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Recent Developments in High-Performance Membranes for CO2 Separation

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Recent Developments in High-Performance Membranes for CO2 Separation membranes Perspective Recent Developments in High-Performance Membranes for CO2 Separation Zi Tong 1,2,* and Ali K. Sekizkardes 1,3,* 1 National Energy Technology Laboratory, U.S. Department of Energy, 626 Cochrans Mill Road, Pittsburgh, PA 15236, USA 2 Oak Ridge Institute for Science and Education, Pittsburgh, PA 15236, USA 3 Leidos Research Support Team, 626 Cochrans Mill Road, P.O. Box 10940, Pittsburgh, PA 15236, USA * Correspondence: [email protected] (Z.T.); [email protected] (A.K.S.) Abstract: In this perspective article, we provide a detailed outlook on recent developments of high-performance membranes used in CO2 separation applications. A wide range of membrane materials including polymers of intrinsic microporosity, thermally rearranged polymers, metal– organic framework membranes, poly ionic liquid membranes, and facilitated transport membranes were surveyed from the recent literature. In addition, mixed matrix and polymer blend membranes were covered. The CO2 separation performance, as well as other membrane properties such as film flexibility, processibility, aging, and plasticization, were analyzed. 1. Introduction Despite the remarkable renewable energy capacities being operated around the world, global CO2 concentrations continue to rise. A set of transformational carbon capture, Citation: Tong, Z.; Sekizkardes, A.K. utilization, and storage (CCUS) technologies are urgently needed that can prevent CO2 Recent Developments in from entering the atmosphere, use the captured CO2 for downstream applications, and High-Performance Membranes for safely and permanently store it deep under the ground [1]. Membrane gas separation CO2 Separation. Membranes 2021, 11, technology has been believed to be one of the most promising technologies to replace the 156. https://doi.org/10.3390/ traditional technologies such as amine scrubbing, due to its small footprint, simplicity, membranes11020156 and high energy efficiency. To overcome the challenges in lowering carbon capture cost or profitable carbon capture, a membrane material will need to be on or above the Robeson Academic Editor: Klaus Rätzke Upper Bound, i.e., in the high permeability/moderate selectivity regime [2]. The state-of- the-art membranes utilized in industry are heavily dependent on conventional membrane Received: 27 January 2021 materials such as cellulose acetate, polysulfone, polydimethylsiloxane, polyethylene oxide, Accepted: 19 February 2021 etc. Applications of these gas separation membranes are clustered around hydrogen Published: 23 February 2021 recovery and nitrogen separation, methane reforming, and vapor recovery [3]. On the other hand, current CO separation membranes have been relatively less preferred and did not Publisher’s Note: MDPI stays neutral 2 surpass the cost efficiency of conventional CO separation technologies such as solvents and with regard to jurisdictional claims in 2 published maps and institutional affil- sorbents. Recent studies suggested that the CO2 permeability for a potential membrane iations. candidate should be at least two orders of magnitude larger than the permeability of conventional membranes to break through [4]. The high CO2 permeability should be also complemented with adequate selectivity over other gases, such as nitrogen, in gas mixtures. Therefore, there is a clear need for more advanced membrane materials to be used CO2 separation. Recently, a growing amount of interest has been concentrated in advanced Copyright: © 2021 by the authors. membrane materials to achieve cost-efficient CO separation. A large body of literature Licensee MDPI, Basel, Switzerland. 2 has been accumulated in the past decade covering these high-performance membranes. This article is an open access article distributed under the terms and Accordingly, several new classes of advanced membrane materials have been introduced. conditions of the Creative Commons Membranes include polymers of intrinsic micro porosity (PIMs) [5], thermally rearranged Attribution (CC BY) license (https:// (TR) polymers [6], polyethylene oxide (PEO)-based copolymers [7], poly ionic liquids [8] creativecommons.org/licenses/by/ and facilitated transport membranes [9]. In addition, mixed matrix and polymer blend 4.0/). membranes have been introduced by mixing membranes with versatile types of filler Membranes 2021, 11, 156. https://doi.org/10.3390/membranes11020156 https://www.mdpi.com/journal/membranes Membranes 2021, 11, x FOR PEER REVIEW 2 of 9 and polymer blend membranes have been introduced by mixing membranes with versa- tile types of filler materials and polymers [10]. Although most of the membranes are pol- ymeric materials, more recently, promising results have been also reported for inorganic membranes using metal–organic frameworks [11]. 2. Discussion Facilitated transport membranes are an emerging solution that combines the reversi- ble reaction between CO2 and the carrier with the intrinsic kinetic properties of a mem- brane process. On the feed interface of the membrane, CO2 reacts with a free amine and forms a carbamate complex, which diffuses through the membrane into the permeate in- Membranes 2021, 11, 156 terface of the membrane (Figure 1). With the presence of inert sweeping gas or vacuum2 of 9 on the permeate side, CO2 dissociates from the complex because of the near-zero CO2 par- tial pressure on the permeate side. Meanwhile, the non-reactive gases, such as N2, H2, and materialsCH4, can only and polymerstransport [through10]. Although the membrane most of thevia membranesa physical solution–diffusion are polymeric materials, process, morein which recently, the gas promising is adsorbed results by have the beenmembrane also reported on the feed for inorganic interfacemembranes and then diffuses using metal–organicthrough the membrane frameworks along [11 ].its concentration gradient to the permeate interface where the desorption occurs. Most non-facilitated polymeric membranes separate gases follow- 2.ing Discussion the solution–diffusion mechanism, based on the differences in solubility and/or diffu- sivityFacilitated of gas pairs. transport A variety membranes of approaches are an emergingare being solutionexplored that and combines studied to the improve reversible the reactionpermeability between and CO selectivity2 and the of carrier facilitated with transport the intrinsic membranes, kinetic properties such as tuning of a membrane the chain process.flexibility On of the the feed hydrogel interface polymer, of the membrane,increasing the CO carrier2 reacts density with a freeinside amine the membrane, and forms aetc. carbamate This article complex, focuses which on the diffuses discussion through of two the highly membrane effective into approaches, the permeate which interface rep- ofresent the membrane the most promising (Figure1). future With the direction presence of ofthe inert technology: sweeping (1) gas improving or vacuum the on carrier the permeateefficiency side,by tuning CO2 dissociatesthe molecular from struct theure complex and (2) because constructing of the the near-zero ultrafast CO CO2 partial2-selec- pressuretive transport on the channel. permeate side. Meanwhile, the non-reactive gases, such as N2,H2, and CH4,As can a only result transport of the throughspecific reaction the membrane between via CO a physical2 and the solution–diffusion amine carrier, facilitated process, intransport which the membranes gas is adsorbed usually by possess the membrane high selectivity. on the feedHowever, interface the and amine then is diffusesalso the throughorigin of the a hydrogen membrane bonding along its formation concentration that results gradient in toa reduction the permeate in the interface diffusivity where of the the desorptionCO2–amine occurs. complex. Most To non-facilitateddisrupt the hydrogen-bonding polymeric membranes network, separate a favorable gases carrier following mo- thelecular solution–diffusion structure is needed. mechanism, The Hideto based onMats theuyama differences research in solubility group at and/or Kobe diffusivityUniversity ofinvestigated gas pairs. a A variety variety of of amino approaches acid ionic are beingliquid-type explored carriers and with studied different to improve molecular the permeabilitystructures and and found selectivity that a ofcyclic facilitated amino transport acid ionic membranes, liquid had suchthe smallest as tuning viscosity the chain in- flexibilitycrease upon of theCO2 hydrogel absorption polymer, owing to increasing the ring structur the carriere that density limits the inside available the membrane, hydrogen etc.atoms This to form article hydrogen focuses onbonding the discussion [12]. They of later two used highly the effective prolinate approaches, ionic liquid whichcarrier representand achieved the most an ultra-high promising CO future2 permeability direction of of the 52,000 technology: Barrer and (1) improving CO2/N2 selectivity the carrier of efficiency8100 at 30 by °C, tuning 70% therelative molecular humidity structure (RH) andand (2) 0.1 constructing KPa of CO2the partial ultrafast pressure, CO2-selective showing transportgreat promise channel. for the direct capture of CO2 from the atmosphere [13]. Figure 1. Schematic of CO2 and amine carrier interaction and an ultrafast CO2-selective transport Figure 1. Schematic of CO2 and amine carrier interaction and an ultrafast CO2-selective transport channelchannel inside inside a a facilitated facilitated transport transport membrane. membrane. As a result of the specific reaction between CO2 and the amine
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