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Phosphate Polymer Nanogel for Selective and Efficient Rare Earth Element Recovery
Demand for rare earth elements (REEs) is increasing, and REE production from ores is energy-intensive. Recovering REEs from waste streams can provide a more sustainable approach to help meet REE demand but requires materials with high selectivity and capacity for REEs due to the low concentration of...
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Published in: | Environmental science & technology 2021-09, Vol.55 (18), p.12549-12560 |
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creator | Zhang, Yilin Yan, Jiajun Xu, Jiang Tian, Chong Matyjaszewski, Krzysztof Tilton, Robert D Lowry, Gregory V |
description | Demand for rare earth elements (REEs) is increasing, and REE production from ores is energy-intensive. Recovering REEs from waste streams can provide a more sustainable approach to help meet REE demand but requires materials with high selectivity and capacity for REEs due to the low concentration of REEs and high competing ion concentrations. Here, we developed a phosphate polymer nanogel (PPN) to selectively recover REEs from low REE content waste streams, including leached fly ash. A high phosphorus content (16.2 wt % P as phosphate groups) in the PPN provides an abundance of coordination sites for REE binding. In model solutions, the distribution coefficient (K d) for all REEs ranged from 1.3 × 105 to 3.1 × 105 mL g–1 at pH = 7, and the sorption capacity (q m) for Nd, Gd, and Ho were ∼300 mg g–1. The PPN was selective toward REEs, outcompeting cations (Ca, Mg, Fe, Al) at up to 1000-fold excess concentration. The PPN had a K d of ∼105–106 mL g–1 for lanthanides in coal fly ash leachate (pH = 5), orders of magnitude higher than the K d of major competing ions (∼103–104 mL g–1). REEs were recovered from the PPN using 3.5% HNO3, and the material remained effective over three sorption–elution cycles. The high REE capacity and selectivity and good durability in a real waste stream matrix suggest its potential to recover REEs from a broad range of secondary REE stocks. |
doi_str_mv | 10.1021/acs.est.1c01877 |
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Recovering REEs from waste streams can provide a more sustainable approach to help meet REE demand but requires materials with high selectivity and capacity for REEs due to the low concentration of REEs and high competing ion concentrations. Here, we developed a phosphate polymer nanogel (PPN) to selectively recover REEs from low REE content waste streams, including leached fly ash. A high phosphorus content (16.2 wt % P as phosphate groups) in the PPN provides an abundance of coordination sites for REE binding. In model solutions, the distribution coefficient (K d) for all REEs ranged from 1.3 × 105 to 3.1 × 105 mL g–1 at pH = 7, and the sorption capacity (q m) for Nd, Gd, and Ho were ∼300 mg g–1. The PPN was selective toward REEs, outcompeting cations (Ca, Mg, Fe, Al) at up to 1000-fold excess concentration. The PPN had a K d of ∼105–106 mL g–1 for lanthanides in coal fly ash leachate (pH = 5), orders of magnitude higher than the K d of major competing ions (∼103–104 mL g–1). REEs were recovered from the PPN using 3.5% HNO3, and the material remained effective over three sorption–elution cycles. The high REE capacity and selectivity and good durability in a real waste stream matrix suggest its potential to recover REEs from a broad range of secondary REE stocks.</description><identifier>ISSN: 0013-936X</identifier><identifier>EISSN: 1520-5851</identifier><identifier>DOI: 10.1021/acs.est.1c01877</identifier><language>eng</language><publisher>Easton: American Chemical Society</publisher><subject>Aluminum ; Cations ; Durability ; Fly ash ; Gadolinium ; Iron ; Lanthanides ; Leachates ; Magnesium ; Materials selection ; pH effects ; Phosphorus ; Polymers ; Rare earth elements ; Selectivity ; Sorption ; Treatment and Resource Recovery ; Waste management ; Waste streams</subject><ispartof>Environmental science & technology, 2021-09, Vol.55 (18), p.12549-12560</ispartof><rights>2021 American Chemical Society</rights><rights>Copyright American Chemical Society Sep 21, 2021</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a338t-b850f74e624d646d79c6584c0cf2e797780c115d9a354464caa6940a05e4914b3</citedby><cites>FETCH-LOGICAL-a338t-b850f74e624d646d79c6584c0cf2e797780c115d9a354464caa6940a05e4914b3</cites><orcidid>0000-0001-8599-008X ; 0000-0003-1960-3402 ; 0000-0003-3286-3268 ; 0000-0003-0369-4848 ; 0000-0002-6535-9415 ; 0000-0003-4246-3620</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids></links><search><creatorcontrib>Zhang, Yilin</creatorcontrib><creatorcontrib>Yan, Jiajun</creatorcontrib><creatorcontrib>Xu, Jiang</creatorcontrib><creatorcontrib>Tian, Chong</creatorcontrib><creatorcontrib>Matyjaszewski, Krzysztof</creatorcontrib><creatorcontrib>Tilton, Robert D</creatorcontrib><creatorcontrib>Lowry, Gregory V</creatorcontrib><title>Phosphate Polymer Nanogel for Selective and Efficient Rare Earth Element Recovery</title><title>Environmental science & technology</title><addtitle>Environ. Sci. Technol</addtitle><description>Demand for rare earth elements (REEs) is increasing, and REE production from ores is energy-intensive. Recovering REEs from waste streams can provide a more sustainable approach to help meet REE demand but requires materials with high selectivity and capacity for REEs due to the low concentration of REEs and high competing ion concentrations. Here, we developed a phosphate polymer nanogel (PPN) to selectively recover REEs from low REE content waste streams, including leached fly ash. A high phosphorus content (16.2 wt % P as phosphate groups) in the PPN provides an abundance of coordination sites for REE binding. In model solutions, the distribution coefficient (K d) for all REEs ranged from 1.3 × 105 to 3.1 × 105 mL g–1 at pH = 7, and the sorption capacity (q m) for Nd, Gd, and Ho were ∼300 mg g–1. The PPN was selective toward REEs, outcompeting cations (Ca, Mg, Fe, Al) at up to 1000-fold excess concentration. The PPN had a K d of ∼105–106 mL g–1 for lanthanides in coal fly ash leachate (pH = 5), orders of magnitude higher than the K d of major competing ions (∼103–104 mL g–1). REEs were recovered from the PPN using 3.5% HNO3, and the material remained effective over three sorption–elution cycles. The high REE capacity and selectivity and good durability in a real waste stream matrix suggest its potential to recover REEs from a broad range of secondary REE stocks.</description><subject>Aluminum</subject><subject>Cations</subject><subject>Durability</subject><subject>Fly ash</subject><subject>Gadolinium</subject><subject>Iron</subject><subject>Lanthanides</subject><subject>Leachates</subject><subject>Magnesium</subject><subject>Materials selection</subject><subject>pH effects</subject><subject>Phosphorus</subject><subject>Polymers</subject><subject>Rare earth elements</subject><subject>Selectivity</subject><subject>Sorption</subject><subject>Treatment and Resource Recovery</subject><subject>Waste management</subject><subject>Waste streams</subject><issn>0013-936X</issn><issn>1520-5851</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp1kMtLw0AQxhdRsFbPXhe8CJI6m30lRyn1AUXrC7yF7WZiU5Js3U0L_e9NbPEgeBqY-X3fzHyEnDMYMYjZtbFhhKEdMQss0fqADJiMIZKJZIdkAMB4lHL1cUxOQlgCQMwhGZDn2cKF1cK0SGeu2tbo6aNp3CdWtHCevmKFti03SE2T00lRlLbEpqUvxiOdGN8u6KTC-qeF1m3Qb0_JUWGqgGf7OiTvt5O38X00fbp7GN9MI8N50kbzREKhBapY5EqoXKdWyURYsEWMOtU6AcuYzFPDpRBKWGNUKsCARJEyMedDcrnzXXn3te4-z-oyWKwq06BbhyyWKoklE5x16MUfdOnWvumu6yjdrVKc9dT1jrLeheCxyFa-rI3fZgyyPuKsizjr1fuIO8XVTtEPfi3_o78BDil9HQ</recordid><startdate>20210921</startdate><enddate>20210921</enddate><creator>Zhang, Yilin</creator><creator>Yan, Jiajun</creator><creator>Xu, Jiang</creator><creator>Tian, Chong</creator><creator>Matyjaszewski, Krzysztof</creator><creator>Tilton, Robert D</creator><creator>Lowry, Gregory V</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7QO</scope><scope>7ST</scope><scope>7T7</scope><scope>7U7</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>P64</scope><scope>SOI</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0001-8599-008X</orcidid><orcidid>https://orcid.org/0000-0003-1960-3402</orcidid><orcidid>https://orcid.org/0000-0003-3286-3268</orcidid><orcidid>https://orcid.org/0000-0003-0369-4848</orcidid><orcidid>https://orcid.org/0000-0002-6535-9415</orcidid><orcidid>https://orcid.org/0000-0003-4246-3620</orcidid></search><sort><creationdate>20210921</creationdate><title>Phosphate Polymer Nanogel for Selective and Efficient Rare Earth Element Recovery</title><author>Zhang, Yilin ; Yan, Jiajun ; Xu, Jiang ; Tian, Chong ; Matyjaszewski, Krzysztof ; Tilton, Robert D ; Lowry, Gregory V</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a338t-b850f74e624d646d79c6584c0cf2e797780c115d9a354464caa6940a05e4914b3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Aluminum</topic><topic>Cations</topic><topic>Durability</topic><topic>Fly ash</topic><topic>Gadolinium</topic><topic>Iron</topic><topic>Lanthanides</topic><topic>Leachates</topic><topic>Magnesium</topic><topic>Materials selection</topic><topic>pH effects</topic><topic>Phosphorus</topic><topic>Polymers</topic><topic>Rare earth elements</topic><topic>Selectivity</topic><topic>Sorption</topic><topic>Treatment and Resource Recovery</topic><topic>Waste management</topic><topic>Waste streams</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Yilin</creatorcontrib><creatorcontrib>Yan, Jiajun</creatorcontrib><creatorcontrib>Xu, Jiang</creatorcontrib><creatorcontrib>Tian, Chong</creatorcontrib><creatorcontrib>Matyjaszewski, Krzysztof</creatorcontrib><creatorcontrib>Tilton, Robert D</creatorcontrib><creatorcontrib>Lowry, Gregory V</creatorcontrib><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Environment Abstracts</collection><collection>Industrial and Applied Microbiology Abstracts (Microbiology A)</collection><collection>Toxicology Abstracts</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>Environment Abstracts</collection><collection>MEDLINE - Academic</collection><jtitle>Environmental science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Yilin</au><au>Yan, Jiajun</au><au>Xu, Jiang</au><au>Tian, Chong</au><au>Matyjaszewski, Krzysztof</au><au>Tilton, Robert D</au><au>Lowry, Gregory V</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Phosphate Polymer Nanogel for Selective and Efficient Rare Earth Element Recovery</atitle><jtitle>Environmental science & technology</jtitle><addtitle>Environ. Sci. Technol</addtitle><date>2021-09-21</date><risdate>2021</risdate><volume>55</volume><issue>18</issue><spage>12549</spage><epage>12560</epage><pages>12549-12560</pages><issn>0013-936X</issn><eissn>1520-5851</eissn><abstract>Demand for rare earth elements (REEs) is increasing, and REE production from ores is energy-intensive. Recovering REEs from waste streams can provide a more sustainable approach to help meet REE demand but requires materials with high selectivity and capacity for REEs due to the low concentration of REEs and high competing ion concentrations. Here, we developed a phosphate polymer nanogel (PPN) to selectively recover REEs from low REE content waste streams, including leached fly ash. A high phosphorus content (16.2 wt % P as phosphate groups) in the PPN provides an abundance of coordination sites for REE binding. In model solutions, the distribution coefficient (K d) for all REEs ranged from 1.3 × 105 to 3.1 × 105 mL g–1 at pH = 7, and the sorption capacity (q m) for Nd, Gd, and Ho were ∼300 mg g–1. The PPN was selective toward REEs, outcompeting cations (Ca, Mg, Fe, Al) at up to 1000-fold excess concentration. The PPN had a K d of ∼105–106 mL g–1 for lanthanides in coal fly ash leachate (pH = 5), orders of magnitude higher than the K d of major competing ions (∼103–104 mL g–1). REEs were recovered from the PPN using 3.5% HNO3, and the material remained effective over three sorption–elution cycles. The high REE capacity and selectivity and good durability in a real waste stream matrix suggest its potential to recover REEs from a broad range of secondary REE stocks.</abstract><cop>Easton</cop><pub>American Chemical Society</pub><doi>10.1021/acs.est.1c01877</doi><tpages>12</tpages><orcidid>https://orcid.org/0000-0001-8599-008X</orcidid><orcidid>https://orcid.org/0000-0003-1960-3402</orcidid><orcidid>https://orcid.org/0000-0003-3286-3268</orcidid><orcidid>https://orcid.org/0000-0003-0369-4848</orcidid><orcidid>https://orcid.org/0000-0002-6535-9415</orcidid><orcidid>https://orcid.org/0000-0003-4246-3620</orcidid></addata></record> |
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subjects | Aluminum Cations Durability Fly ash Gadolinium Iron Lanthanides Leachates Magnesium Materials selection pH effects Phosphorus Polymers Rare earth elements Selectivity Sorption Treatment and Resource Recovery Waste management Waste streams |
title | Phosphate Polymer Nanogel for Selective and Efficient Rare Earth Element Recovery |
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