Supporting Information

for Adv. Sustainable Syst., DOI 10.1002/adsu.202300597

Mixed-Dimensional Membranes with Double 0D@2D Structures Enable Efficient and

Sustainable Water Treatment

Zixin Zhang, Huaqiang Fu, Zhe Wang*, Wei Qian, Xin Zhao, Yunfa Si, Jiannan Guo, Shaowen
Cao and Daping He
Supporting Information for

Mixed-dimensional membranes with double

0D@2D structures enable efficient and
sustainable water treatment
Zixin Zhang,‡ Huaqiang Fu,‡ Zhe Wang,* Wei Qian, Xin Zhao, Yunfa Si, Jiannan Guo,
Shaowen Cao, and Daping He

Z. Zhang, Z. Wang, S. Cao

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing
Wuhan University of Technology
Wuhan 430070, P. R. China
E-mail: wangzhe0614@whut.edu.cn

H. Fu, Y. Si, D. He
School of Materials Science and Engineering
Wuhan University of Technology
Wuhan 430070, P. R. China

W. Qian, X. Zhao, J. Guo, D. He

Hubei Engineering Research Center of Radio Frequency Microwave Technology and
Application
Wuhan University of Technology
Wuhan 430070, P. R. China

‡
These authors contributed equally

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 Structural characterizations: Field-emission scanning electron microscopy (JSM-
7610F Plus) was used to image the surface and cross-section morphologies of the
membranes. Elemental mappings were conducted using energy dispersive X-ray
spectroscopy (EDS). The TEM images were taken with a high-resolution transmission
electron microscopy (JEM-1400 Plus). Optical microscopy was performed using a
NewView7100 microscope. XRD patterns were taken with X-ray diffractometer
(Rigaku Smartlab) with Cu Kα radiation. XPS spectra were obtained using X-ray
energy spectroscopy (ESCALAB 250Xi). The water contact angle tests were carried
out using an automatic contact angle measuring instrument (OCA35). The
concentrations of feed and filter solution were determined by ultraviolet/visible (UV-
vis) spectrophotometer (Shimadzu UV-1800).

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Figure S1. a) Top-view SEM image and b–e) corresponding elemental mappings of
SiO2@GO/TiO2@MXene-2 (SGTM-2) membrane surface.

The Si and Ti elements are uniformly distributed on the surface of SGTM-2

membrane.

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Figure S2. a) Digital images of the SGTM composite membrane before and after drying.
b) Digital images of the TiO2@MXene (TM) membrane before and after drying.

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Figure S3. a-b) Digital images of the SGTM composite membrane when bent.

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Figure S4. a) TEM image of the SiO2@GO (SG). b) Size distribution of SiO2
nanoparticles in SG membrane.

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Figure S5. SEM images of a) the MAX phase and b) multilevel MXene.

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Figure S6. a-c) SEM images of TM-1, TM-2 and TM-3. d-f) Size distribution of TiO2
nanoparticles in TM.

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Figure S7. a) Top-view SEM image and b–d) corresponding elemental mappings of

TM membrane surface.

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Figure S8. XRD spectra of all composite membranes.

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Figure S9. a) Cross-sectional SEM image and b-e) corresponding elemental mapping
images of SGTM-2 membrane.

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Figure S10. (a) The surface roughness and (b) typical height profiles of membranes
measured by optical profilometry.

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Figure S11. a) Water contact angles and b) water permeance under −0.08MPa of the
prepared membranes. c) Dye rejection ratios of the prepared membranes toward MB,
RhB, and MO.

The number of functional groups on TM grew with the increasing of hydrothermal

oxidation time, thus leading to a descending order of hydrophilicity: SGTM-3 > SGTM-
2 > SGTM-1 (Figure S11a).
Considering that the amount of SG used in each membrane was the same, the
increased water flux indicated that the intercalation of TM into SG increased interlayer
spacing and provided more nano channels, facilitating the transportation of water
molecules (Figure S11b). With the further increase of mass ratios of TiO2 to MXene,
the declination of water flux may result from the overloading of TiO2 nanoparticles on
MXene nanosheets, which occupied more interlayer space and reduced available
nanochannels.

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Figure S12. The stability of SGTM-2 membranes in aqueous solution at (a-c) pH=2,
(d-f) pH=7 and (h-i) pH=11 for three, seven and fourteen days, respectively.

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Figure S13. XRD spectra of SGTM membrane (a) and TM (b) before and after being
soaked in water for three days.

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Figure S14. a–c) UV-vis spectra of methylene blue (MB), rhodamine B (RhB) and
methyl orange (MO) dye solutions before and after filtering using SGTM-2 membranes
under −0.08 MPa.

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Figure S15. a–c) UV-vis spectra of RhB, MB and MO solutions with different
concentrations. d–f) The fitted calibration curves of dye concentrations as a function of
UV-vis absorption at characteristic wavelength.

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Figure S16. a) Photocatalytic degradation efficiency of MB by different samples of
SGTM-1, 2 and 3 membranes. b) The apparent reaction rate constants.

It can be seen that the MB photocatalytic degradation efficiency of SGTM-2

membrane was superior to others, and the reaction rate constant of SGTM-2 membrane
was the largest.

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Figure S17. UV-vis spectra of MB solution with different illumination times of the
membranes.

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Figure S18. The detailed information about the MB rejection and water permeance
recovery of SGTM-2 membrane.

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Table S1. The three dye molecule solutions of different sizes and charges.
Molecular
Name Acronym Charge Formula
weight

Methyl blue MB 799.80 + C15H17ClN4

Rhodamine B RhB 479.01 + C28H31ClN2O3

Methyl Orange MO 327.33 - C14H14N3NaO3S

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Table S2. Comparison of water performance and pollutant rejection of composite
membranes containing GO, MXene and both GO and MXene.
Composite membranes Water Pollutant Ref
performance rejection
(L m-2 h-1 rate (%)
bar-1)
rGO/PDA/g-C3N4 75 99.8 S1
PAA@NM88B/GO 68.21 97 S2
rGO/AgNP@g-C3N4 210.9 92.7 S3
GO
GO/M88A 30.6 97.87 S4
GO 130 99 S5
prGO/Ag/M88A 189 99.7 S6
MXene/COF 169.3 98 S7
ZnO@MXene 138.81 95.44 S8
MXene
MXene@CS/MCN 71.7 98 S9
MXene/Al2O3 88.8 99.5 S10
GO/PAA/g-C3N4/MXene 38.69 99 S11
GO/TiO2@MXene 89.6 97 S12
r-HGO/MXene 121 90 S13
MXene and rPGO-MXene 198.8 100 S14
GO GO/MXene 71.9 99.5 S15
GO/MXene-PPS 45.78 99.99 S16
GO/MXene 79.58 99 S17
SiO2@GO/TiO2@MXene 2114 96.3 this work
Note:
PDA: polydopamine;
PAA: polyacrylic acid
NM88B: NH2-MIL-88B(Fe)
AgNP: Ag nanoparticle
M88A: MIL-88A(Fe)
prGO: partially reduced graphene oxide
COF: covalent organic framework
CS: chitosan
MCN: g-C3N4/PVDF
r-HGO: reduced-holy GO
rPGO: reduced porous GO
PPS: polyphenylene sulfide

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Reference
[S1] F. Li, Z. Yu, H. Shi, Q. Yang, Q. Chen, Y. Pan, G. Zeng, L. Yan, Chem. Eng. J.
2017, 322, 33.
[S2] Y. Gao, S. Yan, Y. He, Y. Fan, L. Zhang, J. Ma, R. Hou, L. Chen, J. Chen, J.
Membr. Sci. 2021, 626, 119192.
[S3] C. Chen, L. Chen, X. Zhu, B. Chen, Chem. Eng. J. 2022, 441, 136089
[S4] A. Xie, J. Cui, J. Yang, Y. Chen, J. Lang, C. Li, Y. Yan, J. Dai, Appl. Catal., B
2020, 264, 118548.
[S5] R. Yue, T. Chen, Z. Ye, B. Barbeau, M. S. Rahaman, J. Water Process. Eng.
2021, 44, 102443.
[S6] R. Yue, B. Raisi, J. Rahmatinejad, Z. Ye, B. Barbeau, M. S. Rahaman, J. Colloid
Interface Sci. 2021, 604, 458.
[S7] X. Gong, G. Zhang, H. Dong, H. Wang, J. Nie, G. Ma, J. Membr. Sci. 2022, 657,
120667.
[S8] Y. Li, H. Luo, W. Ji, S. Li, P. Nian, N. Xu, N. Ye, Y. Wei, Sep. Purif. Technol.
2023, 323, 124420.
[S9] Q. Lin, G. Zeng, S. Pu, G. Yan, J. Luo, Y. Wan, Z. Zhao, Chem. Eng. J. 2022,
443, 136335.
[S10] Q. Long, S. Zhao, J. Chen, Z. Zhang, G. Qi, Z.-Q. Liu, J. Membr. Sci. 2021, 635,
119464.
[S11] W. Tu, Y. Liu, M. Chen, L. Ma, L. Li, B. Yang, Sep. Purif. Technol. 2022, 296,
121398.
[S12] R. Han, P. Wu, J. Mater. Chem. A 2019, 7, 6475.
[S13] J. Hou, S. Guo, N. Graham, W. Yu, K. Sun, T. Liu, J. Membr. Sci. 2024, 691,
122216.
[S14] S. Li, J. Lu, D. Zou, L. Cui, B. Chen, F. Wang, J. Qiu, T. Yu, Y. Sun, W. Jing,
Chem. Eng. J. 2023, 457, 141217.
[S15] T. Liu, X. Liu, N. Graham, W. Yu, K. Sun, J. Membr. Sci. 2020, 593, 117431.
[S16] X.-Y. Ma, T.-T. Fan, G. Wang, Z.-H. Li, J.-H. Lin, Y.-Z. Long, Compos.
Commun. 2022, 29, 101017.
[S17] D. Yu, L. Sun, Y. Zhang, Y. Song, C. Jia, Y. Wang, Y. Wang, M. J. Kipper, J.
Tang, L. Huang, Chem. Eng. J. 2024, 480, 148009.

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