2D transition metal carbides and nitrides (MXenes), a class of emerging nanomaterials with intriguing properties, have attracted significant attention in recent years. However, owing to the highly hydrophilic nature of MXene nanosheets, assembly strategies of MXene at liquid–liquid interfaces have been very limited and challenging. Herein, through the cooperative assembly of MXene and amine‐functionalized polyhedral oligomeric silsesquioxane at the oil–water interface, we report the formation, assembly, and jamming of a new type MXene‐based Janus‐like nanoparticle surfactants, termed MXene‐surfactants (MXSs), which can significantly enhance the interfacial activity of MXene nanosheets. More importantly, this simple assembly strategy opens a new platform for the fabrication of functional MXene assemblies from mesoscale (e.g., structured liquids) to macroscale (e.g., aerogels), that can be used for a range of applications, including nanocomposites, electronic devices, and all‐liquid microfluidic devices.

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Amphiphilic Janus MXene nanosheets are synthesized for the first time by a one-step transferring method, which can act as promising solid surfactants to stabilize emulsions, and assemble into macroscopic 2D ultrathin MXene films and 3D MXene aerogels.

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Membrane capacitive deionization (MCDI) featuring both high electrosorption capacity and high energy effi ciency holds promise for desalination. However, the large-scale applications of MCDI are limited greatly by the high cost of commercial ion-exchange membranes and the interfacial resistance. Here, a new strategy for high-performance MCDI is established using sulfonated graphene (SG) as cation-selective coating. A continuous ultrathin SG coating via self-assembly is formed and attached tightly onto the surface of electrospun carbon nanofi bers (CNFs) by a simple yet effective dip-coating technique, yielding SG-CNF composites with a hydrophilic surface, high electrochemical specifi c capacitance, and greatly reduced interfacial charge transfer rate. These result in signifi cantly enhanced capacitive deionization performance in terms of both electrosorption capacity and charge effi ciency. The SG coating shows excellent cation selectivity for an asymmetric cell with SG-CNFs as a cathode. The new approach may pave a way to novel micro-MCDI, i.e. novel applications of functional graphene-based materials for highperformance, energy-effi cient, and cost-effective desalination.Adv. Mater. Interfaces 2015, 2, 1500372 www.advmatinterfaces.de www.MaterialsViews.com Adv. Mater . Interfaces 2015, 2, 1500372 www.advmatinterfaces.de www.MaterialsViews.com Scheme 1. a) Schematic of the three-step synthesis of SG; insets display the digital images of rGO and SG suspension after standing for 1 week. b) Schematic of the "dip-coating" process; insets show the digital images of rGO-CNFs and SG-CNFs.

Polyelectrolyte microcapsules can be produced either by the layer-by-layer assembly technique or the formation of polyelectrolyte complexes at the liquid− liquid interface. Here, we describe the design and construction of DNA microcapsules using the cooperative assembly of DNA and amine-functionalized polyhedral oligomeric silsesquioxane (POSS-NH2) at the oil−water interface. "Janus-like" DNA surfactants (DNASs) assemble in situ at the interface, forming an elastic film. By controlling the jamming and unjamming behavior of DNASs, the interfacial assemblies can assume three different physical states: solid-like, elastomer-like, and liquid-like, similar to that seen with thermoplastics upon heating, that change from a glassy to a rubbery state, and then to a viscous liquid. By the interfacial jamming of DNASs, the liquid structures can be locked-in and reconfigured, showing promising potentials for drug delivery, biphasic reactors, and programmable liquid constructs.