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Multivariate Polycrystalline Metal-Organic Framework Membranes for CO₂/CH₄ Separation.

Weidong Fan¹, Yunpan Ying¹, Shing Bo Peh¹

¹Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, 117585 Singapore.

Journal of the American Chemical Society

|October 5, 2021

Summary

This study introduces advanced MIL-160 membranes for natural gas separation, offering improved selectivity and permeance for CO2/CH4. These novel membranes demonstrate enhanced resistance to moisture and hydrocarbons compared to traditional silicoaluminophosphate-34 membranes.

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Area of Science:

Materials Science
Chemical Engineering
Separation Technology

Background:

Membrane technology offers energy-efficient natural gas separation.
Microporous inorganic membranes like silicoaluminophosphate-34 (SAPO-34) show promise but suffer from moisture and hydrocarbon adsorption.
Developing robust membranes resistant to contaminants is crucial for industrial natural gas processing.

Purpose of the Study:

To fabricate and characterize a novel MIL-160 membrane for natural gas separation.
To investigate the effect of pore size and ligand functionality on membrane performance using reticular chemistry.
To evaluate the performance of fluorine-functionalized MIL-160/CAU-10-F membranes and compare them with existing SAPO-34 membranes.

Main Methods:

In situ hydrothermal synthesis of polycrystalline MIL-160 membranes on an Al2O3 substrate.
Fabrication of fluorine-functionalized MIL-160/CAU-10-F membranes.
Gas separation performance testing, including CO2/CH4 selectivity and CO2 permeance measurements.
Evaluation of membrane resistance to water vapor and hydrocarbons.

Main Results:

A 3 μm thick MIL-160 membrane exhibiting a significant molecular sieving effect was successfully fabricated.
Reticular chemistry allowed precise control over the MIL-160 membrane's pore size and environment.
The fluorine-functionalized MIL-160/CAU-10-F membrane showed a 10.7% increase in CO2/CH4 selectivity and a 31.2% increase in CO2 permeance compared to MIL-160.
Both MIL-160 and MIL-160/CAU-10-F membranes demonstrated superior resistance to water vapor and hydrocarbons over SAPO-34 membranes.

Conclusions:

MIL-160 membranes are effective for natural gas separation with tunable properties via reticular chemistry.
Fluorine-functionalization enhances CO2/CH4 separation performance and CO2 permeance.
These novel hydrophobic membranes offer improved stability and performance in the presence of contaminants, outperforming hydrophilic SAPO-34 membranes.