Constructing a selective blocked-nanolayer on nanofiltration membrane via surface-charge inversion for promoting Li+ permselectivity over Mg2+

Lu, Dan; Ma, Tao; Lin, Shupeng; Zhou, Zhijun; Li, Ge; An, Quan‐Fu; Yao, Zhikan; Sun, Qi; Sun, Zhilin; Zhang, Lin

doi:10.1016/j.memsci.2021.119504

Cited by 111 publications

(33 citation statements)

References 42 publications

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“…This indicated that DABIL modification rendered the membrane with improved antifouling capability. The improved antifouling performance of the DABIL-5 membrane can be reasonably attributed to the enhanced surface hydrophilicity and high SFE, 37,50,51 as well as the reinforced Donnan exclusion effect of the strong positively charged surface toward the high-valent scaling ions, 52 which creates unfavorable circumstances that decrease the chances of foulant adsorption. In this way, the DABIL-5 membrane demonstrates effectiveness in mitigating the scaling risk on the membrane surface and thus indicates applicable potential in the practical Mg 2+ /Li + separation process.…”

Section: Antifouling and Chemical Stabilitymentioning

confidence: 99%

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Liu

Wen

Liao

2022

ACS Appl. Mater. Interfaces

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Lithium separation is of great significance to overcome the lithium supply shortage resulting from a heightened demand in the energy sector. The low selectivity of polymer nanofiltration membranes for lithium extraction from concentrated Mg/Li mixtures caused by miniaturized pore structures and weak and unstable positive surface charges limits their practical implementation. To address the surface charge strength and stability, a novel ionic liquid monomer, N1-(6-aminohexyl)-N1,N1,N6,N6,N6-pentamethylhexane-1,6-diaminium bromide (denoted as DABIL), is first synthesized and covalently anchored on a pristine polyamide thin-film composite (TFC) membrane via a secondary amidation reaction for improved selective lithium separation from Mg/Li mixtures. DABIL modification of the polyamide network contributes to increased surface hydrophilicity, an enlarged membrane pore structure, and reinforced Donnan exclusion effects. Molecular dynamics simulation confirmed that the difference of the interaction energies between water and the multication groups dominates the surface properties. The DABIL membrane exhibits sixfold enhancement of water permeability compared to the unmodified membrane and outperforms the recently reported state-of-the-art positively charged membranes. It presents an improved Li+/Mg2+ selectivity of 26.49, suggesting the membranes’ potential for lithium recovery. Moreover, the membrane shows efficient antibacterial activity for mitigating biofilm formation. We establish that functionalization of TFC membranes with ionic liquids containing multication side chains could be a promising approach to achieve improved and sustainable permselectivity for the recovery of critical metal resources.

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Section: Antifouling and Chemical Stabilitymentioning

confidence: 99%

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Liu

Wen

Liao

2022

ACS Appl. Mater. Interfaces

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“…The use of alcohol ensures no deterioration effect of the nascent thin film and does not compromise its permeance. In this way, precise control of the ratio of positive and negative functional groups on the membrane surface can be achieved, obtaining a series of electroneutral NF membranes, which has not been reported in previous solvation works 34,35 . Thanks to the charge‐balance state of the electroneutral membrane, 36,37 the anti‐fouling property is enhanced sharply and the Donnan equilibrium effect is minimized while the size sieving is highlighted.…”

Section: Introductionmentioning

confidence: 93%

“…Substituting alcohols for water as the medium for the secondary reaction will inhibit the hydrolysis of acyl chloride groups into carboxyl groups, thereby reducing the negative membrane charges. Meanwhile, benefiting from its miscibility with n ‐hexane and solvation effect of alcohol, 34,35 short linear amines can aminate acyl chlorides more thoroughly, thereby introducing more positively charged groups without sacrificing the free volume. The use of alcohol ensures no deterioration effect of the nascent thin film and does not compromise its permeance.…”

Section: Introductionmentioning

confidence: 99%

“…In this way, precise control of the ratio of positive and negative functional groups on the membrane surface can be achieved, obtaining a series of electroneutral NF membranes, which has not been reported in previous solvation works. 34,35 Thanks to the chargebalance state of the electroneutral membrane, 36,37 (EDA, AR, Aladdin), diethylenetriamine (DETA, 97%, Aladdin), triethylenetetramine (TETA, AR, Aladdin), tetraethylenepentamine (TEPA, AR, Aladdin), pentaethylenehexamine (PEHA, AR, Aladdin), trimesoyl chloride (TMC, 98%, Aladdin), and alcohols (ethanol, isopropyl alcohol, and n-butanol; AR; Shanghai Hushi Chem. Co., Ltd.) were used to fabricate the selective layers.…”

Section: Introductionmentioning

confidence: 99%

“…Meanwhile, benefiting from its miscibility with n-hexane and solvation effect of alcohol, 34,35 short linear amines can aminate acyl chlorides more thoroughly, thereby introducing more positively charged groups without sacrificing the free volume. The use of alcohol ensures no deterioration effect of the nascent thin film and does not compromise its permeance.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Solvation‐amination‐synergy that neutralizes interfacially polymerized membranes for ultrahigh selective nanofiltration

Tang

Liu

et al. 2022

AIChE Journal

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Molecular desalination is broadly used in chemical, food, and textile industries, which needs efficient and anti‐fouling separation technologies to reach this goal. Interfacial polymerization is one of the most promising routes to construct ultrahigh selective nanofiltration membranes. However, the irreversible hydrolysis of residual acyl chlorides makes Donnan charges of nascent films distribute unevenly which hinders fine molecular desalination and anti‐fouling. Here, we propose a pioneering solvation‐amination‐synergy strategy to synchronously inhibit the hydrolysis of residual acyl chlorides and promote their amination. The electroneutral nanofiltration membrane with high water permeance (13.2 L m−2 h−1 bar−1) is quantitatively fabricated that has superb anti‐fouling abilities and minimizes Donnan impacts on competitive ion penetrations, so it transmits Na2SO4 and NaCl while fully obstructs cationic or anionic dyes (< 500 Da). The ultrahigh molecule to ion selectivities outperform state‐of‐art nanofiltration membranes, which may provide a paradigm shift for scalable membrane fabrication for various industrial product desalination.

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Designing Gemini‐Electrolytes for Scalable Mg²⁺/Li⁺ Separation Membranes and Modules

Peng,

Su,

Liu

et al. 2023

Adv Funct Materials

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High performance polyamide nanofiltration membranes play important roles in Mg2+/Li+ separation and Li+ extraction, but they are prepared via multiple time‐/labor demanding steps. Both the scalability of these membranes and the engineering of membrane modules remain an elusive challenge. Here the design of a Gemini‐electrolyte monomer (GEM) featuring bidentate amine groups, quaternary ammonia, and endocyclic contorted conformation is reported. The monomer's low interfacial diffusivity is balanced by high condensational reactivity during its interfacial polymerization with trimesoyl chloride (TMC), leading to the straightforward formation of defect‐free, ≈14 nm thick membranes. The membrane shows the highest permeance (≈19.2 L m−2 h−1 bar−1) among Mg2+/Li+ nanofiltration membranes prepared via straightforward interfacial polymerization without post‐modification, combined with good Mg2+/Li+ selectivity (≈15.4) and stability. The validity of GEM design is verified by control monomers. Large‐area (1 × 2 m2) GEM‐TMC membranes and spiral‐wound modules (effective area: 0.5 m2) are prepared, both of which show reproducible and high performance.

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Constructing a selective blocked-nanolayer on nanofiltration membrane via surface-charge inversion for promoting Li+ permselectivity over Mg2+

Cited by 111 publications

References 42 publications

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Solvation‐amination‐synergy that neutralizes interfacially polymerized membranes for ultrahigh selective nanofiltration

Designing Gemini‐Electrolytes for Scalable Mg²⁺/Li⁺ Separation Membranes and Modules

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Constructing a selective blocked-nanolayer on nanofiltration membrane via surface-charge inversion for promoting Li+ permselectivity over Mg2+

Cited by 111 publications

References 42 publications

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Nanofiltration Membranes Modified with a Clustered Multiquaternary Ammonium-Based Ionic Liquid for Improved Magnesium/Lithium Separation

Solvation‐amination‐synergy that neutralizes interfacially polymerized membranes for ultrahigh selective nanofiltration

Designing Gemini‐Electrolytes for Scalable Mg2+/Li+ Separation Membranes and Modules

Contact Info

Product

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Designing Gemini‐Electrolytes for Scalable Mg²⁺/Li⁺ Separation Membranes and Modules