High-permeance polymer-functionalized single-layer graphene membranes that surpass the postcombustion carbon capture target

He, Guangwei; Huang, Shiqi; Villalobos, Luis Francisco; Zhao, Jing; Mensi, Mounir; Oveisi, Emad; Rezaei, Mojtaba; Agrawal, Kumar Varoon

doi:10.1039/c9ee01238a

Cited by 122 publications

(99 citation statements)

References 52 publications

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“…Recently, there has been an increasing recognition of membrane performance targets for post-combustion CO 2 capture. 48 Depending on specific mode of operation, CO 2 /N 2 selectivity is targeted at 20-150 for pressure-driven operation (pressure ratio 5-15), or 4140 when employing a sweep gas. 49 This selectivity must be present in membranes with CO 2 permeabilities of 10 À13 -10 À12 mol m À1 s À1 Pa À1 to be economically-competitive with existing approaches.…”

Section: Papermentioning

confidence: 99%

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

McNeil

Mutch

Iacoviello

et al. 2020

Energy Environ. Sci.

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Section: Papermentioning

confidence: 99%

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

McNeil

Mutch

Iacoviello

et al. 2020

Energy Environ. Sci.

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“…Consequently, this limitation results in a broad PSD. We have shown that N-SLG with broad PSD can be used for gas separation, albeit using an additional gas-selective layer on top of graphene ( 23 , 24 ). Chemical etching technique involving O 2 ( 8 , 25 ), ultraviolet/O 3 ( 17 ), or O 3 ( 19 , 26 ), in principle, can obtain CO 2 -selective nanopores by slowing down the etching kinetics, e.g., using a low temperature or a small concentration of etchant ( 17 ).…”

Section: Introductionmentioning

confidence: 99%

Millisecond lattice gasification for high-density CO ₂ - and O ₂ -sieving nanopores in single-layer graphene

Huang

Villalobos

et al. 2021

Sci. Adv.

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Etching single-layer graphene to incorporate a high pore density with sub-angstrom precision in molecular differentiation is critical to realize the promising high-flux separation of similar-sized gas molecules, e.g., CO2 from N2. However, rapid etching kinetics needed to achieve the high pore density is challenging to control for such precision. Here, we report a millisecond carbon gasification chemistry incorporating high density (>1012 cm−2) of functional oxygen clusters that then evolve in CO2-sieving vacancy defects under controlled and predictable gasification conditions. A statistical distribution of nanopore lattice isomers is observed, in good agreement with the theoretical solution to the isomer cataloging problem. The gasification technique is scalable, and a centimeter-scale membrane is demonstrated. Last, molecular cutoff could be adjusted by 0.1 Å by in situ expansion of the vacancy defects in an O2 atmosphere. Large CO2 and O2 permeances (>10,000 and 1000 GPU, respectively) are demonstrated accompanying attractive CO2/N2 and O2/N2 selectivities.

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“…This is mainly because CO 2 , N 2 , and CH 4 have only a small difference in their kinetic diameters (≤0.5 Å), and the state‐of‐the‐art etching techniques are not precise enough to avoid the incorporation of nonselective nanopores in graphene. [ 17 ]…”

Section: Introductionmentioning

confidence: 99%

Synergistic CO₂‐Sieving from Polymer with Intrinsic Microporosity Masking Nanoporous Single‐Layer Graphene

Huang

Villalobos

et al. 2020

Adv Funct Materials

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High-flux nanoporous single-layer graphene membranes are highly promising for energy-efficient gas separation. Herein, in the context of carbon capture, a remarkable enhancement in the CO 2 selectivity is demonstrated by uniquely masking nanoporous single-layer graphene with polymer with intrinsic microporosity (PIM-1). In the process, a major bottleneck of the state-of-theart pore-incorporation techniques in graphene has been overcome, where in addition to the molecular sieving nanopores, larger nonselective nanopores are also incorporated, which so far, has restricted the realization of CO 2sieving from graphene membranes. Overall, much higher CO 2 /N 2 selectivity (33) is achieved from the composite film than that from the standalone nanoporous graphene (NG) (10) and the PIM-1 membranes (15), crossing the selectivity target (20) for postcombustion carbon capture. The selectivity enhancement is explained by an analytical gas transport model for NG, which shows that the transport of the stronger-adsorbing CO 2 is dominated by the adsorbed phase transport pathway whereas the transport of N 2 benefits significantly from the direct gas-phase transport pathway. Further, slow positron annihilation Doppler broadening spectroscopy reveals that the interactions with graphene reduce the free volume of interfacial PIM-1 chains which is expected to contribute to the selectivity. Overall, this approach brings graphene membrane a step closer to industrial deployment.

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High-permeance polymer-functionalized single-layer graphene membranes that surpass the postcombustion carbon capture target

Abstract: A single-layer nanoporous graphene membrane functionalized with CO2-phillic polymers shows extremely fast, selective CO2 transport.

Cited by 122 publications

References 52 publications

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

Millisecond lattice gasification for high-density CO ₂ - and O ₂ -sieving nanopores in single-layer graphene

Synergistic CO₂‐Sieving from Polymer with Intrinsic Microporosity Masking Nanoporous Single‐Layer Graphene

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High-permeance polymer-functionalized single-layer graphene membranes that surpass the postcombustion carbon capture target

Abstract: A single-layer nanoporous graphene membrane functionalized with CO2-phillic polymers shows extremely fast, selective CO2 transport.

Cited by 122 publications

References 52 publications

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

Dendritic silver self-assembly in molten-carbonate membranes for efficient carbon dioxide capture

Millisecond lattice gasification for high-density CO 2 - and O 2 -sieving nanopores in single-layer graphene

Synergistic CO2‐Sieving from Polymer with Intrinsic Microporosity Masking Nanoporous Single‐Layer Graphene

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Product

Resources

About

Millisecond lattice gasification for high-density CO ₂ - and O ₂ -sieving nanopores in single-layer graphene

Synergistic CO₂‐Sieving from Polymer with Intrinsic Microporosity Masking Nanoporous Single‐Layer Graphene