Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

Fiber-based structures are highly desirable for wearable electronics that are expected to be light-weight, long-lasting, flexible, and conformable Many fibrous structures have been manufactured by well-established lost-effective textile processing technologies, normally at ambient conditions The advancement of nanotechnology has made it feasible to build electronic devices directly on the surface or inside of single fibers, which have typical thickness of several to tens microns However, imparting electronic functions to porous, highly deformable and three-dimensional fiber assemblies and maintaining them during wear represent great challenges from both views of fundamental understanding and practical implementation This article attempts to critically review the current state-of-arts with respect to materials, fabrication techniques, and structural design of devices as well as applications of the fiber-based wearable electronic products In addition, this review elaborates the performance requirements of the fiber-based wearable electronic products, especially regarding the correlation among materials, fiber/textile structures and electronic as well as mechanical functionalities of fiber-based electronic devices Finally, discussions will be presented regarding to limitations of current materials, fabrication techniques, devices concerning manufacturability and performance as well as scientific understanding that must be improved prior to their wide adoption

Fiber‐Based Wearable Electronics: A Review of Materials, Fabrication, Devices, and Applications

We developed two-step solution-phase reactions to form hybrid materials of Mn3O4 nanoparticles on reduced graphene oxide (RGO) sheets for lithium ion battery applications. Mn3O4 nanoparticles grown selectively on RGO sheets over free particle growth in solution allowed for the electrically insulating Mn3O4 nanoparticles wired up to a current collector through the underlying conducting graphene network. The Mn3O4 nanoparticles formed on RGO show a high specific capacity up to ~900mAh/g near its theoretical capacity with good rate capability and cycling stability, owing to the intimate interactions between the graphene substrates and the Mn3O4 nanoparticles grown atop. The Mn3O4/RGO hybrid could be a promising candidate material for high-capacity, low-cost, and environmentally friendly anode for lithium ion batteries. Our growth-on-graphene approach should offer a new technique for design and synthesis of battery electrodes based on highly insulating materials.

Mn3O4-Graphene Hybrid as a High Capacity Anode Material for Lithium Ion Batteries

Notably, many significant breakthroughs for a new generation of supercapacitors have been reported in recent years, related to theoretical understanding, material synthesis and device designs. Herein, we summarize the state-of-the-art progress toward mechanisms, new materials, and novel device designs for supercapacitors. Firstly, fundamental understanding of the mechanism is mainly focused on the relationship between the structural properties of electrode materials and their electrochemical performances based on some in situ characterization techniques and simulations. Secondly, some emerging electrode materials are discussed, including metal–organic frameworks (MOFs), covalent organic frameworks (COFs), MXenes, metal nitrides, black phosphorus, LaMnO3, and RbAg4I5/graphite. Thirdly, the device innovations for the next generation of supercapacitors are provided successively, mainly emphasizing flow supercapacitors, alternating current (AC) line-filtering supercapacitors, redox electrolyte enhanced supercapacitors, metal ion hybrid supercapacitors, micro-supercapacitors (fiber, plane and three-dimensional) and multifunctional supercapacitors including electrochromic supercapacitors, self-healing supercapacitors, piezoelectric supercapacitors, shape-memory supercapacitors, thermal self-protective supercapacitors, thermal self-charging supercapacitors, and photo self-charging supercapacitors. Finally, the future developments and key technical challenges are highlighted regarding further research in this thriving field.

Latest advances in supercapacitors: from new electrode materials to novel device designs.

The ability to achieve simultaneous intrinsic deformation with fast response in commercially available materials that can safely contact skin continues to be an unresolved challenge for artificial actuating materials. Rather than using a microporous structure, here we show an ambient-driven actuator that takes advantage of inherent nanoscale molecular channels within a commercial perfluorosulfonic acid ionomer (PFSA) film, fabricated by simple solution processing to realize a rapid response, self-adaptive, and exceptionally stable actuation. Selective patterning of PFSA films on an inert soft substrate (polyethylene terephthalate film) facilitates the formation of a range of different geometries, including a 2D (two-dimensional) roll or 3D (three-dimensional) helical structure in response to vapor stimuli. Chemical modification of the surface allowed the development of a kirigami-inspired single-layer actuator for personal humidity and heat management through macroscale geometric design features, to afford a bilayer stimuli-responsive actuator with multicolor switching capability. Intrinsic deformation with fast response in commercially available materials that can safely contact skin continues to be a challenge for artificial actuating materials. Here the authors incorporate nanoscale molecular channels within perfluorosulfonic acid ionomer for self-adaptive and ambient-driven actuation.

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Molecular-channel driven actuator with considerations for multiple configurations and color switching.

The use of solar energy has the potential to provide an effective solution to the energy crisis. Generally, the solar energy is converted into electric energy which is transferred through external electric wires to electrochemical devices, such as lithium ion batteries and supercapacitors, for storage. To further improve the energy conversion and storage efficiency, it is important to simultaneously realize the two functions, photoelectric conversion (PC) and energy storage (ES), in one device. Recently, attempts have been made to directly stack a photovoltaic cell and a supercapacitor into one device which can absorb and store solar energy. However, these stacked devices exhibited low overall photoelectric conversion and storage efficiencies. In addition, the planar format in such stacked devices has limited their applications, such as in electronic textiles where a wire structure is required. Herein, an integrated energy wire has been developed to simultaneously realizes photoelectric conversion and energy storage with high efficiency. The fabrication is schematically shown in the Supporting Information, Figure S1. A titanium wire was modified in sections with aligned titania nanotubes on the surface. Active materials for photoelectric conversion and energy storage were then coated onto the modified parts with titania nanotubes. Aligned carbon nanotube (CNT) fibers were finally twisted with the modified Ti wire to produce the desired device. The Ti wire and CNT fiber had been used as electrodes. Figure 1a schematically shows a wire in which one part capable of photoelectric conversion and one part capable of energy storage. This novel wire device exhibits an overall photoelectric conversion and storage efficiency of 1.5%. Aligned titania nanotubes were grown on the Ti wires by electrochemical anodization in a two-electrode system. Figures 1b and 1c show typical scanning electron microscopy (SEM) images of titania nanotubes. The diameters of titania nanotubes ranged from 50 to 100 nm with the wall thickness varying from 15 to 50 nm, and their length was about 20 mm (Figure S2). In this case, titania nanotubes were mainly used to improve the charge separation and transport in photoelectric conversion and increase the surface area in energy storage. Aligned CNT fibers were spun from spinnable CNTarrays which had been synthesized by chemical vapor deposition. They could be produced with lengths of hundreds of meters through the continuous spinning process, and were typically ranged from 10 to 30 mm in diameter. Figure 1d shows a typical SEM image of a CNT fiber which has a uniform diameter of 10 mm. Figure 1e further shows that the CNTs are highly aligned in the fiber, which enables combined remarkable properties including tensile strength of 10– 10 MPa, electrical conductivity of 10 Scm , and high electrocatalytic activity comparable to the conventional platinum. In addition, the CNT fibers were flexible and could be easily and closely twisted with each other or with the other fiber materials (Figure S3), which was critical for the success in a wire-shaped device. Photoactive materials were deposited onto the titania nanotube-modified parts on the Ti wire, for photoelectric conversion, while the desired gel electrolyte was coated onto the other sections for energy storage. Aligned CNT fibers were then twisted with both photoelectric-conversion and energy-storage parts to produce an integrated wire-shaped device. For simplicity, an “energy wire” which was composed of one photoelectric conversion section and one energy storage section had been mainly investigated in this work. Figure 2a shows a typical photograph of a wire with the left Figure 1. a) Schematic illustration of the integrated wire-shaped device for photoelectric conversion (PC) and energy storage (ES). b),c) Scanning electron microscopy (SEM) images of aligned titania nanotubes grown on a Ti wire by electrochemical anodization for 2 h at low and high magnifications, respectively. d),e) SEM images of a CNT fiber at low and high magnifications, respectively.

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An Integrated "energy wire" for both photoelectric conversion and energy storage.

A coaxial electric double-layer capacitor fiber is developed from the aligned carbon nanotube fiber and sheet, which functions as two electrodes with a polymer gel sandwiched between them. The unique coaxial structure enables a rapid transportation of ions between the two electrodes with a high electrochemical performance. These energy storage fibers are also flexible and stretchable, and can be woven into and widely used for electronic textiles.

Novel electric double-layer capacitor with a coaxial fiber structure.

An all-solid-state, coaxial and self-powered "energy fiber" is demonstrated that simultaneously converts solar energy to electric energy and further stores it. The "energy fiber" is flexible and can be scaled up for the practical application by the well-developed textile technology, and may open a new avenue to future photoelectronics and electronics.

Integrated Polymer Solar Cell and Electrochemical Supercapacitor in a Flexible and Stable Fiber Format

Twisted, aligned carbon nanotube/silicon composite fibers with remarkable mechanical and electronic properties are designed to develop novel flexible lithium-ion batteries with a high cyclic stability. The core-sheath architecture and the aligned structure of the composite nanotube offer excellent combined properties.

Twisted Aligned Carbon Nanotube/Silicon Composite Fiber Anode for Flexible Wire‐Shaped Lithium‐Ion Battery

An electrochromic fiber-shaped super-capacitor is developed by winding aligned carbon nanotube/polyaniline composite sheets on an elastic fiber. The fiber-shaped supercapacitors demonstrate rapid and reversible chromatic transitions under different working states, which can be directly observed by the naked eye. They are also stretchable and flexible, and are woven into textiles to display designed signals in addition to storing energy.

Huijuan Lin

Papers

An Integrated "energy wire" for both photoelectric conversion and energy storage.

Novel electric double-layer capacitor with a coaxial fiber structure.

Integrated Polymer Solar Cell and Electrochemical Supercapacitor in a Flexible and Stable Fiber Format

Twisted Aligned Carbon Nanotube/Silicon Composite Fiber Anode for Flexible Wire‐Shaped Lithium‐Ion Battery

Electrochromic fiber-shaped supercapacitors.