Fabrication of nanoporous graphene/polymer composite membranes

Madauß, Lukas; Schumacher, J.; Ghosh, Mandakranta; Ochedowski, Oliver; Meyer, Jens; Lebius, H.; Ban-d’Etat, B.; Toimil-Molares, María Eugenia; Trautmann, C.; Lammertink, Rob G.H.; Ulbricht, Mathias; Schleberger, Marika

doi:10.1039/c7nr02755a

Cited by 62 publications

(55 citation statements)

References 28 publications

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“…This can be achieved by either highly charged or by very fast (swift) heavy ions. For both it has been shown that they can be used for defect engineering of 2D materials such as carbon nano-membranes, 26,27 graphene, [28][29][30][31][32][33] hexagonal boron nitride, 34 and MoS 2 . [35][36][37] Swift heavy ions (SHI) excite target atoms along their trajectory and the corresponding energy deposited per track length into the target material is usually given in terms of electronic stopping power S e = dE/dx.…”

Section: Introductionmentioning

confidence: 99%

Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation

et al. 2018

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Section: Introductionmentioning

confidence: 99%

Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation

et al. 2018

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“…However, i) large‐area membrane quality graphene synthesis and transfer to suitable porous supports (without polymer residue or other contamination from transfer), ii) mitigation of nonselective leakage by plugging tears/damages to graphene from transfer and subsequent processing during membrane fabrication, and most importantly iii) the formation of nanopores with a high density and narrow size distribution using cost‐effective, scalable processes are some of the major challenges that need to be collectively addressed to realize NATMs for practical applications . Here, we note that large‐area monolayer graphene synthesis has been demonstrated via roll‐to‐roll chemical vapor deposition (CVD) processes .…”

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Facile Fabrication of Large‐Area Atomically Thin Membranes by Direct Synthesis of Graphene with Nanoscale Porosity

et al. 2018

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NATMs). [1,3,[7][8][9][10][11][12][13][14][15][16][17][18] Such NATMs with extremely high permeance and selectivity [3,4,7,8,[12][13][14][15][16][17][18][19][20] are expected to offer significant advances over current state-of-the-art polymer membranes, specifically for diffusion-based separation processes such as dialysis. [9] However, i) large-area membrane quality graphene synthesis [1,21,22] and transfer to suitable porous supports (without polymer residue or other contamination from transfer), [1,9,21,[23][24][25][26] ii) mitigation of nonselective leakage by plugging tears/ damages to graphene from transfer and subsequent processing during membrane fabrication, [1,9,13,26] and most importantly iii) the formation of nanopores with a high density and narrow size distribution using cost-effective, scalable processes [1,9,13,27,28] are some of the major challenges that need to be collectively addressed to realize NATMs for practical applications. [22,29] Here, we note that large-area monolayer graphene synthesis has been demonstrated via roll-to-roll chemical vapor deposition (CVD) processes. [22,30] Further, graphene transfer at large scale has also been shown [30,31] (although complete elimination of polymer residue remains nontrivial) [17,32,33] and widely used scalable membrane manufacturing techniques such as interfacial polymerization have been adapted to effectively plug leakage across tears/damage in graphene. [13] However, facile, cost-effective processes to form nanoscale defects in Direct synthesis of graphene with well-defined nanoscale pores over large areas can transform the fabrication of nanoporous atomically thin membranes (NATMs) and greatly enhance their potential for practical applications. However, scalable bottom-up synthesis of continuous sheets of nanoporous graphene that maintain integrity over large areas has not been demonstrated. Here, it is shown that a simple reduction in temperature during chemical vapor deposition (CVD) on Cu induces in-situ formation of nanoscale defects (≤2-3 nm) in the graphene lattice, enabling direct and scalable synthesis of nanoporous monolayer graphene. By solution-casting of hierarchically porous polyether sulfone supports on the as-grown nanoporous CVD graphene, large-area (>5 cm2 ) NATMs for dialysis applications are demonstrated. The synthesized NATMs show size-selective diffusive transport and effective separation of small molecules and salts from a model protein, with ≈2-100× increase in permeance along with selectivity better than or comparable to state-of-the-art commercially available polymeric dialysis membranes. The membranes constitute the largest fully functional NATMs fabricated via bottom-up nanopore formation, and can be easily scaled up to larger sizes permitted by CVD synthesis. The results highlight synergistic benefits in blending traditional membrane casting with bottom-up pore creation during graphene CVD for advancing NATMs toward practical applications.

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“…However, the reproducible formation of sub-nanometer pores in 2D membranes with high pore density remains a challenge. 7,8 Porous 2D membranes are commonly fabricated via top-down methods: starting with a continuous 2D layer, followed by the formation of pores by ion bombardment, electron bombardment or reactive plasma exposure. 9 As evident from a recent review focusing on top-down approaches to fabricate porous 2D membranes, pore densities of 1-10 pores per 100 nm 2 were the highest obtained.…”

Section: Introductionmentioning

confidence: 99%

Selective ion sieving through arrays of sub-nanometer nanopores in chemically tunable 2D carbon membranes

et al. 2019

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Two-dimensional (2D) membranes featuring arrays of sub-nanometer pores have applications in purification, solvent separation and water desalination. Compared to channels in bulk membranes, 2D nanopores have lower resistance to transmembrane transport, leading to faster passage of ions. However, the formation of nanopores in 2D membranes requires expensive post-treatment using plasma or ion bombardment. Here, we study bottom-up synthesized porous carbon nanomembranes (CNMs) of biphenyl thiol (BPT) precursors. Sub-nanometer pores arise intrinsically during the BPT-CNM synthesis with a density of 2 ± 1 pore per 100 nm 2 . We employ BPT-CNM based pore arrays as efficient ion sieving channels, and demonstrate selectivity of the membrane towards ion transport when exposed to a range of concentration gradients of KCl, CsCl and MgCl 2 . The selectivity of the membrane towards K + over Cl − ions is found be 16.6 mV at a 10 : 1 concentration ratio, which amounts to ∼30% efficiency relative to the Nernst potential for complete ion rejection. The pore arrays in the BPT-CNM show similar transport and selectivity properties to graphene and carbon nanotubes, whilst the fabrication method via self-assembly offers a facile means to control the chemical and physical properties of the membrane, such as surface charge, chemical nature and pore density. CNMs synthesized from self-assembled monolayers open the way towards the rational design of 2D membranes for selective ion sieving.

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Fabrication of nanoporous graphene/polymer composite membranes

Cited by 62 publications

References 28 publications

Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation

Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation

Facile Fabrication of Large‐Area Atomically Thin Membranes by Direct Synthesis of Graphene with Nanoscale Porosity

Selective ion sieving through arrays of sub-nanometer nanopores in chemically tunable 2D carbon membranes

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Fabrication of nanoporous graphene/polymer composite membranes

Cited by 62 publications

References 28 publications

Highly active single-layer MoS2 catalysts synthesized by swift heavy ion irradiation

Highly active single-layer MoS2 catalysts synthesized by swift heavy ion irradiation

Facile Fabrication of Large‐Area Atomically Thin Membranes by Direct Synthesis of Graphene with Nanoscale Porosity

Selective ion sieving through arrays of sub-nanometer nanopores in chemically tunable 2D carbon membranes

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Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation

Highly active single-layer MoS₂ catalysts synthesized by swift heavy ion irradiation