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Room Temperature Electrorefining of Rare Earth Metals from End-of-use Nd-Fe-B Magnets

Recovering rare earth elements (REE) from used permanent magnets, which contains about 30 wt.% of rare earth elements, has been persistent technological challenge. Current recycling methods relies on pyrometallurgical or hydrometallurgical processes which are energy- and chemical- intensive and not economically and environmentally viable for rare earth containing magnets. Enabling efficient and simplistic recovery and refining of REEs contained in End-of-Use (EoU) products, such as Neodymium-Iron-Boron (Nd-Fe-B) based magnets will play an important and complementary role in the total supply of REEs in the future. We designed a new electrochemical method and demonstrated a room temperature one-pot process that concurrently separates and electroplates REE from commercial Nd-Fe-B magnets. By establishing selective oxidation and reductive potential as electrochemical control parameter along with electrochemically compatible non-aqueous electrolyte system, we demonstrated selective electroleaching of lanthanides (Nd and Preseodymium (Pr)) from anode and concurrent plating as alloy at Pt cathode. The morphological and chemical evolution of the Nd-Fe-B magnets during electroleaching reveals the electrochemical stimuli and rate of dissolution depends on microstructural complexities of the Nd-Fe-B magnet. The concomitant electroplating process leads to Nd-Pr based alloy which can be used as raw metallic alloy for manufacturing new permanent magnet and other devices. Our study demonstrates a scalable separation and refining methodology, based on widely available organic electrolyte system and without any consumptive chemical use, for selective lanthanide recovery from waste magnets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Materials Data on PrNd3 by Materials Project

Nd3Pr is Copper-derived structured and crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. there are two inequivalent Nd sites. In the first Nd site, Nd is bonded to eight Nd and four equivalent Pr atoms to form NdPr4Nd8 cuboctahedra that share corners with twelve equivalent NdPr4Nd8 cuboctahedra, edges with eight equivalent PrNd12 cuboctahedra, edges with sixteen NdPr4Nd8 cuboctahedra, faces with four equivalent PrNd12 cuboctahedra, and faces with fourteen NdPr4Nd8 cuboctahedra. There are four shorter (3.68 Å) and four longer (3.69 Å) Nd–Nd bond lengths. All Nd–Pr bond lengths are 3.69 Å. In the second Nd site, Nd is bonded to eight equivalent Nd and four equivalent Pr atoms to form NdPr4Nd8 cuboctahedra that share corners with four equivalent NdPr4Nd8 cuboctahedra, corners with eight equivalent PrNd12 cuboctahedra, edges with twenty-four NdPr4Nd8 cuboctahedra, faces with six equivalent PrNd12 cuboctahedra, and faces with twelve NdPr4Nd8 cuboctahedra. All Nd–Pr bond lengths are 3.68 Å. Pr is bonded to twelve Nd atoms to form PrNd12 cuboctahedra that share corners with four equivalent PrNd12 cuboctahedra, corners with eight equivalent NdPr4Nd8 cuboctahedra, edges with eight equivalent PrNd12 cuboctahedra, edges with sixteen equivalent NdPr4Nd8 cuboctahedra, faces with four equivalent PrNd12 cuboctahedra, and faces with fourteen NdPr4Nd8 cuboctahedra.

36 MATERIALS SCIENCE↗

Materials Data on PrNd by Materials Project

NdPr is Magnesium-derived structured and crystallizes in the hexagonal P-6m2 space group. The structure is three-dimensional. Nd is bonded to six equivalent Nd and six equivalent Pr atoms to form NdPr6Nd6 cuboctahedra that share corners with eighteen equivalent NdPr6Nd6 cuboctahedra, edges with six equivalent NdPr6Nd6 cuboctahedra, edges with twelve equivalent PrPr6Nd6 cuboctahedra, faces with eight equivalent NdPr6Nd6 cuboctahedra, and faces with twelve equivalent PrPr6Nd6 cuboctahedra. All Nd–Nd bond lengths are 3.71 Å. All Nd–Pr bond lengths are 3.73 Å. Pr is bonded to six equivalent Nd and six equivalent Pr atoms to form PrPr6Nd6 cuboctahedra that share corners with eighteen equivalent PrPr6Nd6 cuboctahedra, edges with six equivalent PrPr6Nd6 cuboctahedra, edges with twelve equivalent NdPr6Nd6 cuboctahedra, faces with eight equivalent PrPr6Nd6 cuboctahedra, and faces with twelve equivalent NdPr6Nd6 cuboctahedra. All Pr–Pr bond lengths are 3.71 Å.

36 MATERIALS SCIENCE↗

Materials Data on PrNd by Materials Project

NdPr is alpha Samarium-derived structured and crystallizes in the hexagonal P6_3/mmc space group. The structure is three-dimensional. Nd is bonded to six equivalent Nd and six equivalent Pr atoms to form NdPr6Nd6 cuboctahedra that share corners with twelve equivalent NdPr6Nd6 cuboctahedra, edges with twelve equivalent NdPr6Nd6 cuboctahedra, edges with twelve equivalent PrPr6Nd6 cuboctahedra, faces with six equivalent NdPr6Nd6 cuboctahedra, and faces with twelve equivalent PrPr6Nd6 cuboctahedra. All Nd–Nd bond lengths are 3.71 Å. All Nd–Pr bond lengths are 3.68 Å. Pr is bonded to six equivalent Nd and six equivalent Pr atoms to form PrPr6Nd6 cuboctahedra that share corners with eighteen equivalent PrPr6Nd6 cuboctahedra, edges with six equivalent PrPr6Nd6 cuboctahedra, edges with twelve equivalent NdPr6Nd6 cuboctahedra, faces with eight equivalent PrPr6Nd6 cuboctahedra, and faces with twelve equivalent NdPr6Nd6 cuboctahedra. All Pr–Pr bond lengths are 3.71 Å.

36 MATERIALS SCIENCE↗

Materials Data on Pr3Nd by Materials Project

NdPr3 is Copper-derived structured and crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. Nd is bonded to twelve Pr atoms to form NdPr12 cuboctahedra that share corners with four equivalent NdPr12 cuboctahedra, corners with eight equivalent PrPr8Nd4 cuboctahedra, edges with eight equivalent NdPr12 cuboctahedra, edges with sixteen equivalent PrPr8Nd4 cuboctahedra, faces with four equivalent NdPr12 cuboctahedra, and faces with fourteen PrPr8Nd4 cuboctahedra. All Nd–Pr bond lengths are 3.72 Å. There are two inequivalent Pr sites. In the first Pr site, Pr is bonded to four equivalent Nd and eight Pr atoms to form PrPr8Nd4 cuboctahedra that share corners with twelve equivalent PrPr8Nd4 cuboctahedra, edges with eight equivalent NdPr12 cuboctahedra, edges with sixteen PrPr8Nd4 cuboctahedra, faces with four equivalent NdPr12 cuboctahedra, and faces with fourteen PrPr8Nd4 cuboctahedra. All Pr–Pr bond lengths are 3.72 Å. In the second Pr site, Pr is bonded to four equivalent Nd and eight equivalent Pr atoms to form PrPr8Nd4 cuboctahedra that share corners with four equivalent PrPr8Nd4 cuboctahedra, corners with eight equivalent NdPr12 cuboctahedra, edges with twenty-four PrPr8Nd4 cuboctahedra, faces with six equivalent NdPr12 cuboctahedra, and faces with twelve PrPr8Nd4 cuboctahedra.

36 MATERIALS SCIENCE↗