Tuneable ion selectivity in vermiculite membranes intercalated with unexchangeable ions

Fuente: arXiv
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Main Authors: Liu, Zhuang, Tan, Yumei, Qian, Jianhao, Cao, Min, Hoenig, Eli, Yang, Guowei, Wang, Fengchao, Peeters, Francois M., Zou, Yi-Chao, Chu, Liang-Yin, Lozada-Hidalgo, Marcelo
Format: Preprint
Published: 2025
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author Liu, Zhuang
Tan, Yumei
Qian, Jianhao
Cao, Min
Hoenig, Eli
Yang, Guowei
Wang, Fengchao
Peeters, Francois M.
Zou, Yi-Chao
Chu, Liang-Yin
Lozada-Hidalgo, Marcelo
author_facet Liu, Zhuang
Tan, Yumei
Qian, Jianhao
Cao, Min
Hoenig, Eli
Yang, Guowei
Wang, Fengchao
Peeters, Francois M.
Zou, Yi-Chao
Chu, Liang-Yin
Lozada-Hidalgo, Marcelo
contents Membranes selective to ions of the same charge are increasingly sought for wastewater processing and valuable element recovery. However, while narrow channels are known to be essential, other membrane parameters remain difficult to identify and control. Here we show that Zr$^{4+}$, Sn$^{4+}$, Ir$^{4+}$, and La$^{3+}$ ions intercalated into vermiculite laminate membranes become effectively unexchangeable, creating stable channels, one to two water layers wide, that exhibit robust and tuneable ion selectivity. Ion permeability in these membranes spans five orders of magnitude, following a trend dictated by the ions' Gibbs free energy of hydration. Unexpectedly, different intercalated ions lead to two distinct monovalent ion selectivity sequences, despite producing channels of identical width. The selectivity instead correlates with the membranes' stiffness and the entropy of hydration of the intercalated ions. These results introduce a new ion selectivity mechanism driven by entropic and mechanical effects, beyond classical size and charge exclusion.
format Preprint
id arxiv_https___arxiv_org_abs_2510_23153
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Tuneable ion selectivity in vermiculite membranes intercalated with unexchangeable ions
Liu, Zhuang
Tan, Yumei
Qian, Jianhao
Cao, Min
Hoenig, Eli
Yang, Guowei
Wang, Fengchao
Peeters, Francois M.
Zou, Yi-Chao
Chu, Liang-Yin
Lozada-Hidalgo, Marcelo
Soft Condensed Matter
Materials Science
Chemical Physics
Membranes selective to ions of the same charge are increasingly sought for wastewater processing and valuable element recovery. However, while narrow channels are known to be essential, other membrane parameters remain difficult to identify and control. Here we show that Zr$^{4+}$, Sn$^{4+}$, Ir$^{4+}$, and La$^{3+}$ ions intercalated into vermiculite laminate membranes become effectively unexchangeable, creating stable channels, one to two water layers wide, that exhibit robust and tuneable ion selectivity. Ion permeability in these membranes spans five orders of magnitude, following a trend dictated by the ions' Gibbs free energy of hydration. Unexpectedly, different intercalated ions lead to two distinct monovalent ion selectivity sequences, despite producing channels of identical width. The selectivity instead correlates with the membranes' stiffness and the entropy of hydration of the intercalated ions. These results introduce a new ion selectivity mechanism driven by entropic and mechanical effects, beyond classical size and charge exclusion.
title Tuneable ion selectivity in vermiculite membranes intercalated with unexchangeable ions
topic Soft Condensed Matter
Materials Science
Chemical Physics
url https://arxiv.org/abs/2510.23153