Author
Listed:
- 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
The Pennsylvania State University)
- Joseph A. Cotruvo
(The Pennsylvania State University)
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.
Suggested Citation
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 & Joseph A. Cotruv, 2023.
"Enhanced rare-earth separation with a metal-sensitive lanmodulin dimer,"
Nature, Nature, vol. 618(7963), pages 87-93, June.
Handle:
RePEc:nat:nature:v:618:y:2023:i:7963:d:10.1038_s41586-023-05945-5
DOI: 10.1038/s41586-023-05945-5
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Citations
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Cited by:
- Kevin Y. Huang & Lizette Cardenas & Andrew D. Ellington & David J. F. Walker, 2024.
"Supercharged fluorescent proteins detect lanthanides via direct antennae signaling,"
Nature Communications, Nature, vol. 15(1), pages 1-11, December.
- Yuxia Liu & Duyang Gao & Yuanyuan He & Jing Ma & Suet Yen Chong & Xinyi Qi & Hui Jun Ting & Zichao Luo & Zhigao Yi & Jingyu Tang & Chao Chang & Jiongwei Wang & Zonghai Sheng & Hairong Zheng & Xiaogang, 2024.
"Single-point mutated lanmodulin as a high-performance MRI contrast agent for vascular and kidney imaging,"
Nature Communications, Nature, vol. 15(1), pages 1-14, December.
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