Silver recovery as Ag~0 nanoparticles from ion-exchange regenerant solution using electrolysis
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摘要
Many silver(Ag)containing consumer-products(e.g.textiles)release Ag into the environment,posing ecotoxicological risks.Ag recovery mitigates environmental hazards,recycles Ag,and leads to sustainability.In the present work,Ag has been recovered as Ag~0nanoparticles from the spent solution(thiourea(TU)～0.5 mol/L pH～1.1–1.2,and Ag～550 mg/L)obtained from the regeneration of an Ag-loaded resin using a simple undivided electrolytic cell.The reclaimed regenerant solution has been recycled and reused in a closed-loop scheme over multiple cycles.The process parameters,i.e.,current(0.05 A)and stirring speed(600 r/min),have been optimized for Ag recovery of～94%and TU loss of～2%.The reclaimed regenerant solution has been shown to regenerate Ag-loaded resin samples with>90%regeneration efficiency over 4 cycles of consecutive extraction and regeneration.The recovered Ag~0nanoparticles are monodisperse,consistently spherical in shape,and have a mean diameter of～6 nm with standard deviation of the Gaussian fit as～2.66 nm.
Many silver(Ag)containing consumer-products(e.g.textiles)release Ag into the environment,posing ecotoxicological risks.Ag recovery mitigates environmental hazards,recycles Ag,and leads to sustainability.In the present work,Ag has been recovered as Ag~0nanoparticles from the spent solution(thiourea(TU)～0.5 mol/L pH～1.1–1.2,and Ag～550 mg/L)obtained from the regeneration of an Ag-loaded resin using a simple undivided electrolytic cell.The reclaimed regenerant solution has been recycled and reused in a closed-loop scheme over multiple cycles.The process parameters,i.e.,current(0.05 A)and stirring speed(600 r/min),have been optimized for Ag recovery of～94%and TU loss of～2%.The reclaimed regenerant solution has been shown to regenerate Ag-loaded resin samples with>90%regeneration efficiency over 4 cycles of consecutive extraction and regeneration.The recovered Ag~0nanoparticles are monodisperse,consistently spherical in shape,and have a mean diameter of～6 nm with standard deviation of the Gaussian fit as～2.66 nm.
Many silver(Ag)containing consumer-products(e.g.textiles)release Ag into the environment,posing ecotoxicological risks.Ag recovery mitigates environmental hazards,recycles Ag,and leads to sustainability.In the present work,Ag has been recovered as Ag~0nanoparticles from the spent solution(thiourea(TU)～0.5 mol/L pH～1.1–1.2,and Ag～550 mg/L)obtained from the regeneration of an Ag-loaded resin using a simple undivided electrolytic cell.The reclaimed regenerant solution has been recycled and reused in a closed-loop scheme over multiple cycles.The process parameters,i.e.,current(0.05 A)and stirring speed(600 r/min),have been optimized for Ag recovery of～94%and TU loss of～2%.The reclaimed regenerant solution has been shown to regenerate Ag-loaded resin samples with>90%regeneration efficiency over 4 cycles of consecutive extraction and regeneration.The recovered Ag~0nanoparticles are monodisperse,consistently spherical in shape,and have a mean diameter of～6 nm with standard deviation of the Gaussian fit as～2.66 nm.
引文
Absalan,G.,Mehrdjardi,M.A.,2003.Separation and preconcentration of silver ion using 2-mercaptobenzothiazole immobilized on surfactant-coated alumina.Sep.Purif.Technol.33(1),95-101.
Ahamed,M.,Alsalhi,M.S.,Siddiqui,M.K.J.,2010.Silver nanoparticle applications and human health.Clin.Chim.Acta 411(23),1841-1848.
Balá?,P.,Ficeriová,J.,Leon,C.V.,2003.Silver leaching from a mechanochemically pretreated complex sulfide concentrate.Hydrometallurgy 70(1),113-119.
Benn,T.M.,Westerhoff,P.,2008.Nanoparticle silver released into water from commercially available sock fabrics.Environ.Sci.Technol 42(11),4133-4139.
Brownson,D.A.C.,Banks,C.E.,2014.Interpreting Electrochemistry.The Handbook of Graphene Electrochemistry.Springer,London,pp.23-77.
Caswell,K.K.,Bender,C.M.,Murphy,C.J.,2003.Seedless,surfactantless wet chemical synthesis of silver nanowires.Nano Lett.3(5),667-669.
Díaz,M.E.P.,Alonso,A.R.,González,I.,Lapidus,G.T.,2012.Influence of oxygen reduction and hydrogen evolution in the gold and silver direct electrodeposition process from thiourea solutions in a filter press type reactor.Hydrometallurgy 129,90-96.
Gagné,F.,André,C.,Skirrow,R.,Gélinas,M.,Auclair,J.,Van Aggelen,G.,et al.,2012.Toxicity of silver nanoparticles to rainbow trout:a toxicogenomic approach.Chemosphere 89(5),615-622.
Geranio,L.,Heuberger,M.,Nowack,B.,2009.The behavior of silver nanotextiles during washing.Environ.Sci.Technol.43(21),8113-8118.
GFMS World Silver Survey,2017.The Silver Institute.Available:.http://www.silverinstitute.org/site/WSS2017.pdf,Accessed date:17 November 2017.
Gherrou,A.,Kerdjoudj,H.,Molinari,R.,Drioli,E.,2001.Modelization of the transport of silver and copper in acidic thiourea medium through a supported liquid membrane.Desalination 139(1-3),317-325.
Gurung,M.,Adhikari,B.B.,Kawakita,H.,Ohto,K.,Inoue,K.,Alam,S.,2013.Recovery of gold and silver from spent mobile phones by means of acidothiourea leaching followed by adsorption using biosorbent prepared from persimmon tannin.Hydrometallurgy 133,84-93.
Lorenz,C.,Windler,L.,Von Goetz,N.,Lehmann,R.P.,Schuppler,M.,Hungerbühler,K.,et al.,2012.Characterization of silver release from commercially available functional(nano)textiles.Chemosphere 89(7),817-824.
Ma,H.,Yin,B.,Wang,S.,Jiao,Y.,Pan,W.,Huang,S.,et al.,2004.Synthesis of silver and gold nanoparticles by a novel electrochemical method.ChemPhysChem 5(1),68-75.
Mitrano,D.M.,Arroyo Rojas Dasilva,Y.,Nowack,B.,2015.Effect of variations of washing solution chemistry on nanomaterial physicochemical changes in the laundry cycle.Environ.Sci.Technol.49(16),9665-9673.
Moores,A.,Goettmann,F.,2006.The plasmon band in noble metal nanoparticles:an introduction to theory and applications.New J.Chem.30(8),1121-1132.
Morley,N.,Eatherley,D.,2008.Material Security:Ensuring Resource Availability for the UK Economy.C-Tech Innovation Limited,Chester.
Murray,B.J.,Li,Q.,Newberg,J.T.,Menke,E.J.,Hemminger,J.C.,Penner,R.M.,2005.Shape-and size-selective electrochemical synthesis of dispersed silver(I)oxide colloids.Nano Lett.5(11),2319-2324.
Nawaz,T.,Sengupta,S.,2017a.Silver recovery from greywater:Role of competing cations and regeneration.Sep.Purif.Technol.176,145-158.
Nawaz,T.,Sengupta,S.,2017b.Silver recovery from laundry washwater:the role of detergent chemistry.ACS Sustain.Chem.Eng.6(1),600-608.
Pillai,Z.S.,Kamat,P.V.,2004.What factors control the size and shape of silver nanoparticles in the citrate ion reduction method?J.Phys.Chem.B 108(3),945-951.
Poisot-Díaz,M.E.,González,I.,Lapidus,G.T.,2008.Electrodeposition of a silver-gold alloy(DORE)from thiourea solutions in the presence of other metallic ion impurities.Hydrometallurgy 93(1),23-29.
Reents,B.,Plieth,W.,Macagno,V.A.,Lacconi,G.I.,1998.Influence of thiourea on silver deposition:Spectroscopic investigation.J.Electroanal.Chem.453(1),121-127.
Rodriguez-Sanchez,L.,Blanco,M.C.,Lopez-Quintela,M.A.,2000.Electrochemical synthesis of silver nanoparticles.J.Phys.Chem.B 104(41),9683-9688.
Stamplecoskie,K.G.,Scaiano,J.C.,2010.Light emitting diode irradiation can control the morphology and optical properties of silver nanoparticles.J.Am.Chem.Soc.132(6),1825-1827.
Tan,J.M.,Qiu,G.,Ting,Y.P.,2015.Osmotic membrane bioreactor for municipal wastewater treatment and the effects of silver nanoparticles on system performance.J.Clean.Prod.88,146-151.
Teutli,M.,Lapidus,G.,González,I.,1990.The kinetics of silver cementation from thiourea solutions using aluminum.Adv.Gold Silver Proc.249-256.
Turkevich,J.,Stevenson,P.C.,Hillier,J.,1951.A study of the nucleation and growth processes in the synthesis of colloidal gold.Discuss.Faraday Soc.11,55-75.
Vance,M.E.,Kuiken,T.,Vejerano,E.P.,McGinnis,S.P.,Hochella Jr.,M.F.,Rejeski,D.,et al.,2015.Nanotechnology in the real world:Redeveloping the nanomaterial consumer products inventory.Beilstein J.Nanotechnol.6,1769.
Varentsov,V.K.,Varentsova,V.I.,2004.Electrolysis with carbongraphite flow electrodes for solving problems of precious metal extraction from jewellery manufacturing wastes.Chem.Sust.Develop.12,293.
Westerhoff,P.,Lee,S.,Yang,Y.,Gordon,G.W.,Hristovski,K.,Halden,R.U.,et al.,2015.Characterization,recovery opportunities,and valuation of metals in municipal sludges from USwastewater treatment plants nationwide.Environ.Sci.Technol.49(16),9479-9488.
Yan,M.,Liu,K.,Jiang,Z.,1996.Electrochemical oxidation of thiourea studied by use of in situ FTIR spectroscopy.J.Electroanal.Chem.408(1-2),225-229.
Yeo,M.K.,Yoon,J.W.,2009.Comparison of the effects of nanosilver antibacterial coatings and silver ions on zebrafish embryogenesis.Mol.Cell.Toxicol.5(1),23-31.
Yin,B.,Ma,H.,Wang,S.,Chen,S.,2003.Electrochemical synthesis of silver nanoparticles under protection of poly(N-vinylpyrrolidone).J.Phys.Chem.B 107(34),8898-8904.
Zhu,J.,Liu,S.,Palchik,O.,Koltypin,Y.,Gedanken,A.,2000.Shapecontrolled synthesis of silver nanoparticles by pulse sonoelectrochemical methods.Langmuir 16(16),6396-6399.
Ahamed,M.,Alsalhi,M.S.,Siddiqui,M.K.J.,2010.Silver nanoparticle applications and human health.Clin.Chim.Acta 411(23),1841-1848.
Balá?,P.,Ficeriová,J.,Leon,C.V.,2003.Silver leaching from a mechanochemically pretreated complex sulfide concentrate.Hydrometallurgy 70(1),113-119.
Benn,T.M.,Westerhoff,P.,2008.Nanoparticle silver released into water from commercially available sock fabrics.Environ.Sci.Technol 42(11),4133-4139.
Brownson,D.A.C.,Banks,C.E.,2014.Interpreting Electrochemistry.The Handbook of Graphene Electrochemistry.Springer,London,pp.23-77.
Caswell,K.K.,Bender,C.M.,Murphy,C.J.,2003.Seedless,surfactantless wet chemical synthesis of silver nanowires.Nano Lett.3(5),667-669.
Díaz,M.E.P.,Alonso,A.R.,González,I.,Lapidus,G.T.,2012.Influence of oxygen reduction and hydrogen evolution in the gold and silver direct electrodeposition process from thiourea solutions in a filter press type reactor.Hydrometallurgy 129,90-96.
Gagné,F.,André,C.,Skirrow,R.,Gélinas,M.,Auclair,J.,Van Aggelen,G.,et al.,2012.Toxicity of silver nanoparticles to rainbow trout:a toxicogenomic approach.Chemosphere 89(5),615-622.
Geranio,L.,Heuberger,M.,Nowack,B.,2009.The behavior of silver nanotextiles during washing.Environ.Sci.Technol.43(21),8113-8118.
GFMS World Silver Survey,2017.The Silver Institute.Available:.http://www.silverinstitute.org/site/WSS2017.pdf,Accessed date:17 November 2017.
Gherrou,A.,Kerdjoudj,H.,Molinari,R.,Drioli,E.,2001.Modelization of the transport of silver and copper in acidic thiourea medium through a supported liquid membrane.Desalination 139(1-3),317-325.
Gurung,M.,Adhikari,B.B.,Kawakita,H.,Ohto,K.,Inoue,K.,Alam,S.,2013.Recovery of gold and silver from spent mobile phones by means of acidothiourea leaching followed by adsorption using biosorbent prepared from persimmon tannin.Hydrometallurgy 133,84-93.
Lorenz,C.,Windler,L.,Von Goetz,N.,Lehmann,R.P.,Schuppler,M.,Hungerbühler,K.,et al.,2012.Characterization of silver release from commercially available functional(nano)textiles.Chemosphere 89(7),817-824.
Ma,H.,Yin,B.,Wang,S.,Jiao,Y.,Pan,W.,Huang,S.,et al.,2004.Synthesis of silver and gold nanoparticles by a novel electrochemical method.ChemPhysChem 5(1),68-75.
Mitrano,D.M.,Arroyo Rojas Dasilva,Y.,Nowack,B.,2015.Effect of variations of washing solution chemistry on nanomaterial physicochemical changes in the laundry cycle.Environ.Sci.Technol.49(16),9665-9673.
Moores,A.,Goettmann,F.,2006.The plasmon band in noble metal nanoparticles:an introduction to theory and applications.New J.Chem.30(8),1121-1132.
Morley,N.,Eatherley,D.,2008.Material Security:Ensuring Resource Availability for the UK Economy.C-Tech Innovation Limited,Chester.
Murray,B.J.,Li,Q.,Newberg,J.T.,Menke,E.J.,Hemminger,J.C.,Penner,R.M.,2005.Shape-and size-selective electrochemical synthesis of dispersed silver(I)oxide colloids.Nano Lett.5(11),2319-2324.
Nawaz,T.,Sengupta,S.,2017a.Silver recovery from greywater:Role of competing cations and regeneration.Sep.Purif.Technol.176,145-158.
Nawaz,T.,Sengupta,S.,2017b.Silver recovery from laundry washwater:the role of detergent chemistry.ACS Sustain.Chem.Eng.6(1),600-608.
Pillai,Z.S.,Kamat,P.V.,2004.What factors control the size and shape of silver nanoparticles in the citrate ion reduction method?J.Phys.Chem.B 108(3),945-951.
Poisot-Díaz,M.E.,González,I.,Lapidus,G.T.,2008.Electrodeposition of a silver-gold alloy(DORE)from thiourea solutions in the presence of other metallic ion impurities.Hydrometallurgy 93(1),23-29.
Reents,B.,Plieth,W.,Macagno,V.A.,Lacconi,G.I.,1998.Influence of thiourea on silver deposition:Spectroscopic investigation.J.Electroanal.Chem.453(1),121-127.
Rodriguez-Sanchez,L.,Blanco,M.C.,Lopez-Quintela,M.A.,2000.Electrochemical synthesis of silver nanoparticles.J.Phys.Chem.B 104(41),9683-9688.
Stamplecoskie,K.G.,Scaiano,J.C.,2010.Light emitting diode irradiation can control the morphology and optical properties of silver nanoparticles.J.Am.Chem.Soc.132(6),1825-1827.
Tan,J.M.,Qiu,G.,Ting,Y.P.,2015.Osmotic membrane bioreactor for municipal wastewater treatment and the effects of silver nanoparticles on system performance.J.Clean.Prod.88,146-151.
Teutli,M.,Lapidus,G.,González,I.,1990.The kinetics of silver cementation from thiourea solutions using aluminum.Adv.Gold Silver Proc.249-256.
Turkevich,J.,Stevenson,P.C.,Hillier,J.,1951.A study of the nucleation and growth processes in the synthesis of colloidal gold.Discuss.Faraday Soc.11,55-75.
Vance,M.E.,Kuiken,T.,Vejerano,E.P.,McGinnis,S.P.,Hochella Jr.,M.F.,Rejeski,D.,et al.,2015.Nanotechnology in the real world:Redeveloping the nanomaterial consumer products inventory.Beilstein J.Nanotechnol.6,1769.
Varentsov,V.K.,Varentsova,V.I.,2004.Electrolysis with carbongraphite flow electrodes for solving problems of precious metal extraction from jewellery manufacturing wastes.Chem.Sust.Develop.12,293.
Westerhoff,P.,Lee,S.,Yang,Y.,Gordon,G.W.,Hristovski,K.,Halden,R.U.,et al.,2015.Characterization,recovery opportunities,and valuation of metals in municipal sludges from USwastewater treatment plants nationwide.Environ.Sci.Technol.49(16),9479-9488.
Yan,M.,Liu,K.,Jiang,Z.,1996.Electrochemical oxidation of thiourea studied by use of in situ FTIR spectroscopy.J.Electroanal.Chem.408(1-2),225-229.
Yeo,M.K.,Yoon,J.W.,2009.Comparison of the effects of nanosilver antibacterial coatings and silver ions on zebrafish embryogenesis.Mol.Cell.Toxicol.5(1),23-31.
Yin,B.,Ma,H.,Wang,S.,Chen,S.,2003.Electrochemical synthesis of silver nanoparticles under protection of poly(N-vinylpyrrolidone).J.Phys.Chem.B 107(34),8898-8904.
Zhu,J.,Liu,S.,Palchik,O.,Koltypin,Y.,Gedanken,A.,2000.Shapecontrolled synthesis of silver nanoparticles by pulse sonoelectrochemical methods.Langmuir 16(16),6396-6399.