Porous yet densely packed carbon electrodes with high ion-accessible surface area and low ion transport resistance are crucial to the realization of high-density electrochemical capacitive energy storage but have proved to be very challenging to produce. Taking advantage of chemically converted graphene's intrinsic microcorrugated two-dimensional configuration and self-assembly behavior, we show that such materials can be readily formed by capillary compression of adaptive graphene gel films in the presence of a nonvolatile liquid electrolyte. This simple soft approach enables subnanometer scale integration of graphene sheets with electrolytes to form highly compact carbon electrodes with a continuous ion transport network. Electrochemical capacitors based on the resulting films can obtain volumetric energy densities approaching 60 watt-hours per liter.

Modified graphene can self‐gel at the liquid–solid interface in a face‐to‐face manner to form an oriented conductive hydrogel film. This unusual gelation behavior enables a new generation of electroconductive hydrogels combining exceptional mechanical strength, high electrical conductivity, mechanical flexibility, and anisotropic responsive properties. Scale bar: 1 μm.

Ion transport in nanoconfinement differs from that in bulk and has been extensively researched across scientific and engineering disciplines. For many energy and water applications of nanoporous materials, concentration-driven ion diffusion is simultaneously subjected to a local electric field arising from surface charge or an externally applied potential. Due to the uniquely crowded intermolecular forces under severe nanoconfinement (<2 nm), the transport behaviours of ions can be influenced by the interfacial electrical double layer (EDL) induced by a surface potential, with complex implications, engendering unusual ion dynamics. However, it remains an experimental challenge to investigate how such a surface potential and its coupling with nanoconfinement manipulate ion diffusion. Here, we exploit the tunable nanoconfinement in layered graphene-based nanoporous membranes to show that sub-2 nm confined ion diffusion can be strongly modulated by the surface potential-induced EDL. Depending on the potential sign, the combination and concentration of ion pairs, diffusion rates can be reversibly modulated and anomalously enhanced by 4~7 times within 0.5 volts, across a salt concentration gradient up to seawater salinity. Modelling suggests that this anomalously enhanced diffusion is related to the strong ion-ion correlations under severe nanoconfinement, and cannot be explained by conventional theoretical predictions.

An electrogenetic layered graphene hydrogel membrane (GHM) possesses ultra-large interlayer spacing of about 10 nm, forming charged 2D nanocapillaries between graphene sheets that selectively permeate counter-ions and exclude co-ions. When an electrolyte flow goes through the GHM, it functions as an integrated 2D nanofluidic generator converting hydraulic motion into electricity. The maximum streaming conductance density approaches 16.8 μA cm(-2) bar(-1) .

A combination of experiments and simulations unveils unusual nanoconfined ion transport in layered graphene membranes.

From a materials science point of view, graphene is essentially a polymer having a giant, two-dimensional molecular configuration. In this Progress Report, solvated graphene and its derivatives are illustrated from the perspective of soft matter. Firstly, the key appealing features of graphene as a molecular building block for assembling bulk soft materials are highlighed. It is then demonstrated how the intersheet interactions in solution are correlated with the molecular structure of graphene, and how a combination of the unique molecular structure and colloidal interactions can lead to simple, solution-phase approaches for assembling graphenes into a variety of macroscopic nanoarchitectures. A number of new exciting functions and applications are also highlighted, which are enabled by the solvation effect and in particular, it is discussed why and how solvated graphenes can offer exciting functions that are unattainable with the dried, hard counterpart. The discussion is concluded with some personal perspectives on the future directions in which this emerging class of functional soft materials could be pursued.

The architecture of the nanofiller phase in polymer nanocomposites matters! Polymer hydrogels that can combine stimuli-responsiveness with excellent electrically conductivity and mechanical strength can be fabricated by incorporation of the polymer into an ultralight and superelastic graphene aerogel to form a binary network.

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