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Register a new userTuneable Sieving of Ions Using Graphene Oxide Membranes
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Added by
Rahul Raveendran Nair
Publication date
2017
fields
Physics
and research's language is
English
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Graphene oxide membranes show exceptional molecular permeation properties, with a promise for many applications. However, their use in ion sieving and desalination technologies is limited by a permeation cutoff of ~9 Angstrom, which is larger than hydrated ion diameters for common salts. The cutoff is determined by the interlayer spacing d ~13.5 Angstrom, typical for graphene oxide laminates that swell in water. Achieving smaller d for the laminates immersed in water has proved to be a challenge.Here we describe how to control d by physical confinement and achieve accurate and tuneable ion sieving. Membranes with d from ~ 9.8 Angstrom to 6.4 Angstrom are demonstrated, providing the sieve size smaller than typical ions hydrated diameters.In this regime, ion permeation is found to be thermally activated with energy barriers of ~10-100 kJ/mol depending on d. Importantly, permeation rates decrease exponentially with decreasing the sieve size but water transport is weakly affected (by a factor of <2). The latter is attributed to a low barrier for water molecules entry and large slip lengths inside graphene capillaries. Building on these findings, we demonstrate a simple scalable method to obtain graphene-based membranes with limited swelling, which exhibit 97% rejection for NaCl.
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There has been intense interest in filtration and separation properties of graphene-based materials that can have well-defined nanometer pores and exhibit low frictional water flow inside them. Here we investigate molecular permeation through graphene oxide laminates. They are vacuum-tight in the dry state but, if immersed in water, act as molecular sieves blocking all solutes with hydrated radii larger than 4.5A. Smaller ions permeate through the membranes with little impedance, many orders of magnitude faster than the diffusion mechanism can account for. We explain this behavior by a network of nanocapillaries that open up in the hydrated state and accept only species that fit in. The ultrafast separation of small salts is attributed to an ion sponge effect that results in highly concentrated salt solutions inside graphene capillaries.
Developing smart membranes that allow precise and reversible control of molecular permeation using external stimuli would be of intense interest for many areas of science: from physics and chemistry to life-sciences. In particular, electrical control of water permeation through membranes is a long-sought objective and is of crucial importance for healthcare and related areas. Currently, such adjustable membranes are limited to the modulation of wetting of the membranes and controlled ion transport, but not the controlled mass flow of water. Despite intensive theoretical work yielding conflicting results, the experimental realisation of electrically controlled water permeation has not yet been achieved. Here we report electrically controlled water permeation through micrometre-thick graphene oxide (GO) membranes. By controllable electric breakdown, conductive filaments are created in the GO membrane. The electric field concentrated around such current carrying filaments leads to controllable ionisation of water molecules in graphene capillaries, allowing precise control of water permeation: from ultrafast permeation to complete blocking. Our work opens up an avenue for developing smart membrane technologies and can revolutionize the field of artificial biological systems, tissue engineering and filtration.
The interaction of graphene with neighboring materials and structures plays an important role in its behavior, both scientifically and technologically. The interactions are complicated due to the interplay between surface forces and possibly nonlinear elastic behavior. Here we review recent experimental and theoretical advances in the understanding of graphene adhesion. We organize our discussion into experimental and theoretical efforts directed toward: graphene conformation to a substrate, determination of adhesion energy, and applications where graphene adhesion plays an important role. We conclude with a brief prospectus outlining open issues.
Water transport through graphene-derived membranes has gained much interest recently due to its promising potential in filtration and separation applications. In this work, we explore water permeation in graphene oxide membranes using atomistic simulations, by considering flow through interlayer gallery, expanded pores such as wrinkles of interedge spaces, and pores within the sheet. We find that although flow enhancement can be established by nanoconfinement, fast water transport through pristine graphene channels is prohibited by a prominent side-pinning effect from capillaries formed between oxidized regions. We then discuss flow enhancement in situations according to several recent experiments. These understandings are finally integrated into a complete picture to understand water permeation through the layer-by-layer and porous microstructure and could guide rational design of functional membranes for energy and environmental applications.
The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.
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