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An effective pathway to build macroscopic scale functional architectures bearing diverse structural dimensions is one of the critical challenges in the two-dimensional (2D) MXene research area. Unfortunately, assembling MXene without adhesive binder is largely limited due to its innate brittle nature and the relatively weak inter-flake van der Waals contact, in contrast to other mechanically compliant 2D materials such as graphene. Herein, an electrochemical self-assembly of pure Ti3C2Tx MXenes is presented for functional multidimensional MXene structures, effectively driven by layer-by-layer spontaneous interfacial reduction at metal template surfaces and subsequent defunctionalization. A three-dimensional open porous aerogel as well as 2D highly stacked thin film structures could be readily obtained in this approach, along with largely enhanced electrical properties induced by spontaneous removal of charge-trapping oxygen functional groups. Accordingly, supercapacitors and electromagnetic interference shielding films based on the multidimensional assembly demonstrate excellent performances.

Many interesting properties of 2D materials and their assembled structures are strongly dependent on the lateral size and size distribution of 2D materials. Accordingly, effective size separation of polydisperse 2D sheets is critical for desirable applications. Here, we introduce flow field-flow fractionation (FlFFF) for a wide-range size fractionation of graphene oxide (GO) up to 100 μm. Two different separation mechanisms are identified for FlFFF, including normal mode and steric/hyperlayer mode, to size fractionate wide size-distributed GOs while employing a crossflow field for either diffusion or size-controlled migration of GO. Obviously, the 2D GO sheet reveals size separation behavior distinctive from typical spherical particles arising from its innate planar geometry. We also investigate 2D sheet size-dependent mechanical and electrical properties of three different graphene fibers produced from size-fractionated GOs. This FlFFF-based size selection methodology can be used as a generic approach for effective wide-range size separation for 2D materials, including rGO, TMDs, and MXene.

Two-dimensional (2D) MXene has shown enormous potential in scientific fields, including energy storage and electromagnetic interference (EMI) shielding. Unfortunately, MXene-based material structures generally suffer from mechanical fragility and vulnerability to oxidation. Herein, mussel-inspired dopamine successfully addresses those weaknesses by improving interflake interaction and ordering in MXene assembled films. Dopamine undergoes in situ polymerization and binding at MXene flake surfaces by spontaneous interfacial charge transfer, yielding an ultrathin adhesive layer. Resultant nanocomposites with highly aligned tight layer structures achieve approximately seven times enhanced tensile strength with a simultaneous increase of elongation. Ambient stability of MXene films is also greatly improved by the effective screening of oxygen and moisture. Interestingly, angstrom thick polydopamine further promotes the innate high electrical conductivity and excellent EMI shielding properties of MXene films. This synergistic concurrent enhancement of physical properties proposes MXene/polydopamine hybrids as a general platform for MXene based reliable applications.

An effective pathway to build macroscopic scale functional architectures bearing diverse structural dimensions is one of the critical challenges in the two-dimensional (2D) MXene research area. Unfortunately, assembling MXene without adhesive binder is largely limited due to its innate brittle nature and the relatively weak inter-flake van der Waals contact, in contrast to other mechanically compliant 2D materials such as graphene. Herein, an electrochemical self-assembly of pure Ti

Two-dimensional (2D) MXene has shown enormous potential in scientific fields, including energy storage and electromagnetic interference (EMI) shielding. Unfortunately, MXene-based material structures generally suffer from mechanical fragility and vulnerability to oxidation. Herein, mussel-inspired dopamine successfully addresses those weaknesses by improving interflake interaction and ordering in MXene assembled films. Dopamine undergoes

Block copolymer (BCP) lithography is an effective nanopatterning methodology exploiting nanoscale self-assembled periodic patterns in BCP thin films. This approach has a critical limitation for nonplanar substrate geometry arising from the reflow and modification of BCP films upon the thermal or solvent annealing process, which is inevitable to induce the mobility of BCP chains for the self-assembly process. Herein, reflow-free, 3D BCP nanopatterning is demonstrated by introducing a conformally grown adlayer by the initiated chemical vapor deposition (iCVD) process. A highly cross-linked poly(divinylbenzene) layer was deposited directly onto the BCP thin film surface by iCVD, which effectively prevented the reflow of BCP thin film during an annealing process. BCP nanopatterns could be stabilized on various substrate geometry, including a nonplanar deformed polymer substrate, a pyramid shape substrate, and a graphene fiber surface. A fiber-type hydrogen evolution reaction (HER) catalyst is suggested by stabilizing lamellar Pt nanopatterns on severely rough graphene fiber surfaces.

Graphene oxide (GO) is aqueous-dispersible oxygenated graphene, which shows colloidal discotic liquid crystallinity. Many properties of GO-based materials, including electrical conductivity and mechanical properties, are limited by the small flake size of GO. Unfortunately, typical sonochemical exfoliation of GO from graphite generally leads to a broad size and shape distribution. Here, we introduce a facile size selection of large-size GO exploiting liquid crystallinity and investigate the size-dependent N-doping and oxygen reduction catalysis. In the biphasic GO dispersion where both isotropic and liquid crystalline phases are equilibrated, large-size GO flakes (20 μm) are spontaneously concentrated within the liquid crystalline phase. N-Doping and reduction of the size-selected GO exhibit that N-dopant type is highly dependent on GO flake size. Large-size GO demonstrates quaternary dominant N-doping and the lowest onset potential (-0.08 V) for oxygen reduction catalysis, signifying that quaternary N-dopants serve as principal catalytic sites in N-doped graphene.