Mild synthesis of bi-carboxylated COFs nanosheets for the preparation of high-efficiency nano-wrinkled TFN membrane

Wenqiao Meng; Qiang Xue; Kayode Hassan Lasisi; Kaisong Zhang

doi:10.1016/j.seppur.2024.130661

Mild synthesis of bi-carboxylated COFs nanosheets for the preparation of high-efficiency nano-wrinkled TFN membrane

Wenqiao Meng, Qiang Xue, Kayode Hassan Lasisi, Kaisong Zhang

Department of Chemical Engineering

Research output: Contribution to journal › Article › peer-review

11 Citations (SciVal)

Abstract

The development of thinner and nano-wrinkled polyamide (PA) layer is crucial for overcoming the inherent trade-off between permeance and selectivity in conventional nanofiltration membranes. In this study, bi-carboxylated covalent organic frameworks (COFs) nanosheets (TpPa-(COOH)₂ CONs) with ordered open pore channels were synthesized by employing green deep eutectic solvents (DES). Subsequently, the TpPa-(COOH)₂ CONs were dispersed in the aqueous phase to regulate the interfacial polymerization (IP) process, leading to the formation of thin-film nanocomposite (TFN) membranes with thinner and nano-wrinkled PA layer. The resultant membranes exhibited superior water permeance of 12.20 L·m⁻²·h⁻¹·bar⁻¹ and Na₂SO₄ rejection of 99.15 %, which was significantly superior to the TFC membrane without TpPa-(COOH)₂ CONs (5.70 L·m⁻²·h⁻¹·bar⁻¹ and 96.28 %). Moreover, the modified membranes demonstrated enhanced removal rates for five major antibiotics, exceeding 85.00 %. Molecular dynamics (MD) simulation confirmed the regulation of PIP diffusion by nanosheets. The excellent stability and anti-fouling characteristics of the resultant membrane contributes to its promising application prospect in seawater desalination. This work presented a valuable strategy for the preparation of high-efficiency nano-wrinkled TFN-NF membranes for desalination.

Original language	English
Article number	130661
Number of pages	18
Journal	Separation and Purification Technology
Volume	359
Early online date	23 Nov 2024
DOIs	https://doi.org/10.1016/j.seppur.2024.130661
Publication status	Published - 22 Jun 2025

Data Availability Statement

No data was used for the research described in the article

Acknowledgements

The authors would like to acknowledge H. Ren for TEM sample
making, Z. Xu for the XPS test, D. Pan for the AFM test, and T. Yue for the
MD simulation. KS Zhang and the co-authors thanks the editor and reviewers for their helpful and insightful comments which improved the
paper greatly.

Funding

This work was supported by grants from the National Key R&D Program of China (2023YFC3709005, 2021YFC3201402), the Ministry of Science and Technology. The Fujian Provincial Department of Science and Technology (2022T3002). KS Zhang thanks Ocean Univesity of China for providing Zhufeng Distinguished Professor Fellowship. The authors thank Oxiamembrane Co., Ltd. for the financial and technical support.

Keywords

Antibiotics removal
Bi-carboxylated CONs
Interfacial polymerization
MD stimulation
Nanofiltration

ASJC Scopus subject areas

Analytical Chemistry
Filtration and Separation

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10.1016/j.seppur.2024.130661

Cite this

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title = "Mild synthesis of bi-carboxylated COFs nanosheets for the preparation of high-efficiency nano-wrinkled TFN membrane",

abstract = "The development of thinner and nano-wrinkled polyamide (PA) layer is crucial for overcoming the inherent trade-off between permeance and selectivity in conventional nanofiltration membranes. In this study, bi-carboxylated covalent organic frameworks (COFs) nanosheets (TpPa-(COOH)2 CONs) with ordered open pore channels were synthesized by employing green deep eutectic solvents (DES). Subsequently, the TpPa-(COOH)2 CONs were dispersed in the aqueous phase to regulate the interfacial polymerization (IP) process, leading to the formation of thin-film nanocomposite (TFN) membranes with thinner and nano-wrinkled PA layer. The resultant membranes exhibited superior water permeance of 12.20 L·m−2·h−1·bar−1 and Na2SO4 rejection of 99.15 \%, which was significantly superior to the TFC membrane without TpPa-(COOH)2 CONs (5.70 L·m−2·h−1·bar−1 and 96.28 \%). Moreover, the modified membranes demonstrated enhanced removal rates for five major antibiotics, exceeding 85.00 \%. Molecular dynamics (MD) simulation confirmed the regulation of PIP diffusion by nanosheets. The excellent stability and anti-fouling characteristics of the resultant membrane contributes to its promising application prospect in seawater desalination. This work presented a valuable strategy for the preparation of high-efficiency nano-wrinkled TFN-NF membranes for desalination.",

keywords = "Antibiotics removal, Bi-carboxylated CONs, Interfacial polymerization, MD stimulation, Nanofiltration",

author = "Wenqiao Meng and Qiang Xue and Lasisi, \{Kayode Hassan\} and Kaisong Zhang",

year = "2025",

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doi = "10.1016/j.seppur.2024.130661",

language = "English",

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journal = "Separation and Purification Technology",

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AU - Meng, Wenqiao

AU - Xue, Qiang

AU - Lasisi, Kayode Hassan

AU - Zhang, Kaisong

PY - 2025/6/22

Y1 - 2025/6/22

N2 - The development of thinner and nano-wrinkled polyamide (PA) layer is crucial for overcoming the inherent trade-off between permeance and selectivity in conventional nanofiltration membranes. In this study, bi-carboxylated covalent organic frameworks (COFs) nanosheets (TpPa-(COOH)2 CONs) with ordered open pore channels were synthesized by employing green deep eutectic solvents (DES). Subsequently, the TpPa-(COOH)2 CONs were dispersed in the aqueous phase to regulate the interfacial polymerization (IP) process, leading to the formation of thin-film nanocomposite (TFN) membranes with thinner and nano-wrinkled PA layer. The resultant membranes exhibited superior water permeance of 12.20 L·m−2·h−1·bar−1 and Na2SO4 rejection of 99.15 %, which was significantly superior to the TFC membrane without TpPa-(COOH)2 CONs (5.70 L·m−2·h−1·bar−1 and 96.28 %). Moreover, the modified membranes demonstrated enhanced removal rates for five major antibiotics, exceeding 85.00 %. Molecular dynamics (MD) simulation confirmed the regulation of PIP diffusion by nanosheets. The excellent stability and anti-fouling characteristics of the resultant membrane contributes to its promising application prospect in seawater desalination. This work presented a valuable strategy for the preparation of high-efficiency nano-wrinkled TFN-NF membranes for desalination.

AB - The development of thinner and nano-wrinkled polyamide (PA) layer is crucial for overcoming the inherent trade-off between permeance and selectivity in conventional nanofiltration membranes. In this study, bi-carboxylated covalent organic frameworks (COFs) nanosheets (TpPa-(COOH)2 CONs) with ordered open pore channels were synthesized by employing green deep eutectic solvents (DES). Subsequently, the TpPa-(COOH)2 CONs were dispersed in the aqueous phase to regulate the interfacial polymerization (IP) process, leading to the formation of thin-film nanocomposite (TFN) membranes with thinner and nano-wrinkled PA layer. The resultant membranes exhibited superior water permeance of 12.20 L·m−2·h−1·bar−1 and Na2SO4 rejection of 99.15 %, which was significantly superior to the TFC membrane without TpPa-(COOH)2 CONs (5.70 L·m−2·h−1·bar−1 and 96.28 %). Moreover, the modified membranes demonstrated enhanced removal rates for five major antibiotics, exceeding 85.00 %. Molecular dynamics (MD) simulation confirmed the regulation of PIP diffusion by nanosheets. The excellent stability and anti-fouling characteristics of the resultant membrane contributes to its promising application prospect in seawater desalination. This work presented a valuable strategy for the preparation of high-efficiency nano-wrinkled TFN-NF membranes for desalination.

KW - Antibiotics removal

KW - Bi-carboxylated CONs

KW - Interfacial polymerization

KW - MD stimulation

KW - Nanofiltration

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ER -

Mild synthesis of bi-carboxylated COFs nanosheets for the preparation of high-efficiency nano-wrinkled TFN membrane

Abstract

Data Availability Statement

Acknowledgements

Funding

Keywords

ASJC Scopus subject areas

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