Enhanced rare-earth separation with a metal-sensitive lanmodulin dimer

Mattocks, Joseph A.; Jung, Jonathan J.; Lin, Chi-Yun; Dong, Ziye; Yennawar, Neela H.; Featherston, Emily R.; Kang-Yun, Christina S.; Hamilton, Timothy A.; Park, Dan M.; Boal, Amie K.; Cotruvo, Joseph A.

doi:10.1038/s41586-023-05945-5

Enhanced rare-earth separation with a metal-sensitive lanmodulin dimer

Journal Article · Wed May 31 00:00:00 EDT 2023 · Nature (London)

DOI:https://doi.org/10.1038/s41586-023-05945-5· OSTI ID:1993554

^[1]; ^[1]; ^[1]; Dong, Ziye ^[2]; ^[1]; Featherston, Emily R. ^[1]; Kang-Yun, Christina S. ^[2]; ^[1]; ^[2]; ^[1]; ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Technologically critical rare-earth elements are notoriously difficult to separate, owing to their subtle differences in ionic radius and coordination number. The natural lanthanide-binding protein lanmodulin (LanM) is a sustainable alternative to conventional solvent-extraction-based separation. Here we characterize a new LanM, from Hansschlegelia quercus (Hans-LanM), with an oligomeric state sensitive to rare-earth ionic radius, the lanthanum(III)-induced dimer being >100-fold tighter than the dysprosium(III)-induced dimer. X-ray crystal structures illustrate how picometre-scale differences in radius between lanthanum(III) and dysprosium(III) are propagated to Hans-LanM’s quaternary structure through a carboxylate shift that rearranges a second-sphere hydrogen-bonding network. Comparison to the prototypal LanM from Methylorubrum extorquens reveals distinct metal coordination strategies, rationalizing Hans-LanM’s greater selectivity within the rare-earth elements. Finally, structure-guided mutagenesis of a key residue at the Hans-LanM dimer interface modulates dimerization in solution and enables single-stage, column-based separation of a neodymium(III)/dysprosium(III) mixture to >98% individual element purities. This work showcases the natural diversity of selective lanthanide recognition motifs, and it reveals rare-earth-sensitive dimerization as a biological principle by which to tune the performance of biomolecule-based separation processes.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO); National Science Foundation (NSF); National Institutes of Health (NIH)

Grant/Contract Number:: AC52-07NA27344; AC02-06CH11357; SC0021007

OSTI ID:: 1993554

Report Number(s):: LLNL-JRNL-840467; 1061823

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7963 Vol. 618; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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