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

Joseph A. Mattocks, Jonathan J. Jung, Chi-Yun Lin, Ziye Dong, Neela H. Yennawar, Emily R. Featherston, Christina S. Kang-Yun, Timothy A. Hamilton, Dan M. Park (), Amie K. Boal () and Joseph A. Cotruvo ()
Additional contact information
Joseph A. Mattocks: The Pennsylvania State University
Jonathan J. Jung: The Pennsylvania State University
Chi-Yun Lin: The Pennsylvania State University
Ziye Dong: Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory
Neela H. Yennawar: The Huck Institutes of the Life Sciences, The Pennsylvania State University
Emily R. Featherston: The Pennsylvania State University
Christina S. Kang-Yun: Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory
Timothy A. Hamilton: The Pennsylvania State University
Dan M. Park: Critical Materials Institute, Physical and Life Sciences Directorate, Lawrence Livermore National Laboratory
Amie K. Boal: The Pennsylvania State University
Joseph A. Cotruvo: The Pennsylvania State University

Nature, 2023, vol. 618, issue 7963, 87-93

Abstract: Abstract Technologically critical rare-earth elements are notoriously difficult to separate, owing to their subtle differences in ionic radius and coordination number1–3. The natural lanthanide-binding protein lanmodulin (LanM)4,5 is a sustainable alternative to conventional solvent-extraction-based separation6. 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.

Date: 2023
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DOI: 10.1038/s41586-023-05945-5

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