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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.

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.

Graphene fibers (GFs) are promising elements for flexible conductors and energy storage devices, while translating the extraordinary properties of individual graphene sheets into the macroscopically assembled 1D structures. We report that a small amount of water addition to the graphene oxide (GO) N-methyl-2-pyrrolidone (NMP) dispersion has significant influences on the mesophase structures and physical properties of wet-spun GFs. Notably, 2 wt % of water successfully hydrates GO flakes in NMP dope to form a stable graphene oxide liquid crystal (GOLC) phase. Furthermore, 4 wt % of water addition causes spontaneous planarization of wet-spun GFs. Motivated from these interesting findings, we develop highly electroconductive and mechanically strong flat GFs by introducing highly crystalline electrochemically exfoliated graphene (EG) in the wet-spinning of NMP-based GOLC fibers. The resultant high-performance hybrid GFs can be sewn on cloth, taking advantage of the mechanical robustness and high flexibility., A small amount of water can hydrate graphene oxide dispersed in organic solvents, resulting in formation of a liquid crystal phase and spontaneous rearrangement of graphene fibers in a flat geometry.

Energy storage system (ESS) can mediate the smart distribution of local energy to reduce the overall carbon footprint in the environment. South Korea is actively involved in the integration of ESS into renewable energy development. This perspective highlights the research and development status of ESS in South Korea. We provide an overview of different ESS technologies practiced in South Korea with a special emphasise on the electrochemical energy storage systems. We also discuss the possible strategies for the sustainable development of ESS in South Korea.

Unzipping carbon nanotubes (CNTs) may offer a valuable route to synthesize graphene nanoribbon (GNR) structures with semiconducting properties. Unfortunately, currently available unzipping methods commonly rely on a random harsh chemical reaction and thereby cause significant degradation of the crystalline structure and electrical properties of GNRs. Herein, crystalline semiconducting GNRs are achieved by a synergistic, judiciously designed two-step unzipping method for N-doped CNTs (NCNTs). NCNTs are effectively unzipped by damage-minimized, dopant-specific electrochemical unzipping and subsequent sonochemical treatment into long ribbon-like nanostructures with crystalline basal planes. Owing to the nanoscale dimension originating from the dense nucleation of the unzipping reaction at highly NCNTs, the resultant GNRs demonstrate semiconducting properties, which can be exploited for chemiresistor-type gas-sensing devices and many other applications.

We report ultrafast recrystallization of perovskite (methylammonium lead tribromide, MAPbBr3) by flash light annealing (FLA) for light-emitting diode (LED) application. Intense near-infrared (NIR) peak spectrum (830 and 900 nm) of flash light could rapidly heat MAPbBr3 based LED structures over ∼320 °C without radiative damage. Cuboidal morphology of the perovskite active layer was evolved into the dense recrystallized structure with a noticeably small grain size (∼38 nm) by FLA, which significantly promoted the radiative recombination. Surface roughness (root mean square (RMS)) of the perovskite layer was decreased by 62% (from 8.47 to 3.22 nm) via FLA, while inhibiting the leakage current that limit current efficiency (CE) of perovskite LED (PeLED). Three dimensional temperature simulation was investigated for the mechanism of flash-induced MAPbBr3 recrystallization. Finally, FLA was successfully exploited for the flexible PeLEDs on polyethylene naphthalate substrates, which exhibited 252% larger CE compared to thermally annealed counterpart.

We investigate the unusually rapid directed self-assembly of block copolymer (BCP) thin films by imposing an in-plane electric field. Blending short chain BCPs dramatically enhances the generically retarded chain diffusivity for BCP self-assembly in thin films. In addition, photopatterned, few-layer solution-cast chemically modified graphene is introduced as a disposable and versatile electrode for electric field applications. A variety of laterally ordered self-assembled lamellar BCP nanopatterns are attained within a 10 min time scale, including an arbitrary large-area unidirectionally oriented lamellar array.

Rational design of 2D materials is crucial for the realization of their profound implications in energy and environmental fields. The past decade has witnessed significant developments in 2D material research, yet a number of critical challenges remain for real-world applications. Nanoscale assembly, precise control over the orientational and positional ordering, and complex interfaces among 2D layers are essential for the continued progress of 2D materials, especially for energy storage and conversion and environmental remediation. Herein, recent progress, the status, future prospects, and challenges associated with nanoscopic assembly of 2D materials are highlighted, specifically targeting energy and environmental applications. Geometric dimensional diversity of 2D material assembly is focused on, based on novel assembly mechanisms, including 1D fibers from the colloidal liquid crystalline phase, 2D films by interfacial tension (Marangoni effect), and 3D nanoarchitecture assembly by electrochemical processes. Relevant critical advantages of 2D material assembly are highlighted for application fields, including secondary batteries, supercapacitors, catalysts, gas sensors, desalination, and water decontamination.

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.

Miniaturization of electronics demands electromagnetic interference (EMI) shielding of nanoscale dimension. The authors report a systematic exploration of EMI shielding behavior of 2D Ti3 C2 Tx MXene assembled films over a broad range of film thicknesses, monolayer by monolayer. Theoretical models are used to explain the shielding mechanism below skin depth, where multiple reflection becomes significant, along with the surface reflection and bulk absorption of electromagnetic radiation. While a monolayer assembled film offers ≈20% shielding of electromagnetic waves, a 24-layer film of ≈55 nm thickness demonstrates 99% shielding (20 dB), revealing an extraordinarily large absolute shielding effectiveness (3.89 × 106 dB cm2 g-1 ). This remarkable performance of nanometer-thin solution processable MXene proposes a paradigm shift in shielding of lightweight, portable, and compact next-generation electronic devices.

Graphene, despite being the best known strong and electrical/thermal conductive material, has found limited success in practical applications, mostly due to difficulties in the formation of desired large-scale highly organized structures. Our discovery of a liquid crystalline phase formation in graphene oxide dispersion has enabled a broad spectrum of highly aligned graphene-based structures, including films, fibers, membranes, and mesoscale structures. In this review, the current understanding of the structure-property relationship of graphene oxide liquid crystals (GOLCs) is overviewed. Various synthetic methods and parameters that can be optimized for GOLC phase formation are highlighted. Along with the results from different characterization methods for the identification of the GOLC phases, the typical characteristics of different types of GOLC phases introduced so far, including nematic, lamellar and chiral phases, are carefully discussed. Finally, various interesting applications of GOLCs are outlined together with the future prospects for their further developments.

Cost effective scalable method for uniform film formation is highly demanded for the emerging applications of 2D transition metal dichalcogenides (TMDs). We demonstrate a reliable and fast interfacial self-assembly of TMD thin films and their heterostructures. Large-area 2D TMD monolayer films are assembled at air-water interface in a few minutes by simple addition of ethyl acetate (EA) onto dilute aqueous dispersions of TMDs. Assembled TMD films can be directly transferred onto arbitrary nonplanar and flexible substrates. Precise thickness controllability of TMD thin films, which is essential for thickness-dependent applications, can be readily obtained by the number of film stacking. Most importantly, complex structures such as laterally assembled 2D heterostructures of TMDs can be assembled from mixture solution dispersions of two or more different TMDs. This unusually fast interfacial self-assembly could open up a novel applications of 2D TMD materials with precise tunability of layer number and film structures.

Spatial arrangement of 1D nanomaterials may offer enormous opportunities for advanced electronics and photonics. Moreover, morphological complexity and chemical diversity in the nanoscale components may lead to unique properties that are hardly anticipated in randomly distributed homogeneous nanostructures. Here, controlled chemical segmentation of metal nanowire arrays using block copolymer lithography and subsequent reversible metal ion loading are demonstrated. To impose chemical heterogeneity in the nanowires generated by block copolymer lithography, reversible ion loading method highly specific for one particular polymer block is introduced. Reversibility of the metal ion loading enables area-selective localized replacement of metal ions in the self-assembled patterns and creates segmented metal nanowire arrays with different metallic components. Further integration of this method with shear aligning process produces high aligned segmented metal nanowire array with desired local chemical compositions.

Inspired by mussel adhesive polydopamine (PDA), effective reinforcement of graphene-based liquid crystalline fibers to attain high mechanical and electrical properties simultaneously is presented. The two-step defect engineering, relying on bioinspired surface polymerization and subsequent solution infiltration of PDA, addresses the intrinsic limitation of graphene fibers arising from the folding and wrinkling of graphene layers during the fiber-spinning process. For a clear understanding of the mechanism of PDA-induced defect engineering, interfacial adhesion between graphene oxide sheets is straightforwardly analyzed by the atomic force microscopy pull-off test. Subsequently, PDA could be converted into an N-doped graphitic layer within the fiber structure by a mild thermal treatment such that mechanically strong fibers could be obtained without sacrificing electrical conductivity. Bioinspired graphene-based fiber holds great promise for a wide range of applications, including flexible electronics, multifunctional textiles, and wearable sensors.