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Direct Chemical Vapor Deposition Synthesis of Porous Single‐Layer Graphene Membranes with High Gas Permeances and Selectivities
Name
10.1002-adma.202104308.pdf
Size
1.67 MB
Format
Adobe PDF
Checksum (MD5)
1230e4a0cf002e7042bccfbeb6f4d00a
Author(s)
Yuan, Zhe
He, Guangwei
Faucher, Samuel
Kuehne, Matthias
Li, Sylvia Xin
Blankschtein, Daniel
Strano, Michael S.
Date Issued
September 12, 2021
Journal
Advanced Materials
Publisher
Wiley
Citation
Yuan, Zhe, He, Guangwei, Faucher, Samuel, Kuehne, Matthias, Li, Sylvia Xin et al. 2021. "Direct Chemical Vapor Deposition Synthesis of Porous Single‐Layer Graphene Membranes with High Gas Permeances and Selectivities." Advanced Materials, 33 (44).
Version
Author's final manuscript
Abstract
Single-layer graphene containing molecular-sized in-plane pores is regarded as a promising membrane material for high-performance gas separations due to its atomic thickness and low gas transport resistance. However, typical etching-based pore generation methods cannot decouple pore nucleation and pore growth, resulting in a trade-off between high areal pore density and high selectivity. In contrast, intrinsic pores in graphene formed during chemical vapor deposition are not created by etching. Therefore, intrinsically porous graphene can exhibit high pore density while maintaining its gas selectivity. In this work, the density of intrinsic graphene pores is systematically controlled for the first time, while appropriate pore sizes for gas sieving are precisely maintained. As a result, single-layer graphene membranes with the highest H2 /CH4 separation performances recorded to date (H2 permeance > 4000 GPU and H2 /CH4 selectivity > 2000) are fabricated by manipulating growth temperature, precursor concentration, and non-covalent decoration of the graphene surface. Moreover, it is identified that nanoscale molecular fouling of the graphene surface during gas separation where graphene pores are partially blocked by hydrocarbon contaminants under experimental conditions, controls both selectivity and temperature dependent permeance. Overall, the direct synthesis of porous single-layer graphene exploits its tremendous potential as high-performance gas-sieving membranes.
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DOI of Published Version
http://dx.doi.org/10.1002/adma.202104308
