Abstract
The development of an effective host molecule to separate lanthanide (Ln) ions and a method for predicting its guest recognition/self-assembly behavior based on primary chemical structures are highly sought after in both academia and industry. Herein, we report the improvement of one-pot Ln ion recovery and a performance prediction method for four new cyclic peptide hosts that differ in the position of acidic amino acids. These cyclic peptide hosts could recognize Ln3+ directly through a 1:1 complexation–precipitation process and exhibited high Lu3+ selectivity in spite of similar ion size and electronegativity when the positions of the acidic amino acids were changed. This unpredictable selectivity was explained by considering the dipole moment, lowest unoccupied molecular orbital, and cohesion energy. In addition, a semi-empirical function using these parameters was proposed for screening the sequence and estimating the isolated yields without long-time molecular dynamics calculations. The insights obtained from this study can be employed for the development of high-performance peptides for the selective recovery of Ln and other metal ions, as well as for the construction of diverse supramolecular recognition systems.
Highlights
Academic Editor: M AkbarLanthanides are indispensable for applications in advanced materials; a cost-effective recovery process with low energy expenditure is required to meet the rapidly increasing demand for these elements [1]
We recently reported a lanthanide ion mineralization peptide (Lamp1) with a cyclic structure that was inspired by natural mineralization, such as the pearl formation of pearl oysters [2]
The major driving force of Lamp1 in Ln3+ recognition is the electrostatic interactions from the side-chain COOH moieties of the acidic amino acids (AAs), namely aspartic acid (D) and glutamic acid (E)
Summary
Lanthanides are indispensable for applications in advanced materials; a cost-effective recovery process with low energy expenditure is required to meet the rapidly increasing demand for these elements [1]. We recently reported a lanthanide ion mineralization peptide (Lamp1) with a cyclic structure that was inspired by natural mineralization, such as the pearl formation of pearl oysters [2]. Lamp could directly recover lanthanide ions (Ln3+ ) as precipitates in water under ambient conditions in a one-pot, environmentally friendly, and low-energy process, without the use of organic solvents or column chromatography. Using a genetic recombination technique, we have created functional silk fused with Lamp and proven the direct recovery of Ln3+ using silk materials [3]. The precipitation is driven by self-assembly, which is promoted by the hydrophobic nature of the formed Ln complex
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