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Preparation of heteroatom isomorphously substituted MEL zeolite membranes for pervaporation separation of dimethylformamide/water mixtures

  • Materials (Organic, Inorganic, Electronic, Thin Films)
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Abstract

The recovery of dimethylformamide (DMF) by pervaporation is less energy intensive and more economical than the traditional distillation method. High/pure silica zeolite is a typical organics perm-selective material for pervaporation membrane due to its hydrophobic nature, demonstrating great potential for recovering organic components from aqueous solutions. In this study, as an attempt to further enhance the membrane hydrophobicity, titanium and zirconium-substituted MEL type zeolite membranes (Ti-silicalite-2 and Zr-silicalite-2) were synthesized on the α-Al2O3 discs by a secondary growth method. X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FTIR) results confirmed the isomorphous substitution of the MEL framework by Ti and Zr atoms. The effects of isomorphous substitution, feed temperature and concentration on the DMF recovery performance were investigated via systematically designed pervaporation experiments. The fluxes and separation factors both increased with the isomorphous substitution of heteroatom, as well as increasing feed temperature and decreasing feed concentration. The Ti-silicalite-2 membrane exhibited a high separation factor of 6.4 with a total flux of 0.98 kg·m−2·h−1 for a 5 wt% DMF/water feed at 343 K.

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Abbreviations

A:

effective membrane area [m2]

d:

spacing between the planes in the atomic lattice [Å]

J:

permeate flux [kg·m−2·h−1]

Kf :

Freundlich constant [-]

M:

weight of the permeate [kg]

n:

Freundlich constant [-]

p:

adsorbate pressure [mbar]

qe :

equilibrium adsorption capacity [mmol·g−1]

R2 :

correlation coefficient [-]

t:

time [h]

v:

unit cell volume [Å3]

X:

mass fraction of feed [-]

Y:

mass fraction of permeate [-]

α:

separation factor [-]

θ:

X-ray diffraction angle [°]

λ:

wavelength[nm]

BEA:

Beta-Type

CHA:

chabazite

DMF:

dimethylformamide

FAU:

faujasite

FT-IR:

Fourier transform infrared

GC:

gas chromatography

IGA:

intelligent gravimetric analyzer

LTA:

Linde-Type A

MEL:

Mobil eleven

MFI:

Mobil five

MOR:

mordenite

MW:

microwave

NaA:

Natrium A

SEM:

scanning electron microscopy

TBAOH:

tetrabutylammonium hydroxide

TBOT:

tetrabutyl titanate

TEOS:

tetraethylorthosilicate

XRD:

X-ray diffraction

ZBOT:

zirconium n-butoxide

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Acknowledgement

This work was supported by Natural Science Foundation of Jiangsu Province (BK20200982), Natural Science Foundation of the Jiangsu Higher Education Institutions of China (18KJA530001), Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and State Key Laboratory of Materials-Oriented Chemical Engineering.

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Authors and Affiliations

  1. National & Local Joint Engineering Research Center of Biomass Refining and High-Quality Utilization, Institute of Urban & Rural Mining, Changzhou University, Changzhou, 213164, China

    Qigang Wu & Zhengzhong Zhou

  2. Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou, 213164, China

    Rong Xu, Hui Shao, Jing Zhong & Xiuxiu Ren

Authors
  1. Qigang Wu
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  2. Rong Xu
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  3. Hui Shao
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  4. Jing Zhong
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  5. Xiuxiu Ren
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  6. Zhengzhong Zhou
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Correspondence to Jing Zhong.

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Preparation of heteroatom isomorphously substituted MEL zeolite membranes for pervaporation separation of dimethylformamide/water mixtures

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Wu, Q., Xu, R., Shao, H. et al. Preparation of heteroatom isomorphously substituted MEL zeolite membranes for pervaporation separation of dimethylformamide/water mixtures. Korean J. Chem. Eng. 38, 2150–2156 (2021). https://doi.org/10.1007/s11814-021-0839-8

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  • DOI: https://doi.org/10.1007/s11814-021-0839-8

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