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Carbon molecular sieve membranes (CMSMs) incorporating metal-organic polyhedra (MOP-18) exhibit enhanced CO2/CH4 separation performance and stability. These pillared CMSMs surpass the 2019 Robeson upper bound, outperforming non-pillared membranes.

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Polymer Science

Background:

  • High free volume polyimides like BTDA-BAF offer potential for gas separation membranes.
  • Polyimide-derived carbon molecular sieve membranes (CMSMs) often suffer from pore collapse and aging, limiting their performance.
  • Achieving high permeability and selectivity simultaneously remains a challenge in membrane technology.

Purpose of the Study:

  • To develop robust carbon molecular sieve membranes (CMSMs) with improved gas separation performance and stability.
  • To investigate the effect of incorporating metal-organic polyhedra (MOP-18) on the structure and properties of CMSMs.
  • To evaluate the CO2/CH4 separation capabilities and aging resistance of the developed membranes.

Main Methods:

  • Synthesis of BTDA-BAF polyimide via polycondensation.
  • Preparation of CMSMs by carbonizing BTDA-BAF and MOP-18/BTDA-BAF composites at 550 °C.
  • Characterization of membrane structure, including pore collapse and graphitic sheet integrity.
  • Gas permeation testing for CO2 and CH4 to determine permeability and selectivity.
  • Evaluation of membrane aging over time.

Main Results:

  • MOP-18 incorporation and subsequent copper nanoparticle formation prevented pore collapse and membrane aging.
  • Pillared CMSMs achieved high CO2 permeability (12,729 Barrer) and CH4 permeability (659 Barrer) with a CO2/CH4 selectivity of 19.3.
  • The permselectivity of MOP-18/BTDA-BAF CMSMs reached the 2019 Robeson upper bound.
  • Pure BTDA-BAF CMSMs showed lower performance (5337 Barrer CO2, 573 Barrer CH4, 9.3 selectivity) and aged significantly faster.

Conclusions:

  • Metal-organic polyhedra-pillared carbon molecular sieve membranes offer superior CO2/CH4 separation performance and enhanced stability.
  • The use of MOP-18 effectively mitigates pore collapse and aging in CMSMs, leading to sustained high permselectivity.
  • These advanced CMSMs represent a promising direction for efficient natural gas purification and carbon capture technologies.