Juqing Liu

Graphene‐Based Electrodes

Graphene, the thinnest two dimensional carbon material, has become the subject of intensive investigation in various research fields because of its remarkable electronic, mechanical, optical and thermal properties. Graphene-based electrodes, fabricated from mechanically cleaved graphene, chemical vapor deposition (CVD) grown graphene, or massively produced graphene derivatives from bulk graphite, have been applied in a broad range of applications, such as in light emitting diodes, touch screens, field-effect transistors, solar cells, supercapacitors, batteries, and sensors. In this Review, after a short introduction to the properties and synthetic methods of graphene and its derivatives, we will discuss the importance of graphene-based electrodes, their fabrication techniques, and application areas.

Preparation of MoS2-Polyvinylpyrrolidone Nanocomposites for Flexible Nonvolatile Rewritable Memory Devices with Reduced Graphene Oxide Electrodes

A facile method for exfoliation and dispersion of molybdenum disulfide (MoS2) with the aid of polyvinylpyrrolidone (PVP) is proposed. The resultant PVP-coated MoS2 nanosheets, i.e., MoS2-PVP nanocomposites, are well dispersed in the low-boiling ethanol solvent, facilitating their thin film preparation and the device fabrication by solution processing technique. As a proof of concept, a flexible memory diode with the configuration of reduced graphene oxide (rGO)/MoS2-PVP/Al exhibited a typical bistable electrical switching and nonvolatile rewritable memory effect with the function of flash. These experimental results prove that the electrical transition is due to the charge trapping and detrapping behavior of MoS2 in the PVP dielectric material. This study paves a way of employing two-dimensional nanomaterials as both functional materials and conducting electrodes for the future flexible data storage.

Bulk Heterojunction Polymer Memory Devices with Reduced Graphene Oxide as Electrodes

A unique device structure with a configuration of reduced graphene oxide (rGO) /P3HT:PCBM/Al has been designed for the polymer nonvolatile memory device. The current-voltage (I-V) characteristics of the fabricated device showed the electrical bistability with a write-once-read-many-times (WORM) memory effect. The memory device exhibits a high ON/OFF ratio (10(4)-10(5)) and low switching threshold voltage (0.5-1.2 V), which are dependent on the sheet resistance of rGO electrode. Our experimental results confirm that the carrier transport mechanisms in the OFF and ON states are dominated by the thermionic emission current and ohmic current, respectively. The polarization of PCBM domains and the localized internal electrical field formed among the adjacent domains are proposed to explain the electrical transition of the memory device.

Fabrication of Ultralong Hybrid Microfibers from Nanosheets of Reduced Graphene Oxide and Transition-Metal Dichalcogenides and their Application as Supercapacitors†

Two-dimensional materials have attracted increasing research interest owing to their unique electronic, physical, optical, and mechanical properties. We thus developed a general strategy for the fabrication of ultralong hybrid microfibers from a mixture of reduced graphene oxide and transition-metal dichalcogenides (TMDs), including MoS2 , TiS2 , TaS2 , and NbSe2 . Furthermore, we prepared fiber-based solid-state supercapacitors as a proof-of-concept application. The performance of thus-prepared supercapacitors was greatly improved by the introduction of the TMDs.

Fabrication of Flexible, All‐Reduced Graphene Oxide Non‐Volatile Memory Devices

A flexible, all reduced graphene oxide non-volatile memory device, with lightly reduced GO as an active layer and highly reduced GO as both top and bottom electrodes, is fabricated by a full-solution process and its performance is characterized. It provides a convenient method to construct other all-carbon devices.

Layer thinning and etching of mechanically exfoliated MoS2 nanosheets by thermal annealing in air

A simple thermal annealing method for layer thinning and etching of mechanically exfoliated MoS2 nanosheets in air is reported. Using this method, single-layer (1L) MoS2 nanosheets are achieved after the thinning of MoS2 nanosheets from double-layer (2L) to quadri-layer (4L) at 330 °C. The as-prepared 1L MoS2 nanosheet shows comparable optical and electrical properties with the mechanically exfoliated, pristine one. In addition, for the first time, the MoS2 mesh with high-density of triangular pits is also fabricated at 330 °C, which might arise from the anisotropic etching of the active MoS2 edge sites. As a result of thermal annealing in air, the thinning of MoS2 nanosheet is possible due to its oxidation to form MoO3 . Importantly, the MoO3 fragments on the top of thinned MoS2 layer induces the hole injection, resulting in the p-type channel in fabricated field-effect transistors.

A facile, relative green, and inexpensive synthetic approach toward large-scale production of SnS2 nanoplates for high-performance lithium-ion batteries

A facile, environmentally friendly, and economical synthetic route for production of large-amounts (gram scale) of two-dimensional (2D) layered SnS(2) nanoplates is presented. The electrode fabricated from the SnS(2) nanoplate exhibits excellent lithium-ion battery performance with highly reversible capacity, good cycling stability and excellent capacity retention after 30 cycles.

Coating Two-Dimensional Nanomaterials with Metal–Organic Frameworks

We demonstrate the coating of various 2D nanomaterials including MoS2 nanosheets, graphene oxide (GO), and reduced graphene oxide (rGO) with zeolitic imidazolate frameworks (i.e., ZIF-8) via a facile procedure. Additionally, ternary core-shell structures like Pt-MoS2@ZIF-8, Pt-GO@ZIF-8, and Pt-rGO@ZIF-8 have also been prepared. As a proof-of-concept application, a memory device based on MoS2@ZIF-8 hybrid was fabricated and it exhibited write-once-read-many-times (WORM) memory effect with high ON/OFF ratio and long operating lifetime. It is expected that MOF coated 2D nanomaterials may find wide applications in energy storage and conversion, catalysis, sensing, and information storage devices.

A Universal, Rapid Method for Clean Transfer of Nanostructures onto Various Substrates

Transfer and integration of nanostructures onto target substrates is the prerequisite for their fundamental studies and practical applications. Conventional transfer techniques that involve stamping, lift-off, and/or striping suffer from the process-specific drawbacks, such as the requirement for chemical etchant or high-temperature annealing and the introduction of surface discontinuities and/or contaminations that can greatly hinder the properties and functions of the transferred materials. Herein, we report a universal and rapid transfer method implementable at mild conditions. Nanostructures with various dimensionalities (i.e., nanoparticles, nanowires, and nanosheets) and surface properties (i.e., hydrophilic and hydrophobic) can be easily transferred to diverse substrates including hydrophilic, hydrophobic, and flexible surfaces with good fidelity. Importantly, our method ensures the rapid and clean transfer of two-dimensional materials and allows for the facile fabrication of vertical heterostructures with various compositions used for electronic devices. We believe that our method can facilitate the development of nanoelectronics by accelerating the clean transfer and integration of low-dimensional materials into multidimensional structures.

Interdiffusion Reaction-Assisted Hybridization of Two-Dimensional Metal–Organic Frameworks and Ti3C2Tx Nanosheets for Electrocatalytic Oxygen Evolution

Two-dimensional (2D) metal-organic framework (MOF) nanosheets have been recently regarded as the model electrocatalysts due to their porous structure, fast mass and ion transfer through the thickness, and large portion of exposed active metal centers. Combining them with electrically conductive 2D nanosheets is anticipated to achieve further improved performance in electrocatalysis. In this work, we in situ hybridized 2D cobalt 1,4-benzenedicarboxylate (CoBDC) with Ti3C2Tx (the MXene phase) nanosheets via an interdiffusion reaction-assisted process. The resulting hybrid material was applied in the oxygen evolution reaction and achieved a current density of 10 mA cm-2 at a potential of 1.64 V vs reversible hydrogen electrode and a Tafel slope of 48.2 mV dec-1 in 0.1 M KOH. These results outperform those obtained by the standard IrO2-based catalyst and are comparable with or even better than those achieved by the previously reported state-of-the-art transition-metal-based catalysts. While the CoBDC layer provided the highly porous structure and large active surface area, the electrically conductive and hydrophilic Ti3C2Tx nanosheets enabled the rapid charge and ion transfer across the well-defined Ti3C2Tx-CoBDC interface and facilitated the access of aqueous electrolyte to the catalytically active CoBDC surfaces. The hybrid nanosheets were further fabricated into an air cathode for a rechargeable zinc-air battery, which was successfully used to power a light-emitting diode. We believe that the in situ hybridization of MXenes and 2D MOFs with interface control will provide more opportunities for their use in energy-based applications.