Nanoribbon Yarn with Versatile Inorganic Materials.

Nanomaterial-based yarns have been actively developed owing to their advantageous features, namely, high surface-area-to-volume ratios, flexibility, and unusual material characteristics such as anisotropy in electrical/thermal conductivity. The superior properties of the nanomaterials can be directly imparted and scaled-up to macro-sized structures. However, most nanomaterial-based yarns have thus far, been fabricated with only organic materials such as polymers, graphene, and carbon nanotubes. This paper presents a novel fabrication method for fully inorganic nanoribbon yarn, expanding its applicability by bundling highly aligned and suspended nanoribbons made from various inorganic materials (e.g., Au, Pd, Ni, Al, Pt, WO3, SnO2, NiO, In2O3, and CuO). The process involves depositing the target inorganic material on a nanoline mold, followed by suspension through plasma etching of the nanoline mold, and twisting using a custom-built yarning machine. Nanoribbon yarn structures of various functional inorganic materials are utilized for chemical sensors (Pd-based H2 and metal oxides (MOx)-based green gas sensors) and green energy transducers (water splitting electrodes/triboelectric nanogenerators). This method is expected to provide a comprehensive fabrication strategy for versatile inorganic nanomaterials-based yarns.

Sunlight-Driven Self-Cleaning Ultrafine Particulate Matter Filter with Antibacterial Activity.

Air pollution by particulate matter (PM) and airborne pathogens causes severe health problems in the human body. Presently, popular disposable air filters yield huge waste and have a fatal impact on the environment. Postuse cleaning of air filters also leads to secondary air and water pollution. Here, we report a sunlight-driven self-cleaning PM filter by coupling a full-solar-spectrum-active photocatalyst comprising up-conversion nanoparticles (UCNPs) decorated with semiconductor iron(III) oxide (UCNP@α-Fe2O3) shells stabilized upon graphene functionalized borosilicate fibrous membrane (rGO-BF). While rGO-BF ensures high PM adsorption, UCNP@α-Fe2O3 (NP) enables self-photodegradation of adsorbed PM under abundant sunlight and subsequent membrane regeneration, while preventing secondary air or water pollution. Rational surface chemistry and optimal microstructure enable our filters to remove >99% of PM2.5 under deplorable air-quality conditions. Moreover, our filter shows excellent antibacterial activity toward E. coli and S. aureus, demonstrating its potential for practical utilization in face masks, air filtering devices, and protective medical wear. This work successfully suggests an intriguing design platform for self-sustainable zero-waste air filter membranes.

2D Materials Beyond Post-AI Era: Smart Fibers, Soft Robotics, and Single Atom Catalysts.

Recent consecutive discoveries of various 2D materials have triggered significant scientific and technological interests owing to their exceptional material properties, originally stemming from 2D confined geometry. Ever-expanding library of 2D materials can provide ideal solutions to critical challenges facing in current technological trend of the fourth industrial revolution. Moreover, chemical modification of 2D materials to customize their physical/chemical properties can satisfy the broad spectrum of different specific requirements across diverse application areas. This review focuses on three particular emerging application areas of 2D materials: smart fibers, soft robotics, and single atom catalysts (SACs), which hold immense potentials for academic and technological advancements in the post-artificial intelligence (AI) era. Smart fibers showcase unconventional functionalities including healthcare/environmental monitoring, energy storage/harvesting, and antipathogenic protection in the forms of wearable fibers and textiles. Soft robotics aligns with future trend to overcome longstanding limitations of hard-material based mechanics by introducing soft actuators and sensors. SACs are widely useful in energy storage/conversion and environmental management, principally contributing to low carbon footprint for sustainable post-AI era. Significance and unique values of 2D materials in these emerging applications are highlighted, where the research group has devoted research efforts for more than a decade.

Scalable Solution Phase Synthesis of 2D Siloxene via a Two-Step Interlayer Expansion Process.

Two-dimensional (2D) siloxene is attracting considerable research interest recently principally owing to its inherent compatibility with silicon-based semiconductor technology. -The synthesis of siloxene has been mostly limited to multilayered structures using traditional topochemical reaction procedures. Herein, we report high-yield synthesis of single to few-layer siloxene nanosheets by developing a two-step interlayer expansion and subsequent liquid phase exfoliation procedure. Our protocol enables high-yield production of few-layer siloxene nanosheets with a lateral dimension of up to 4 µm and thickness ranging from 0.8 to 4.8 nm, corresponding to single to a few layers, well stabilized in water. The atomically flat nature of exfoliated siloxene can be exploited for the construction of 2D/2D heterostructure membranes via typical solution processing. We demonstrate highly ordered graphene/siloxene heterostructure films with synergistic mechanical and electrical properties, which deliver noticeably high device capacitance when assembled into a coin cell symmetric supercapacitor device structures. Additionally, we demonstrate that the mechanically flexible exfoliated siloxene-graphene heterostructure enables its direct use in flexible and wearable supercapacitor applications.

Application of 2D Materials for Adsorptive Removal of Air Pollutants.

Air pollution is on the priority list of global safety issues, with the concern of fatal environmental and public health deterioration. 2D materials are potential adsorbent materials for environmental decontamination, owing to their high surface area, manageable interlayer binding, large surface-to-volume ratio, specific binding capability, and chemical, thermal, and mechanistic stability. Specifically, graphene oxide and reduced graphene oxide have been attracting attention, taking advantage of their low cost synthesis, excessive oxygen containing surface functionalities, and intrinsic aqueous dispersibility, making them desirable for the development of cost-effective, high performance air filters. Many different material designs have been proposed to expand their filtration capability, including the functionalization and integration with other metals and metal oxides, which act not only as binding agents to the target pollutants but also as antimicrobial agents. This review highlights the advantages and drawbacks of 2D materials for air filtration and summarizes the interrelationships among various strategies and the resultant filtration performance in terms of structural engineering, morphology control, and material compositions. Finally, potential future directions are suggested toward the idealized designs of 2D material based air filters.

Longitudinal unzipping of 2D transition metal dichalcogenides.

Unzipping of the basal plane offers a valuable pathway to uniquely control the material chemistry of 2D structures. Nonetheless, reliable unzipping has been reported only for graphene and phosphorene thus far. The single elemental nature of those materials allows a straightforward understanding of the chemical reaction and property modulation involved with such geometric transformations. Here we report spontaneous linear ordered unzipping of bi-elemental 2D MX2 transition metal chalcogenides as a general route to synthesize 1D nanoribbon structures. The strained metallic phase (1T') of MX2 undergoes highly specific longitudinal unzipping owing to the self-linearized oxygenation at chalcogenides. Stable dispersions of 1T' MoS2 nanoribbons with widths of 10-120 nm and lengths up to ~4 µm are produced in water. Edge abundant 1T' MoS2 nanoribbons reveal the hidden potential of idealized electrocatalysis for hydrogen evolution reactions at a competitive level with the precious Pt catalyst.

Tungsten nitride-coated graphene fibers for high-performance wearable supercapacitors.

Graphene-fiber (GF) supercapacitors have attracted significant research attention in the field of wearable devices. However, there is still a need for active materials with high energy density. Transition Metal Nitrides (TMNs) are promising candidates for this purpose compared with conventional Transition Metal Oxides (TMOs) or conducting polymers (CPs) owing to their higher electrical conductivity, stability and relevant electrochemical properties. We have successfully integrated Tungsten Nitride (WN) with reduced graphene oxide fibers (rGOF) and developed high-performance hybrid fiber (WN-rGOF) supercapacitors. These hybrid supercapacitors attained a high capacitance of 16.29 F cm-3 at 0.05 A cm-3 and an energy density of 1.448 mW h cm-3, which is 7.5 and 1.75 times higher than those of the pure rGOF supercapacitor and the Tungsten Oxide/rGO hybrid fiber (WO3-rGOF) supercapacitor, respectively. The energy density readily increased up to 2.896 mW h cm-3 when three WN-rGOF supercapacitors were connected in series. The WN-rGOF supercapacitor also showed high capacitance retention of 84.7% after 10 000 cycles along with appreciable performance under severe mechanical deformation.

Self-Planarization of High-Performance Graphene Liquid Crystalline Fibers by Hydration.

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.

Graphene oxide liquid crystals: a frontier 2D soft material for graphene-based functional materials.

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.

Multiwall carbon nanotube reinforced teflon fibrils for oil spill clean up and its effective recycling as textile dye sorbent.

Surface functionalized multiwall carbon nanotube (MWCNT) reinforced teflon fibrils (MWCNT@Teflon) were successfully tested as an - oil - absorbent that can be used as a potential oil recovery material at the time of oil spill accidents in water. We found that oleic acid functionalization of MWCNTs was important for their adhesion onto teflon fibrils and at the same time prevented the MWCNT leaching into oil/water interface. The fibrils had displayed superior mechanical and thermal stability and provided a new insight to oil spill clean-up applications with easy recovery of absorbed oil by simple squeezing. Recycling of exhausted MWCNT@Teflon fibrils after oil recovery applications was conducted by pyrolysis under inert atmosphere in presence of magnetic clay. The magnetic clay absorbed the pyrolysis products, resulting in a heterostructured magnetic clay carbon composite (MCC) which was found super paramagnetic and chemically stable in all pH. The MCC was found capable of adsorbing textile dye from water ultra-fast with in a maximum contact time of 2 min and magnetically separable after adsorption experiments.

Interface-Confined High Crystalline Growth of Semiconducting Polymers at Graphene Fibers for High-Performance Wearable Supercapacitors.

We report graphene@polymer core-shell fibers (G@PFs) composed of N and Cu codoped porous graphene fiber cores uniformly coated with semiconducting polymer shell layers with superb electrochemical characteristics. Aqueous/organic interface-confined polymerization method produced robust highly crystalline uniform semiconducting polymer shells with high electrical conductivity and redox activity. When the resultant core-shell fibers are utilized for fiber supercapacitor application, high areal/volume capacitance and energy densities are attained along with long-term cycle stability. Desirable combination of mechanical flexibility, electrochemical properties, and facile process scalability makes our G@PFs particularly promising for portable and wearable electronics.

Prospects of Supercritical Fluids in Realizing Graphene-Based Functional Materials.

Supercritical-fluids science and technology predate all the approaches that are currently established for graphene production by several decades in advanced materials design. However, it has only recently been proposed as a plausible approach for graphene processing. Since then, supercritical fluids have emerged into contention as an alternative to existing technologies because of their scalability and versatility in processing graphene materials, which include composites, aerogels, and foams. Here, an overview is presented of such materials prepared through supercritical fluids from an advanced materials science standpoint, with a discussion on their fundamental properties and technological applications. The benefits of supercritical-fluid processing over conventional liquid-phase processing are presented. The benefits include not only better performances for advanced applications but also environmental issues associated with the synthesis process. Nevertheless, the limitations of supercritical-fluid processing are also stressed, along with challenges that are still faced toward the achievement of the great expectations from graphene materials.