2022
DOI: 10.1038/s41467-022-32178-3
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Selective separation of light rare-earth elements by supramolecular encapsulation and precipitation

Abstract: Supramolecular chemical strategies for Rare Earth (RE) element separations are emerging which amplify the small changes in properties across the series to bias selectivity in extraction or precipitation. These advances are important as the REs are crucial to modern technologies yet their extraction, separation, and recycling using conventional techniques remain challenging. We report here a pre-organised triamidoarene platform which, under acidic, biphasic conditions, uniquely and selectively precipitates ligh… Show more

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Cited by 41 publications
(49 citation statements)
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“…Yield: 3.83 g (48%); mp 72−74 °C; Raman (80 mW, in cm −1 ) ν: 3083 (16), 2983 (26), 2937 (52), 2929 (53), 2873 (18), 1598 (100), 1570 (13), 1527 (15), 1494 (20), 1450 (23), 1427 (14), 1415 (13), 1402 (19), 1369 (21), 1344 (21), 1313 (14), 1284 (13), 1178 (13), 1095 (25), 1053 (24), 837 (17), 671 (22), 73 (56); IR (ATR, in cm −1 ) ν: 2980 (vw), 2933 (vw), 2877 (vw), 1597 (vw), 1587 (vw), 1562 (w), 1520 (w), 1493 (m), 1468 (w), 1450 (vw), 1414 (w), 1387 (w), 1375 (w), 1336 (w), 1282 (vw), 1269 (vw), 1242 (vw), 1178 (w), 1153 (m), 1101 (w), 1053 (vw), 978 (vs), 937 (w), 899 (w), 887 (w), 850 (vw), 829 (m), 775 (m), 748 (m), 704 (vw), 669 (m), 646 (w), 629 (vw), 607 (w), 575 (s), 530 (w), 519 (w), 503 (w), 422 (w); 1 H NMR (CDCl 3 , 300 K, in ppm): δ 1.28 (6H, d, 3 J HH = 6.2 Hz, H6a), 1.40 (6H, d, 3 J HH = 6.1 Hz, H6b), 2.27 (3H, d, 4 J HP = 0.7 Hz, H4), 4.62 (2H, d sept, 3 J HP = 7.7 Hz, 3 J HH = 6.3 Hz, H5), 7.39 (2H, md, 3 J HH = 9.0 Hz, H9/H10), 7.77 (2H, md, 3 J HH = 9.0 Hz, H9/ H10); 13 4.8. General Procedure for the Syntheses of Lanthanum(III), Europium(III), and Ytterbium(III) Complexes.…”
Section: Synthesis Of Diisopropyl(5-hydroxy-3-methyl-1-phenyl-1hpyraz...mentioning
confidence: 99%
See 1 more Smart Citation
“…Yield: 3.83 g (48%); mp 72−74 °C; Raman (80 mW, in cm −1 ) ν: 3083 (16), 2983 (26), 2937 (52), 2929 (53), 2873 (18), 1598 (100), 1570 (13), 1527 (15), 1494 (20), 1450 (23), 1427 (14), 1415 (13), 1402 (19), 1369 (21), 1344 (21), 1313 (14), 1284 (13), 1178 (13), 1095 (25), 1053 (24), 837 (17), 671 (22), 73 (56); IR (ATR, in cm −1 ) ν: 2980 (vw), 2933 (vw), 2877 (vw), 1597 (vw), 1587 (vw), 1562 (w), 1520 (w), 1493 (m), 1468 (w), 1450 (vw), 1414 (w), 1387 (w), 1375 (w), 1336 (w), 1282 (vw), 1269 (vw), 1242 (vw), 1178 (w), 1153 (m), 1101 (w), 1053 (vw), 978 (vs), 937 (w), 899 (w), 887 (w), 850 (vw), 829 (m), 775 (m), 748 (m), 704 (vw), 669 (m), 646 (w), 629 (vw), 607 (w), 575 (s), 530 (w), 519 (w), 503 (w), 422 (w); 1 H NMR (CDCl 3 , 300 K, in ppm): δ 1.28 (6H, d, 3 J HH = 6.2 Hz, H6a), 1.40 (6H, d, 3 J HH = 6.1 Hz, H6b), 2.27 (3H, d, 4 J HP = 0.7 Hz, H4), 4.62 (2H, d sept, 3 J HP = 7.7 Hz, 3 J HH = 6.3 Hz, H5), 7.39 (2H, md, 3 J HH = 9.0 Hz, H9/H10), 7.77 (2H, md, 3 J HH = 9.0 Hz, H9/ H10); 13 4.8. General Procedure for the Syntheses of Lanthanum(III), Europium(III), and Ytterbium(III) Complexes.…”
Section: Synthesis Of Diisopropyl(5-hydroxy-3-methyl-1-phenyl-1hpyraz...mentioning
confidence: 99%
“…Yield: 88 mg (51%); mp 200−202 °C; Raman (100 mW, in cm −1 ): 2924 (6), 1600 (35), 1328 (100), 1295 (9), 1175 (5), 1113 (20), 1061 (6), 73 (11); IR (ATR, in cm −1 ): 2979 (vw), 1599 (m), 1555 (m), 1514 (m), 1422 (w), 1373 (w), 1325 (vs), 1292 (m), 1157 (m), 1103 (w), 985 (vs), 889 (w), 854 (m), 837 (w), 775 (m), 751 (m), 735 (w), 683 (vw), 636 (w), 623 (w), 593 (m), 579 (s), 548 (w), 534 (w), 496 (w), 420 (vw); The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.2c04221.…”
mentioning
confidence: 99%
“…In particular, a tripodal amido-arene synthon, in a biphasic HNO 3 /toluene system, could form a capsular structure hosting hexanitrometalate anions. The supramolecular assembly showed a lanthanide-dependent precipitation, thus leading to the selective separation of light from heavy lanthanide cations . Despite the similar chemical properties and ionic charges, different lanthanide ions may exhibit different coordination numbers (cn) and geometries when forming coordination compounds .…”
Section: Introductionmentioning
confidence: 99%
“…The supramolecular assembly showed a lanthanide-dependent precipitation, thus leading to the selective separation of light from heavy lanthanide cations. 45 Despite the similar chemical properties and ionic charges, different lanthanide ions may exhibit different coordination numbers (cn) and geometries when forming coordination compounds. 46 The different structural features usually result in different physical properties, as in the case of compounds formed between various lanthanide ions and bidentate-functionalized 8-quinolinols in organic solvents.…”
Section: Introductionmentioning
confidence: 99%
“…The key to this potentially cost-effective separation strategy is finding the optimal ligands for the actinides. Organic, inorganic, or biorelevant ligands have been utilized to achieve selective crystallization of f-block metal ions in the form of metal–organic complexes, metal–organic frameworks (MOFs), or inorganic compounds in the recent decade. However, most of the studies have specified that size-selective crystallization led to intragroup lanthanide separation while the binding preference of these ligands to 5f-block metal ions being involved in the crystallization of An-MOFs is underexplored. We propose to integrate the difference in solubility products ( K sp ) for fractional crystallization as well as the difference in the formation constants of metal complexes ( K f ) in solvent extraction into a unified An-MOF platform due to (i) a wide variety of organic ligands display a higher selectivity for 5f-block metals in contrast to a limited selection of inorganic anions and (ii) the small differences in these constants would be amplified during the crystallization and lead to the efficient isolation of An-MOFs as the primary waste form, which can then be surface-modified, cold-pressed, or encapsulated with geopolymers to fabricate the final waste form (Scheme ).…”
mentioning
confidence: 99%