Metal-organic framework UiO-66 membranes

doi:10.1007/s11705-019-1857-5

Front. Chem. Sci. Eng.

2020, Vol. 14

Issue (2) : 216-232 https://doi.org/10.1007/s11705-019-1857-5

REVIEW ARTICLE

Metal-organic framework UiO-66 membranes

Xinlei Liu(

)

Catalysis Engineering, Department of Chemical Engineering, Delft University of Technology, 2629 HZ Delft, The Netherlands

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Abstract

Metal-organic frameworks (MOFs) have emerged as a class of promising membrane materials. UiO-66 is a prototypical and stable MOF material with a number of analogues. In this article, we review five approaches for fabricating UiO-66 polycrystalline membranes including in situ synthesis, secondary synthesis, biphase synthesis, gas-phase deposition and electrochemical deposition, as well as their applications in gas separation, pervaporation, nanofiltration and ion separation. On this basis, we propose possible methods for scalable synthesis of UiO-66 membranes and their potential separation applications in the future.

Keywords membrane metal-organic framework UiO-66 separation

Corresponding Author(s): Xinlei Liu

Just Accepted Date: 18 September 2019 Online First Date: 19 November 2019 Issue Date: 24 March 2020

Cite this article:

Xinlei Liu. Metal-organic framework UiO-66 membranes[J]. Front. Chem. Sci. Eng., 2020, 14(2): 216-232.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-019-1857-5
https://academic.hep.com.cn/fcse/EN/Y2020/V14/I2/216

Fig.1 (a) The unit cell of UiO-66 constructed with Zr₆ cluster and BDC ligand. (b) The structure of UiO-66 cavities and aperture. The size of cavities and aperture is estimated from the largest spheres which may fit them. (c) Possible tetravalent metal ions for preparing UiO-66 type MOFs. (d) Possible BDC type ligands for constructing UiO-66 type MOFs. Ligands labeled in blue indicate their corresponding MOFs have been reported. Reproduced from [²⁸] and [²⁹] with permission, copyright American Chemical Society, 2015 and Royal Chemical Society, 2015.

Fig.2 (a) Schematic diagram showing in situ synthesis of UiO-66 membranes on YSZ substrate. Scanning electron microscopy (SEM) images of UiO-66 membranes via in situ synthesis on α-alumina hollow fibers (b), YSZ hollow fibers (c), EDXS mapping image, C signal, yellow; Y signal, green), micropatterned YSZ sheets (d) and nanochanneled PET films (scale bar 100 nm) (e). Reproduced from [²⁸,⁸⁶–⁸⁸] with permission, copyright John Wiley and Sons 2017, 2018; American Chemical Society, 2015; the American Association for the Advancement of Science, 2018.

Fig.3 (a) SEM images ((1) surface; (2) cross section) of the UiO-66 membrane prepared by secondary growth and scheme (3) of the octahedrons’ orientation within the UiO-66 membrane and their orientation to the substrate surface; (b) photograph (1) and SEM image (2) of 2D monolayer UiO-66 on a water surface and a silicon platform, respectively; cross-sectional SEM images (3) and the corresponding X-ray diffraction (XRD) patterns (4) of silicon platform-supported UiO-66 films comprising one, two, and three monolayers of microcrystals prepared by repetition of the transfer process using self-assembly; (c) SEM images (1) surface; (2) cross section) of UiO-66 film prepared by three repeated solvothermal syntheses and the corresponding XRD patterns (3). Reproduced from [⁹⁵,¹⁰⁵,¹¹⁷] with permission, copyright American Chemical Society, 2017; John Wiley and Sons 2013; Royal Chemical Society 2015.

Fig.4 Schematic illustrations of (a) terminated and enabled intergrowth of UiO-66 crystals based on ligand deprotonation and (b) the biphase system to synthesize UiO-66 membranes and films. Reproduced from [⁹⁶] with permission, copyright American Chemical Society, 2018.

Fig.5 Fabrication of UiO-66 related films via gas-phase deposition. (a) Deposition of UiO-66 films by all-gas phase process: (1) experimental setup for post-treatment of the hybrid films with acetic acid vapor; XRD patterns (2) and cross-sectional SEM images (3) of the UiO-66 film after the treatment with acetic acid. (b) Schematic diagram of the vapor-assisted conversion process for the fabrication of (111)-oriented UiO-66-NH₂ films. ZrOCl₂, BDC-NH₂, and the modulator acetic acid (if desired) were dissolved in DMF giving the precursor solution on top of the substrate; a mixture of DMF and acetic acid giving the vapor source at the bottom of the vessel. Reproduced from [¹⁰⁶,¹⁰⁸] with permission, copyright Springer Nature, 2016 and American Chemical Society, 2018.

Fig.6 Schematic illustration of the anodic and cathodic electrochemical deposition mechanisms for UiO-66 films. Reproduced from [¹¹⁰] with permission, copyright American Chemical Society, 2015.

Materials	Substrates	Synthetic approaches	Applications	Ref.
UiO-66	α-Alumina hollow fibers	In situ synthesis (Zr⁴⁺/BDC/H₂O/DMF= 1:1:1:500, 72 h, 120°C)	Nanofiltration (K⁺, Na⁺, Ca²⁺, Mg²⁺, Al³⁺, Cl^–, H₂O) Gas separation (H₂, CO₂, N₂, CH₄)	[²⁸]
UiO-66	YSZ hollow fibers	In situ synthesis (Zr⁴⁺/BDC/H₂O/DMF= 1:1:1:500, 48 h, 120°C)	Pervaporation (furfural, THF, acetone, i-butanol, n-butanol, propanol, ethanol, water)	[⁸⁶]
UiO-66	Micro-patterned YSZ discs	In situ synthesis (Zr⁴⁺/BDC/H₂O/DMF= 1:1:1:500, 48 h, 120°C)	Pervaporation (n-butanol, water)	[⁸⁷]
UiO-66	Channeled PET	In situ synthesis (Zr⁴⁺/BDC/DMF= 1:1:500, 24 h, 100°C)	Electro-chemical ion separation (Li⁺, Na⁺, K⁺, Rb⁺)	[⁸⁸]
UiO-66-NH₂	ZrO₂ modified alumina tubes	In situ synthesis (modified substrates) (Zr⁴⁺/BDC-NH₂/H₂O/CH₃COOH/DMF= 1:1:1:150:500, 48 h, 120°C)	Pervaporation (thiophene, n-octane)	[⁹⁰]
UiO-66-NH₂	APTES modified α-alumina tubes	In situ synthesis (modified substrates) (Zr⁴⁺/BDC-NH₂/H₂O/DMF= 1:1:1:500, 24 h, 120°C)	Pervaporation (Na⁺, K⁺, Ca²⁺, Mg²⁺, NH⁴⁺, F^–, Cl^–, and NO^3–, H₂O)	[⁸⁹]
UiO-66	α-alumina tubes	Secondary growth (Zr⁴⁺/BDC/H₂O/CH₃COOH/DMF= 1:1:1:500:x, x = 750, 1000, 1500, 24 h, 120°C, repeated three times)	Pervaporation (Methanol, ethanol, acetone, water, xylene, trimethylbenzene) Gas separation (H₂, CO₂, N₂)	[⁹¹]
UiO-66-CH₃	Porous Ni sheets	Secondary growth (Zr⁴⁺/BDC-CH₃/CH₃COOH/DMF= 1:1:30:430, 24 h, 120°C)	Gas separation (CO₂, N₂)	[⁹²]
UiO-66	α-Alumina tubes	Secondary growth (Zr⁴⁺/BDC-NH₂/H₂O/CH₃COOH/DMF= 1:1:1:150:500, 72 h, 120°C)	Pervaporation (methanol, methyl tert-butyl ether)	[⁹³]
UiO-66-(OH)₂	α-Alumina hollow fibers	Secondary growth (Zr⁴⁺/ODBDC/HCOOH/DMF= 1:1:100:500, 72 h, 120°C)	Nanofiltration (Fe³⁺, Cr³⁺, Zn²⁺, Mg²⁺, Na⁺, Cl^–, H₃BO₃, methyl blue, H₂O)	[⁹⁴]
UiO-66	α-Alumina discs	Secondary growth (Zr⁴⁺/BDC/Benzoic acid/DMF= 1:1:20:100, 24 h, 180°C)	Gas separation (H₂, CO₂, N₂, CH₄, C₂H₆, C₃H₈)	[⁵⁹,⁹⁵]
UiO-66	Anodic aluminum oxide, AAO	Secondary growth (Zr⁴⁺/BDC/H₂O/DMF= 1:1:1:500, 72 h, 120°C)	Gas separation (H₂, CO₂, N₂, CH₄)	[¹²⁶]
UiO-66	α-Alumina discs	Biphase synthesis DMF phase: 15 mL, Zr/BDC/HCOOH/DMF= 1:0.5:125:130, and 1:0.7:125:130, Hexane phase: 1836 mg TEA in 15 mL hexane, 24 h, 120°C	Gas separation (CO₂, N₂)	[⁹⁶]

Tab.1 Summary of UiO-66 type membranes in terms of substrates, synthetic approaches and applications

Materials	Substrates	Synthetic approaches	Applications	Ref.
UiO-66	BDC functionalized FTO glasses	In situ synthesis (modified substrate) (Zr⁴⁺/BDC/CH₃COOH/DMF= 1:1:96:520, 24 h, 120°C)	Cyclic voltammetry ion separation (Ru(NH₃)₆³⁺, Fe(phen)₃²⁺, Fe(CN)₆³⁺)	[⁹⁹]
UiO-66-SO₃H-NH₂	PDA-coated PU foams	In situ synthesis (modified substrate) (Zr⁴⁺/BDC-SO₃H/BDC-NH₂/H₂O/CH₃COOH= 1:0.75:0.25:230:100)	Catalysis (from glucose to HMF)	[¹⁰⁰]
UiO-66	ZrO₂ fibrous mats	In situ synthesis (ZrO₂/BDC/CH₃COOH/H₂O= 1:3.7:2.2:686)	Not reported	[¹⁰¹]
UiO-66-NH₂	ATA modified PAN fibers	In situ synthesis (modified substrate) (Zr⁴⁺/BDC-NH₂/acetone= 1:1:200)	Chlorine adsorption	[¹⁰²]
UiO-66	Silanized a-alumina and ob-SiC foams	In situ synthesis (modified substrate) (Zr⁴⁺/BDC//DMF= 1:0.9:380, 24 h, 120°C)	Not reported	[¹⁰³]
UiO-66	Stainless meshes	Secondary growth (Zirconium propoxide/BDC/DMF, 12 h, RT)	Oil-water separation (diesel, vegetable oil, pump oil, cyclohexane, water)	[¹⁰⁴]
UiO-66	Si discs	Secondary growth (Zr⁴⁺/BDC/H₂O/CH₃COOH/DMF= 1:1:1:0/500:1500, 24 h, 120°C, repeated three times)	Not reported	[¹⁰⁵]
UiO-66	Si discs	Gas-phase deposition (ZrCl₄ (165°C), BDC (220°C), CH₃COOH (RT), N₂; post treatment: 160°C CH₃COOH, 24 h)	Not reported	[¹⁰⁶]
UiO-66-NH₂	Si discs	Gas-phase deposition (ZrCl₄ (165°C), BDC-NH₂ (225°C), N₂; post treatment: 160°C CH₃COOH, 24 h)	Not reported	[¹⁰⁷]
UiO-66-NH₂ (UiO-66)	Gold, Si discs	Vapor-assistant conversion (Precursor solution: ZrOCl₂•8H₂O+ BDC-NH₂ (BDC) + CH₃COOH+ DMF Vapor source: DMF+ CH₃COOH, 100°C, 3 h)	Ethanol adsorption	[¹⁰⁸]
UiO-66	FTO glasses	Electrophoretic deposition (10 mg UiO-66 particles in 20 mL toluene, DC voltage of 90 V)	Not reported	[¹⁰⁹]
UiO-66	Zirconium foil	Electrochemical deposition (BDC:HNO₃:H₂O:CH₃COOH:DMF= 1:2:4:5/10/50:130, 80 mA, 110°C)	Sorbent trap (Toluene)	[¹¹⁰]
UiO-66	Free-standing	Biphase synthesis DMF phase: 5 mL, Zr/BDC/HCOOH/DMF = 1:0.25:87.5:130, 1:0.25:100:130, 1:0.25:118:130, 1:0.4:125:130, 1:0.5:125:130, 1:0.7:125:130, 1:0.6:150:130, 1:0.84:150:130 Hexane phase: 612 mg TEA in 5 mL hexane, 120°C, 24 h	Not reported	[⁹⁶]
UiO-66	Cellulose supports	Filtration (UiO-66 particles in water)	Nanofiltration (methylene blue, water)	[¹¹¹]
UiO-66	Silicon wafers	Solution shearing (UiO-66 particles in DMF/H₂O/MeOH)	Not reported	[¹¹²]
UiO-66	Silicon platform	Self-assembly (PVP modified UiO-66 in ethanol/water solution containing sodium dodecyl sulfate)	Not reported	[¹¹⁷]

Tab.2 Summary of UiO-66 films in terms of substrates, synthetic approaches and applications

Fig.7 (a) Single component permeation data of UiO-66 membranes at 293 K with 1 bar pressure difference; (b) H₂ mixed binary permeation data of (002) oriented UiO-66 membrane at 298 K and 1 bar (absolute pressure) in both feed and sweep sides. Reproduced from [²⁸,⁹⁵] with permission, copyright American Chemical Society, 2015 and 2017.

Fig.8 (a) Flow chart and pervaporative organic (n-butanol and furfural) dehydration performance of UiO-66 membranes during on-stream activation and stability test processes at 30°C with 5 wt-% water in the feed; (b) thiophene/n-octane separation performance of UiO-66-NH₂ membrane and a comparison with polymers. Reproduced from [⁸⁶,⁹⁰] with permission, copyright John Wiley and Sons 2017, and Elsevier 2018.

Fig.9 (a) Desalination performance of the UiO-66 membrane for KCl, NaCl, CaCl₂, MgCl₂ and AlCl₃ aqueous solutions with a concentration of 0.20 wt-% at 20°C under a pressure difference of 10.0 bar; (b) separation performance of the UiO-66-(OH)₂ membrane before and after PSDH under a pressure difference of 3 bar with 2000 ppm NaCl and 100 ppm methyl blue aqueous solutions; (c) scheme of PSDH by relinking. Reproduced from [²⁸,⁹⁴] with permission, copyright American Chemical Society, 2015 and 2017.

Fig.10 (a) Ion selectivity over the pore diameter of MOF and porous membranes; (b) cyclic voltammograms of Ru(NH₃)₆³⁺/Fe(phen)₃²⁺ mixture in aqueous solutions on MOF-coated electrode treated with PDMS (red solid lines) and bare FTO electrode (black dashed lines). Reproduced from [⁸⁸,⁹⁹] with permission, copyright American Association for the Advancement of Science 2018, and John Wiley and Sons 2016.

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