Details
| Original language | English |
|---|---|
| Journal | Small Methods |
| Early online date | 15 Oct 2024 |
| Publication status | E-pub ahead of print - 15 Oct 2024 |
Abstract
Artificial membranes with ion-selective nanochannels for high-efficiency mono/divalent ion separation are of great significance in water desalination and lithium-ion extraction, but they remain a great challenge due to the slight physicochemical property differences of various ions. Here, the successful synthesis of two-dimensional TpEBr-based covalent organic framework (COF) nanosheets, and the stacking of them as consecutive membranes for efficient mono/divalent ion separation is reported. The obtained COF nanosheet membranes with intrinsic one-dimensional pores and abundant cationic sites display high permeation rates for monovalent cations (K+, Na+, Li+) of ≈0.1–0.3 mol m−2 h−1, while the value of divalent cations (Ca2+, Mg2+) is two orders of magnitude lower, resulting in an ultrahigh mono/divalent cation separation selectivity up to 130.4, superior to the state-of-the-art ion sieving membranes. Molecular dynamics simulations further confirm that electrostatic interaction controls the confined transport of cations through the cationic COF nanopores, where multivalent cations face i) strong electrostatic repulsion and ii) steric transport hindrance since the large hydrated divalent cations are retarded due to a layer of strongly adsorbed chloride ions at the pore wall, while smaller monovalent cations can swiftly permeate through the nanopores.
Keywords
- cationic covalent organic frameworks (cationic COFs), confined transport, ion sieving, membrane separation, nanosheets
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Materials Science(all)
- General Materials Science
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In: Small Methods, 15.10.2024.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Engineering of Covalent Organic Framework Nanosheet Membranes for Fast and Efficient Ion Sieving
T2 - Charge-Induced Cation Confined Transport
AU - Wang, Rui
AU - Ding, Li
AU - Xue, Jian
AU - Wu, Haoyu
AU - Cai, Chengzhi
AU - Qiao, Zhiwei
AU - Caro, Jürgen
AU - Wang, Haihui
N1 - Publisher Copyright: © 2024 Wiley-VCH GmbH.
PY - 2024/10/15
Y1 - 2024/10/15
N2 - Artificial membranes with ion-selective nanochannels for high-efficiency mono/divalent ion separation are of great significance in water desalination and lithium-ion extraction, but they remain a great challenge due to the slight physicochemical property differences of various ions. Here, the successful synthesis of two-dimensional TpEBr-based covalent organic framework (COF) nanosheets, and the stacking of them as consecutive membranes for efficient mono/divalent ion separation is reported. The obtained COF nanosheet membranes with intrinsic one-dimensional pores and abundant cationic sites display high permeation rates for monovalent cations (K+, Na+, Li+) of ≈0.1–0.3 mol m−2 h−1, while the value of divalent cations (Ca2+, Mg2+) is two orders of magnitude lower, resulting in an ultrahigh mono/divalent cation separation selectivity up to 130.4, superior to the state-of-the-art ion sieving membranes. Molecular dynamics simulations further confirm that electrostatic interaction controls the confined transport of cations through the cationic COF nanopores, where multivalent cations face i) strong electrostatic repulsion and ii) steric transport hindrance since the large hydrated divalent cations are retarded due to a layer of strongly adsorbed chloride ions at the pore wall, while smaller monovalent cations can swiftly permeate through the nanopores.
AB - Artificial membranes with ion-selective nanochannels for high-efficiency mono/divalent ion separation are of great significance in water desalination and lithium-ion extraction, but they remain a great challenge due to the slight physicochemical property differences of various ions. Here, the successful synthesis of two-dimensional TpEBr-based covalent organic framework (COF) nanosheets, and the stacking of them as consecutive membranes for efficient mono/divalent ion separation is reported. The obtained COF nanosheet membranes with intrinsic one-dimensional pores and abundant cationic sites display high permeation rates for monovalent cations (K+, Na+, Li+) of ≈0.1–0.3 mol m−2 h−1, while the value of divalent cations (Ca2+, Mg2+) is two orders of magnitude lower, resulting in an ultrahigh mono/divalent cation separation selectivity up to 130.4, superior to the state-of-the-art ion sieving membranes. Molecular dynamics simulations further confirm that electrostatic interaction controls the confined transport of cations through the cationic COF nanopores, where multivalent cations face i) strong electrostatic repulsion and ii) steric transport hindrance since the large hydrated divalent cations are retarded due to a layer of strongly adsorbed chloride ions at the pore wall, while smaller monovalent cations can swiftly permeate through the nanopores.
KW - cationic covalent organic frameworks (cationic COFs)
KW - confined transport
KW - ion sieving
KW - membrane separation
KW - nanosheets
UR - http://www.scopus.com/inward/record.url?scp=85206306713&partnerID=8YFLogxK
U2 - 10.1002/smtd.202401111
DO - 10.1002/smtd.202401111
M3 - Article
AN - SCOPUS:85206306713
JO - Small Methods
JF - Small Methods
ER -