Conspectus
Climate change due to anthropogenic carbon dioxide emissions (e.g.,
combustion of fossil fuels) represents one of the most profound environmental
disasters of this century. Equipping power plants with carbon capture
and storage (CCS) technology has the potential to reduce current worldwide
CO2 emissions. However, existing CCS schemes (i.e., amine
scrubbing) are highly energy-intensive. The urgent abatement of CO2 emissions relies on the development of new, efficient technologies
to capture CO2 from existing power plants. Membrane-based
CO2 separation is an attractive technology that meets many
of the requirements for energy-efficient industrial carbon capture.
Within this domain, thin-film composite (TFC) membranes are particularly
attractive, providing high gas permeance in comparison with conventional
thicker (∼50 μm) dense membranes. TFC membranes are usually
composed of three layers: (1) a bottom porous support layer; (2) a
highly permeable intermediate gutter layer; and (3) a thin (<1
μm) species-selective top layer. A key challenge in the development
of TFC membranes has been to simultaneously maximize the transmembrane
gas permeance of the assembled membrane (by minimizing the gas resistance
of each layer) while maintaining high gas-specific selectivity.
In this Account, we provide an overview of our recent development
of high-performance TFC membrane materials as well as insights into
the unique fabrication strategies employed for the selective layer
and gutter layer. Optimization of each layer of the membrane assembly
individually results in significant improvements in overall membrane
performance. First, incorporating nanosized fillers into the selective
layer (poly(ethylene glycol)-based polymers) and reducing its thickness
(to ca. 50 nm) through continuous assembly of polymers technology
yields major improvements in CO2 permeance without
loss of selectivity. Second, we focus on optimization of the middle
gutter layer of TFC membranes. The development of enhanced gutter
layers employing two- and three-dimensional metal–organic framework
materials leads to considerable improvements in both CO2 permeance and selectivity compared with traditional poly(dimethylsiloxane)
materials. Third, incorporation of a porous, flexible support layer
culminates in a mechanically robust high-performance TFC membrane
design that exhibits unprecedented CO2 separation performance
and holds significant potential for industrial CO2 capture.
Alternative strategies are also emerging, whereby the selective layer
and gutter layer may be combined for enhanced membrane efficiency.
This Account highlights the CO2 capture performance, current
challenges, and future research directions in designing high-performance
TFC membranes.