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High-performance polyamide nanofiltration membrane with arch-bridge structure on a highly hydrated cellulose nanofiber support

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  • ReceivedApr 1, 2020
  • AcceptedApr 4, 2020
  • PublishedMay 18, 2020

Abstract

Nanofiltration (NF) membranes with outstanding performance are highly demanded for more efficient desalination and wastewater treatment. However, improving water permeance while maintaining high solute rejection by using the current membrane fabrication techniques remains a challenge. Herein, polyamide (PA) NF membrane with arch-bridge structure is successfully prepared via interfacial polymerization (IP) on a composite support membrane of salt-reinforced hydrophilic bacterial cellulose nanofibers (BCNs) nanofilm/polytetrafluoroethylene (BCNs/PTFE). The strong hydration of BCNs promotes Marangoni convection along water/organic solvent interface during the IP process, which creates extra area for interfacial reaction and produces a thin PA active layer with arch-bridge structures. These arch-bridge structures endow the resulting PA active layer with substantial larger active area for water permeation. Consequently, the PA NF membrane exhibits exceptional desalination performance with a permeance up to 42.5 L m−2 h−1 bar−1 and a rejection of Na2SO4 as high as 99.1%, yielding an overall desalination performance better than almost all of the state-of-the-art NF membranes reported so far in terms of perm-selectivity.


Funded by

the National Natural Science Funds for Distinguished Young Scholar(51625306)

the Key Project of National Natural Science Foundation of China(21433012)

the National Natural Science Foundation of China(51603229,21406258)

the State Key Laboratory of Separation Membranes and Membrane Processes(Tianjin,Polytechnic,University,No.,M1-201801)

and the CAS Pioneer Hundred Talents Program.


Acknowledgment

This work was supported by the National Natural Science Funds for Distinguished Young Scholar (51625306), the Key Project of the National Natural Science Foundation of China (21433012), the National Natural Science Foundation of China (51603229, 21406258), and the State Key Laboratory of Separation Membranes and Membrane Processes (Tianjin Polytechnic University, No. M1-201801). Funding support from the CAS Pioneer Hundred Talents Program is grateful appreciated as well.


Interest statement

The authors declare that they have no conflict of interest.


Contributions statement

Zhu Y and Jin J designed the experiments and developed the theory; Teng X performed the experiments; Lin H performed the measurement of SFG; Liu S contributed to the MD analysis; Teng X, Liang Y, Wang Z, Fang W and Zhu Y performed the data analysis; Teng X and Zhu Y wrote the paper with support from Jin J and Lin S; all authors contributed to the general discussion.


Author information

Jian Jin received her BSc (1996) and PhD degrees (2001) from Jilin University of China. She then worked as a JSPS (Japan Society for the Promotion of Science) postdoctoral fellow in the Research Center of Advanced Science and Technology at Tokyo University, Japan. From 2004 to 2009, she worked as a senior researcher at the National Institute for Materials Science, Japan, under Dr. Izumi Ichinose. In 2009, she joined Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO) at the Chinese Academy of Sciences (CAS) as a group leader. Her research interests include the design of advanced filtration membranes for environmental applications.


Yuzhang Zhu received his BSc degree (2009) from Anhui University of Science and Technology and completed his PhD (2015) from the University of Chinese Academy of Sciences. He then worked as a postdoctoral fellow in Professor Jian Jin’s group at SINANO, CAS. From 2017, he joined SINANO as an associate research professor. His current research interests focus on advanced membranes for nanofiltration, oil/water separation and stimuli-responsive separation.


Xiangxiu Teng received her BSc degree from Qingdao University of Science and Technology in 2016. Then, she joined Shanghai University of Science and Technology. At 2017, she started her research program under the supervision of Professor Jian Jin. Her research interest is the preparation of polyamide nanofiltration membrane for desalination.


Supplement

Supplementary information

Supporting data are available in the online version of the paper.


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  • Scheme 1

    Fabrication of arch-bridge TFC PA NF membrane. (a) Schematic of IP of PA on NaCl-reinforced hydrophilic BCN nanofilm. A schematic demonstrating the formation of PA active layer with arch-bridge structure on a support with good water wettability (b) and with spotted structure on a support with poor water wettability (c).

  • Figure 1

    Characterization of BCNs and BCN nanofilm. (a, b) Photographs of bacterial cellulose bulk and BCN dispersion, respectively. (c, d) AFM image of BCNs and corresponding statistic distribution of BCN diameters. (e, f) Top view and cross-sectional SEM images of BCN nanofilm deposited on PTFE MF membrane. (g, h) Photographs of free-standing BCN nanofilm dyed by Direct Red 80.

  • Figure 2

    Effect of NaCl on the surface wettability and permeance of BCN nanofilm. (a) Surface wettability of the BCN nanofilm to pure water and water containing 1 wt% NaCl. (b) Permeance variation of the BCN nanofilm as a function of filtration time using pure water and 1 wt% NaCl aqueous solution as feed, respectively. Applied pressure is 1 bar.

  • Figure 3

    Structure characterization of TFC-PA NF membranes. (a) Top view SEM image, (b) AFM image, and (c) cross-sectional TEM image of the NF membrane prepared in PIP aqueous solution without addition of salt. (d) Top view SEM image, (e) AFM image, and (f) TEM image of the cross-sectional membrane prepared in PIP aqueous solution with the addition of 1 wt% NaCl.

  • Figure 4

    Desalination performance of TFC-PA NF membranes. (a) Variation of permeance and rejection of TFC-PA NF membrane as a function of NaCl concentration in PIP aqueous solution. (b) Rejection curves of the TFC-PA NF membranes prepared with the addition of 1 wt% NaCl, KCl and LiCl in PIP aqueous solution, respectively, to PEG with different molecular weights and corresponding pore size distributions (inset). (c) Permeance and corresponding rejection of the membrane prepared with the addition of 1 wt% NaCl in PIP aqueous solution to various salts as feed solutions (the concentrations of these feeds are all 1000 ppm). (d) Summary of the desalination performance of the state-of-the-art NF membranes reported previously and the membranes obtained in this work while using Na2SO4 solution as feed. The literatures cited in Fig. 4d (Ref. S1–S17) are listed in Supplementary information.

  • Figure 5

    Characterization of the hydration state of BCN nanofilm. (a) Experimental scheme showing the test of SFG vibrational spectroscopy on BCN nanofilm. (b) SFG spectra of the BCN nanofilm in air, prewetted by pure water, and water containing NaCl with concentrations of 0.5 wt%,1 wt%, and 2 wt%. (c) Snapshot of the simulation system composed by BCN nanofilm (signed as green), water molecules (signed as yellow spheres) and Na+ ions (signed as blue spheres) after 20 ns simulation. (d) Enlarged MD simulated distribution of water molecules and Na+ ions around BCNs. (e) PMF between the BCN nanofilm and water with and without NaCl.

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