Lanthanide-alkali double sulfate precipitation from strong sulfuric acid NiMH battery waste leachate

Antti Porvali; Benjamin P. Wilson; Mari Lundström

doi:10.1016/j.wasman.2017.10.031

Lanthanide-alkali double sulfate precipitation from strong sulfuric acid NiMH battery waste leachate

Antti Porvali
, Benjamin P. Wilson
, Mari Lundström^*

^*Corresponding author for this work

Not published at VTT

Aalto University

Research output: Contribution to journal › Article › Scientific › peer-review

77 Citations (Scopus)

Abstract

In NiMH battery leaching, rare earth element (REE) precipitation from sulfate media is often reported as being a result of increasing pH of the pregnant leach solution (PLS). Here we demonstrate that this precipitation is a phenomenon that depends on both Na⁺ and SO₄ ²⁻ concentrations and not solely on pH. A two-stage leaching for industrially crushed NiMH waste is performed: The first stage consists of H₂SO₄ leaching (2 M H₂SO₄, L/S = 10.4, V = 104 ml, T = 30 °C) and the second stage of H₂O leaching (V = 100 ml, T = 25 °C). Moreover, precipitation experiments are separately performed as a function of added Na₂SO₄ and H₂SO₄. During the precipitation, higher than stoichiometric quantities of Na to REE are utilized and this increase in both precipitation reagent concentrations results in an improved double sulfate precipitation efficiency. The best REE precipitation efficiencies (98–99%) – achieved by increasing concentrations of H₂SO₄ and Na₂SO₄ by 1.59 M and 0.35 M, respectively – results in a 21.8 times Na (as Na₂SO₄) and 58.3 times SO₄ change in stoichiometric ratio to REE. Results strongly indicate a straightforward approach for REE recovery from NiMH battery waste without the need to increase the pH of PLS.

Original language	English
Pages (from-to)	381-389
Number of pages	9
Journal	Waste Management
Volume	71
DOIs	https://doi.org/10.1016/j.wasman.2017.10.031
Publication status	Published - Jan 2018
MoE publication type	A1 Journal article-refereed

Funding

The authors acknowledge METYK project for providing the context where the work was performed. METYK project was financially supported by TEKES, EU, Vipuvoimaa EU:lta 2014-2020, Norilsk Nickel, CrisolteQ, Akkuser, Kuusakoski, Jyväskylän Energia, Luvata, Boliden Harjavalta and municipalities of Pori and Harjavalta. This work has also been supported by the Strategic Research Council at the Academy of Finland , project CloseLoop (grant number 303454 ), NoWASTE (grant number 297962), MineWEEE ( 7100/31/2016 ) and made use of the RawMatTERS Finland Infrastructure (RAMI) based at Aalto University. The authors would like to thank Petteri Halli for operating the SEM-EDS.

Keywords

Double sulfate
Hydrometallurgy
Nickel metal hydride battery
Rare earths
Recycling
Alkalies
Sulfuric Acids/chemistry
Lanthanoid Series Elements/chemistry
Nickel
Sulfates
Electronic Waste

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10.1016/j.wasman.2017.10.031

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@article{ac4d5c9251b841c7b5da60df98491924,

title = "Lanthanide-alkali double sulfate precipitation from strong sulfuric acid NiMH battery waste leachate",

abstract = "In NiMH battery leaching, rare earth element (REE) precipitation from sulfate media is often reported as being a result of increasing pH of the pregnant leach solution (PLS). Here we demonstrate that this precipitation is a phenomenon that depends on both Na+ and SO4 2− concentrations and not solely on pH. A two-stage leaching for industrially crushed NiMH waste is performed: The first stage consists of H2SO4 leaching (2 M H2SO4, L/S = 10.4, V = 104 ml, T = 30 °C) and the second stage of H2O leaching (V = 100 ml, T = 25 °C). Moreover, precipitation experiments are separately performed as a function of added Na2SO4 and H2SO4. During the precipitation, higher than stoichiometric quantities of Na to REE are utilized and this increase in both precipitation reagent concentrations results in an improved double sulfate precipitation efficiency. The best REE precipitation efficiencies (98–99\%) – achieved by increasing concentrations of H2SO4 and Na2SO4 by 1.59 M and 0.35 M, respectively – results in a 21.8 times Na (as Na2SO4) and 58.3 times SO4 change in stoichiometric ratio to REE. Results strongly indicate a straightforward approach for REE recovery from NiMH battery waste without the need to increase the pH of PLS.",

keywords = "Double sulfate, Hydrometallurgy, Nickel metal hydride battery, Rare earths, Recycling, Alkalies, Sulfuric Acids/chemistry, Lanthanoid Series Elements/chemistry, Nickel, Sulfates, Electronic Waste",

author = "Antti Porvali and Wilson, \{Benjamin P.\} and Mari Lundstr{\"o}m",

note = "Funding Information: The authors acknowledge METYK project for providing the context where the work was performed. METYK project was financially supported by TEKES, EU, Vipuvoimaa EU:lta 2014-2020, Norilsk Nickel, CrisolteQ, Akkuser, Kuusakoski, Jyv?skyl?n Energia, Luvata, Boliden Harjavalta and municipalities of Pori and Harjavalta. This work has also been supported by the Strategic Research Council at the Academy of Finland, project CloseLoop (grant number 303454), NoWASTE (grant number 297962), MineWEEE (7100/31/2016) and made use of the RawMatTERS Finland Infrastructure (RAMI) based at Aalto University. The authors would like to thank Petteri Halli for operating the SEM-EDS. Funding Information: The authors acknowledge METYK project for providing the context where the work was performed. METYK project was financially supported by TEKES, EU, Vipuvoimaa EU:lta 2014-2020, Norilsk Nickel, CrisolteQ, Akkuser, Kuusakoski, Jyv{\"a}skyl{\"a}n Energia, Luvata, Boliden Harjavalta and municipalities of Pori and Harjavalta. This work has also been supported by the Strategic Research Council at the Academy of Finland , project CloseLoop (grant number 303454 ), NoWASTE (grant number 297962), MineWEEE ( 7100/31/2016 ) and made use of the RawMatTERS Finland Infrastructure (RAMI) based at Aalto University. The authors would like to thank Petteri Halli for operating the SEM-EDS. Publisher Copyright: {\textcopyright} 2017 The Authors Copyright: Copyright 2018 Elsevier B.V., All rights reserved.",

year = "2018",

month = jan,

doi = "10.1016/j.wasman.2017.10.031",

language = "English",

volume = "71",

pages = "381--389",

journal = "Waste Management",

issn = "0956-053X",

publisher = "Elsevier",

}

TY - JOUR

T1 - Lanthanide-alkali double sulfate precipitation from strong sulfuric acid NiMH battery waste leachate

AU - Porvali, Antti

AU - Wilson, Benjamin P.

AU - Lundström, Mari

N1 - Funding Information: The authors acknowledge METYK project for providing the context where the work was performed. METYK project was financially supported by TEKES, EU, Vipuvoimaa EU:lta 2014-2020, Norilsk Nickel, CrisolteQ, Akkuser, Kuusakoski, Jyv?skyl?n Energia, Luvata, Boliden Harjavalta and municipalities of Pori and Harjavalta. This work has also been supported by the Strategic Research Council at the Academy of Finland, project CloseLoop (grant number 303454), NoWASTE (grant number 297962), MineWEEE (7100/31/2016) and made use of the RawMatTERS Finland Infrastructure (RAMI) based at Aalto University. The authors would like to thank Petteri Halli for operating the SEM-EDS. Funding Information: The authors acknowledge METYK project for providing the context where the work was performed. METYK project was financially supported by TEKES, EU, Vipuvoimaa EU:lta 2014-2020, Norilsk Nickel, CrisolteQ, Akkuser, Kuusakoski, Jyväskylän Energia, Luvata, Boliden Harjavalta and municipalities of Pori and Harjavalta. This work has also been supported by the Strategic Research Council at the Academy of Finland , project CloseLoop (grant number 303454 ), NoWASTE (grant number 297962), MineWEEE ( 7100/31/2016 ) and made use of the RawMatTERS Finland Infrastructure (RAMI) based at Aalto University. The authors would like to thank Petteri Halli for operating the SEM-EDS. Publisher Copyright: © 2017 The Authors Copyright: Copyright 2018 Elsevier B.V., All rights reserved.

PY - 2018/1

Y1 - 2018/1

N2 - In NiMH battery leaching, rare earth element (REE) precipitation from sulfate media is often reported as being a result of increasing pH of the pregnant leach solution (PLS). Here we demonstrate that this precipitation is a phenomenon that depends on both Na+ and SO4 2− concentrations and not solely on pH. A two-stage leaching for industrially crushed NiMH waste is performed: The first stage consists of H2SO4 leaching (2 M H2SO4, L/S = 10.4, V = 104 ml, T = 30 °C) and the second stage of H2O leaching (V = 100 ml, T = 25 °C). Moreover, precipitation experiments are separately performed as a function of added Na2SO4 and H2SO4. During the precipitation, higher than stoichiometric quantities of Na to REE are utilized and this increase in both precipitation reagent concentrations results in an improved double sulfate precipitation efficiency. The best REE precipitation efficiencies (98–99%) – achieved by increasing concentrations of H2SO4 and Na2SO4 by 1.59 M and 0.35 M, respectively – results in a 21.8 times Na (as Na2SO4) and 58.3 times SO4 change in stoichiometric ratio to REE. Results strongly indicate a straightforward approach for REE recovery from NiMH battery waste without the need to increase the pH of PLS.

AB - In NiMH battery leaching, rare earth element (REE) precipitation from sulfate media is often reported as being a result of increasing pH of the pregnant leach solution (PLS). Here we demonstrate that this precipitation is a phenomenon that depends on both Na+ and SO4 2− concentrations and not solely on pH. A two-stage leaching for industrially crushed NiMH waste is performed: The first stage consists of H2SO4 leaching (2 M H2SO4, L/S = 10.4, V = 104 ml, T = 30 °C) and the second stage of H2O leaching (V = 100 ml, T = 25 °C). Moreover, precipitation experiments are separately performed as a function of added Na2SO4 and H2SO4. During the precipitation, higher than stoichiometric quantities of Na to REE are utilized and this increase in both precipitation reagent concentrations results in an improved double sulfate precipitation efficiency. The best REE precipitation efficiencies (98–99%) – achieved by increasing concentrations of H2SO4 and Na2SO4 by 1.59 M and 0.35 M, respectively – results in a 21.8 times Na (as Na2SO4) and 58.3 times SO4 change in stoichiometric ratio to REE. Results strongly indicate a straightforward approach for REE recovery from NiMH battery waste without the need to increase the pH of PLS.

KW - Double sulfate

KW - Hydrometallurgy

KW - Nickel metal hydride battery

KW - Rare earths

KW - Recycling

KW - Alkalies

KW - Sulfuric Acids/chemistry

KW - Lanthanoid Series Elements/chemistry

KW - Nickel

KW - Sulfates

KW - Electronic Waste

UR - https://www.scopus.com/pages/publications/85032205354

U2 - 10.1016/j.wasman.2017.10.031

DO - 10.1016/j.wasman.2017.10.031

M3 - Article

C2 - 29110941

AN - SCOPUS:85032205354

SN - 0956-053X

VL - 71

SP - 381

EP - 389

JO - Waste Management

JF - Waste Management

ER -

Lanthanide-alkali double sulfate precipitation from strong sulfuric acid NiMH battery waste leachate

Abstract

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Keywords

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