skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Scalable synthesis of nanoporous atomically thin graphene membranes for dialysis and molecular separations via facile isopropanol-assisted hot lamination

Journal Article · · Nanoscale
DOI:https://doi.org/10.1039/d0nr07384a· OSTI ID:1785190

Scalable graphene synthesis and facile large-area membrane fabrication are imperative to advance nanoporous atomically thin membranes (NATMs) for molecular separations. Although chemical vapor deposition (CVD) allows for roll-to-roll high-quality monolayer graphene synthesis, facile transfer with atomically clean interfaces to porous supports for large-area NATM fabrication remains extremely challenging. Sacrificial polymer scaffolds commonly used for graphene transfer typically leave polymer residues detrimental to membrane performance and transfers without polymer scaffolds suffer from low yield resulting in high non-selective leakage through NATMs. In this study, we systematically study the factors influencing graphene NATM fabrication and report on a novel roll-to-roll manufacturing compatible isopropanol-assisted hot lamination (IHL) process that enables scalable, facile and clean transfer of CVD graphene on to polycarbonate track etched (PCTE) supports with coverage ≥99.2%, while preserving support integrity/porosity. We demonstrate fully functional centimeter-scale graphene NATMs that show record high permeances (~2–3 orders of magnitude higher) and better selectivity than commercially available state-of-the-art polymeric dialysis membranes, specifically in the 0–1000 Da range. Our work highlights a scalable approach to fabricate graphene NATMs for practical applications and is fully compatible with roll-to-roll manufacturing processes.

Research Organization:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); ACS Petroleum Research Fund; National Science Foundation (NSF)
Grant/Contract Number:
AC05-00OR22725; 59267-DNI10; 1944134
OSTI ID:
1785190
Journal Information:
Nanoscale, Vol. 13, Issue 5; ISSN 2040-3364
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (71)

The structure of suspended graphene sheets journal March 2007
Large-area graphene-nanomesh/carbon-nanotube hybrid membranes for ionic and molecular nanofiltration journal June 2019
DNA Translocation through Graphene Nanopores journal August 2010
Proton transport through one-atom-thick crystals journal November 2014
Clean Transfer of Graphene for Isolation and Suspension journal February 2011
Molecular Sieving Across Centimeter-Scale Single-Layer Nanoporous Graphene Membranes journal May 2017
Measurement of the Optical Conductivity of Graphene journal November 2008
Engineering high charge transfer n-doping of graphene electrodes and its application to organic electronics journal January 2015
Visualization and characterization of interfacial polymerization layer formation journal January 2015
Multifunctional wafer-scale graphene membranes for fast ultrafiltration and high permeation gas separation journal November 2018
A direct transfer of layer-area graphene journal March 2010
Fundamental transport mechanisms, fabrication and potential applications of nanoporous atomically thin membranes journal June 2017
Selective Molecular Transport through Intrinsic Defects in a Single Layer of CVD Graphene journal October 2012
Assessment and control of the impermeability of graphene for atomically thin membranes and barriers journal January 2017
A Direct and Polymer-Free Method for Transferring Graphene Grown by Chemical Vapor Deposition to Any Substrate journal January 2014
Nanoporous Atomically Thin Graphene Membranes for Desalting and Dialysis Applications journal June 2017
Heterogeneous sub-continuum ionic transport in statistically isolated graphene nanopores journal October 2015
Wetting-Assisted Crack- and Wrinkle-Free Transfer of Wafer-Scale Graphene onto Arbitrary Substrates over a Wide Range of Surface Energies journal January 2016
Raman spectroscopy as a versatile tool for studying the properties of graphene journal April 2013
Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils journal May 2009
Paraffin-enabled graphene transfer journal February 2019
Facile Fabrication of Large-Area Atomically Thin Membranes by Direct Synthesis of Graphene with Nanoscale Porosity journal October 2018
Rapid Selective Etching of PMMA Residues from Transferred Graphene by Carbon Dioxide journal October 2013
Reducing Extrinsic Performance-Limiting Factors in Graphene Grown by Chemical Vapor Deposition journal March 2012
Ultra-thin hybrid polyhedral silsesquioxane–polyamide films with potentially unlimited 2D dimensions journal January 2012
Nanofiltration across Defect-Sealed Nanoporous Monolayer Graphene journal April 2015
Selective Proton/Deuteron Transport through Nafion|Graphene|Nafion Sandwich Structures at High Current Density journal January 2018
Roll-to-roll production of 30-inch graphene films for transparent electrodes journal June 2010
Single-layer graphene membranes by crack-free transfer for gas mixture separation journal July 2018
Clean Transfer of Wafer-Scale Graphene via Liquid Phase Removal of Polycyclic Aromatic Hydrocarbons journal March 2015
First-Principles Study of the Role of O 2 and H 2 O in the Decoupling of Graphene on Cu(111) journal August 2016
Freestanding carbon nanomembranes and graphene monolayers nanopatterned via EUV interference lithography journal February 2019
Stable, Temperature-Dependent Gas Mixture Permeation and Separation through Suspended Nanoporous Single-Layer Graphene Membranes journal July 2018
Catalyst Interface Engineering for Improved 2D Film Lift-Off and Transfer journal November 2016
Water and Solute Transport Governed by Tunable Pore Size Distributions in Nanoporous Graphene Membranes journal October 2017
Observing Graphene Grow: Catalyst–Graphene Interactions during Scalable Graphene Growth on Polycrystalline Copper journal September 2013
Direct transfer of graphene onto flexible substrates journal October 2013
Facile Size-Selective Defect Sealing in Large-Area Atomically Thin Graphene Membranes for Sub-Nanometer Scale Separations journal July 2020
Role of Graphene in Water-Assisted Oxidation of Copper in Relation to Dry Transfer of Graphene journal May 2017
Graphene Annealing: How Clean Can It Be? journal December 2011
The Parameter Space of Graphene Chemical Vapor Deposition on Polycrystalline Cu journal October 2012
Broadening the Gas Separation Utility of Monolayer Nanoporous Graphene Membranes by an Ionic Liquid Gating journal October 2020
3D structure of individual nanocrystals in solution by electron microscopy journal July 2015
Water desalination using nanoporous single-layer graphene journal March 2015
Advances in transferring chemical vapour deposition graphene: a review journal January 2017
A Scalable Route to Nanoporous Large-Area Atomically Thin Graphene Membranes by Roll-to-Roll Chemical Vapor Deposition and Polymer Support Casting journal March 2018
Effects of polymethylmethacrylate-transfer residues on the growth of organic semiconductor molecules on chemical vapor deposited graphene journal March 2015
The effect of chemical residues on the physical and electrical properties of chemical vapor deposited graphene transferred to SiO 2 journal September 2011
Capillary flow as the cause of ring stains from dried liquid drops journal October 1997
Direct dry transfer of chemical vapor deposition graphene to polymeric substrates journal March 2015
State-of-the-Art and Future Prospects for Atomically Thin Membranes from 2D Materials journal August 2018
Ion selectivity of graphene nanopores journal April 2016
Synergistic Roll‐to‐Roll Transfer and Doping of CVD‐Graphene Using Parylene for Ambient‐Stable and Ultra‐Lightweight Photovoltaics journal June 2020
Macroscopic Salt Rejection through Electrostatically Gated Nanoporous Graphene journal August 2019
Do-It-Yourself Transfer of Large-Area Graphene Using an Office Laminator and Water journal March 2019
Tunable Anion-Selective Transport through Monolayer Graphene and Hexagonal Boron Nitride journal December 2019
Selective Nanoscale Mass Transport across Atomically Thin Single Crystalline Graphene Membranes journal March 2017
Ultraconformal Contact Transfer of Monolayer Graphene on Metal to Various Substrates journal July 2014
Organic light emitting diodes with environmentally and thermally stable doped graphene electrodes journal January 2014
Selective Ionic Transport through Tunable Subnanometer Pores in Single-Layer Graphene Membranes journal February 2014
Porous Graphene as the Ultimate Membrane for Gas Separation journal December 2009
A Rational Strategy for Graphene Transfer on Substrates with Rough Features journal January 2016
DNA Translocation through Graphene Nanopores journal August 2010
Ultrafast Nanofiltration through Large-Area Single-Layered Graphene Membranes journal March 2017
Multifunctional oxides for integrated manufacturing of efficient graphene electrodes for organic electronics journal February 2015
Ultimate Permeation Across Atomically Thin Porous Graphene journal April 2014
Voltage gated inter-cation selective ion channels from graphene nanopores journal January 2019
Metal Oxide Induced Charge Transfer Doping and Band Alignment of Graphene Electrodes for Efficient Organic Light Emitting Diodes journal June 2014
A facile process for soak-and-peel delamination of CVD graphene from substrates using water journal January 2014
Detaching graphene from copper substrate by oxidation-assisted water intercalation journal March 2016
Fine Structure Constant Defines Visual Transparency of Graphene journal June 2008