nanosized yolk-shell Fe3O4@Zr(OH)xspheres for efficient removal of Pb(II)from aqueous solution.J.Hazard.Mater.309,1-9.
Pawar,R.R.,Gupta,P.,Lalhmunsiama,Bajaj,H.C.,Lee,S.M.,2016.Al-intercalated acid activated bentonite beads for the removal of aqueous phosphate.Sci.Total Environ.572,1222-1230.
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