Improving the operational stability of perovskite solar cells with cesium-doped graphene oxide interlayer

Perovskite solar cells(PSCs)have made great advances in terms of power conversion efficiency(PCE),yet their subpar stability continues to hinder their commercialization.The interface between the perovskite layer and the charge-carrier transporting layers plays a crucial role in undermining the stability of PSCs.In this work,we propose a strategy to stabilize high-performance PSCs with PCE over 23%by introducing a cesium-doped graphene oxide(GO-Cs)as an interlayer between the perovskite and hole-transporting material.The GO-Cs treated PSCs exhibit excellent operational stability with a projected T80(the time where the device PCE reduces to 80%of its initial value)of 2143 h of operation at the maximum powering point under one sun illumination.

Preface to Special Topic:Graphene and 2D Materials for Energy Storage

Graphene, a single layer of graphite, has been one of the first real two dimensional （2D） materials isolated in 2004. Thus, graphene is becoming a cutting edge material that opens up new horizons to a whole family of 2D materials beyond the limited current applicability of graphene. The unique advantages of graphene and analogue 2D materials, such as atomic-scale thickness, high specific surface area, mechanically flexible robustness, superior storage capacity, endow them as high-performance electrodes lbr electrochemical energy storage devices. Although it is hard to say whether or not graphene and 2D materials will be implemented in future energy technologies, the recent achievements in this field demonstrate that their roles will be noticeable in the near future.

Precise Thermoplastic Processing of Graphene Oxide Layered Solid by Polymer Intercalation

The processing capability is vital for the wide applications of materials to forge structures as-demand.Graphene-based macroscopic materials have shown excellent mechanical and functional properties.However,different from usual polymers and metals,graphene solids exhibit limited deformability and processibility for precise forming.Here,we present a precise thermoplastic forming of graphene materials by polymer intercalation from graphene oxide(GO)precursor.The intercalated polymer enables the thermoplasticity of GO solids by thermally activated motion of polymer chains.We detect a critical minimum containing of intercalated polymer that can expand the interlayer spacing exceeding 1.4 nm to activate thermoplasticity,which becomes the criteria for thermal plastic forming of GO solids.By thermoplastic forming,the flat GO-composite films are forged to Gaussian curved shapes and imprinted to have surface relief patterns with size precision down to 360 nm.The plastic-formed structures maintain the structural integration with outstanding electrical(3.07×10^(5) S m^(−1))and thermal conductivity(745.65 W m^(−1) K^(−1))after removal of polymers.The thermoplastic strategy greatly extends the forming capability of GO materials and other layered materials and promises versatile structural designs for more broad applications.

Heteroatom Doped Multi-Layered Graphene Material for Hydrogen Storage Application

A variety of distinctive techniques have been developed to produce graphene sheets and their functionalized subsidiaries or composites. The production of graphene sheets by oxidative exfoliation of graphite can be a suitable route for the preparation of high volumes of graphene derivatives. P-substituted graphene material is developed for its application in hydrogen sorption in room temperature. Phosphorous doped graphene material with multi-layers of graphene shows a nearly ~2.2 wt% hydrogen sorption capacity at 298 K and 100 bar. This value is higher than that for reduced graphene oxide (RGO without phosphorous).

Recent progress in 2D materials for flexible supercapacitors

High performance supercapacitors coupled with mechanical flexibility are needed to drive flexible and wearable electronics that have anesthetic appeal and multi-functionality. Two dimensional（2D） materials have attracted attention owing to their unique physicochemical and electrochemical properties, in addition to their ability to form hetero-structures with other nanomaterials further improving mechanical and electrochemical properties. After a brief introduction of supercapacitors and 2D materials, recent progress on flexible supercapacitors using 2D materials is reviewed. Here we provide insights into the structure–property relationships of flexible electrodes, in particular free-standing films. We also present our perspectives on the development of flexible supercapacitors.

Graphene fiber based supercapacitors:Strategies and perspective toward high performances

Modern wearable electronics are thirsty for flexible, lightweight energy storage and supply devices. Flexible fiber-shaped supercapacitors, possess good flexibility, high power density, fast charging capability and long cycle life, becoming a promising option for wearable devices. The past decade has witnessed the emergence of graphene fiber based supercapacitors（GFSCs） as one of the most active vicinity in fiber-supercapactiors, for their excellent properties including high surface area, chemical stability, excellent electrical conductivity, lightweight and mechanical properties. In this perspective, we introduced the basic energy storage mechanisms of GFSCs, followed by the analysis in improving their overall performances, recent advances, and a conclusive discussion on the challenges and opportunities.

Highly stable two-dimensional graphene oxide:Electronic properties of its periodic structure and optical properties of its nanostructures

According to first principle simulations, we theoretically predict a type of stable single-layer graphene oxide（C_2O）.Using density functional theory（DFT）, C_2O is found to be a direct gap semiconductor. In addition, we obtain the absorption spectra of the periodic structure of C_2O, which show optical anisotropy. To study the optical properties of C_2O nanostructures, time-dependent density functional theory（TDDFT） is used. The C_2O nanostructure has a strong absorption near 7 eV when the incident light polarizes along the armchair-edge. Besides, we find that the optical properties can be controlled by the edge configuration and the size of the C_2O nanostructure. With the elongation strain increasing, the range of light absorption becomes wider and there is a red shift of absorption spectrum.

Effective exposure of nitrogen heteroatoms in 3D porous graphene framework for oxygen reduction reaction and lithium–sulfur batteries

The introduction of nitrogen heteroatoms into carbon materials is a facile and efficient strategy to regulate their reactivities and facilitate their potential applications in energy conversion and storage. However,most of nitrogen heteroatoms are doped into the bulk phase of carbon without site selectivity, which significantly reduces the contacts of feedstocks with the active dopants in a conductive scaffold. Herein we proposed the chemical vapor deposition of a nitrogen-doped graphene skin on the 3D porous graphene framework and donated the carbon/carbon composite as surface N-doped grapheme（SNG）. In contrast with routine N-doped graphene framework（NGF） with bulk distribution of N heteroatoms, the SNG renders a high surface N content of 1.81 at%, enhanced electrical conductivity of 31 S cm^（-1）, a large surface area of 1531 m^2 g^（-1）, a low defect density with a low I_D/I_G ratio of 1.55 calculated from Raman spectrum, and a high oxidation peak of 532.7 ℃ in oxygen atmosphere. The selective distribution of N heteroatoms on the surface of SNG affords the effective exposure of active sites at the interfaces of the electrode/electrolyte, so that more N heteroatoms are able to contact with oxygen feedstocks in oxygen reduction reaction or serve as polysulfide anchoring sites to retard the shuttle of polysulfides in a lithium–sulfur battery. This work opens a fresh viewpoint on the manipulation of active site distribution in a conductive scaffolds for multi-electron redox reaction based energy conversion and storage.

Engineering graphene for high-performance supercapacitors: Enabling role of colloidal chemistry

The high electrical conductivity and high specific surface area of graphene are traditionally regarded as the most intriguing features for its promise as the electrode material for supercapacitors. In this perspective, we highlight that from the engineering point of view, the unique colloidal chemistry of chemically functionalized graphene is the key property that has made graphene stand out as a promising nanoscale building block for constructing unique nanoporous electrodes for capacitive energy storage, We present several examples to demonstrate bow the non-covalent colloidal forces between graphene sheets can be harnessed to engineer the nanostructure of graphene-based bulk electrodes for supercapacitors based on both the electrical double layer storage and the redox reaction or pseudo-capacitance mechanisms. The colloidal engineering strategy can be extended to enable other nanomaterials to achieve high energy storage performance.

The roles of graphene in advanced Li-ion hybrid supercapacitors

Lithium-ion hybrid supercapacitors （LIHSs）, also called Li-ion capacitors, are electrochemical energy stor- age devices that combining the advantages of high power density of supercapacitor and high energy density of Li-ion battery. However, high power density and long cycle life are still challenges for the cul~ rent LIHSs due to the imbalance of charge-storage capacity and electrode kinetics between capacitor-type cathode and battery-type anode. Therefore, great efforts have been made on designing novel cathode materials with high storage capacity and anode material with enhanced kinetic behavior for LIHSs. With unique two-dimensional form and numerous appealing properties, for the past several years, the rational designed graphene and its composites materials exhibit greatly improved electrochemical performance as cathode or anode for LIHSs. Here, we summarized and discussed the latest advances of the state- of-art graphene-based materials for LIHSs applications. The major roles of graphene are highlighted as （1） a superior active material, （2） ultrathin 2D flexible support to remedy the sluggish reaction of the metal compound anode, and （3） good 2D building blocks for constructing macroscopic 3D pOFOUS car- bonjgraphene hybrids. In addition, some high performance aqueous LIHSs using graphene as electrode were also summarized. Finally, the perspectives and challenges are also proposed for further develop- ment of more advanced graphene-based LIHSs.

Flexible,robust and highly efficient broadband nonlinear optical materials based on graphene oxide impregnated polymer sheets

We report a simple solution-processed method for the fabrication of low-cost,flexible optical limiting materials based on graphene oxide(GO) impregnated polyvinyl alcohol(PVA) sheets.Such GO–PVA composite sheets display highly efficient broadband optical limiting activities for femtosecond laser pulses at 400,800,and 1400 nm with very low limiting thresholds.Femtosecond pump–probe measurement results revealed that nonlinear absorption played an important role for the observed optical limiting activities.High flexibility and efficient optical limiting activities of these materials allow these composite sheets to be attached to nonplanar optical sensors in order to protect them from light-induced damage.

High-performance lithium-ion batteries based on polymer/graphene hybrid cathode material

Organic and carbon-based lithium-ion batteries possess abundant resources,nontoxicity,environmental friendliness,and high performance,and they have been widely studied in the past decades.However,it remains a challenge to construct such batteries with high capacity,high cycling stability,and high conductivity simultaneously.Here,we elaborately design and integrate organic polymer(p-FcPZ) with graphene network to create a hybrid material(p-FcPZ@G) for high-performance lithium-ion batteries(LIBs).The bi-polar polymer p-FcPZ containing multiple redox-active sites endows p-FcPZ@G with both remarkable cycling stability and high capacity.The porous conductive graphene network with a large surface area facilitates rapid ions/electrons transportation,resulting in superior rate performance.Therefore,the half-cell based on p-FcPZ@G cathode exhibits simultaneously high capacity(~250 mA h g^(-1) at 50 mA g^(-1)),excellent cycling stability(retention of 99.999% per cycle for 10,000 cycles at 2,000 mA g^(-1)) and superior rate performance.Additionally,the graphene-based full cell assembled with p-FcPZ@G cathode and graphene anode also demonstrates comprehensively high electrochemical performance.

Thermoacoustic theory of graphene films considering heat transfer of substrate materials

Based on thermoacoustic theory, a coupled thermal-mechanical model for graphene films is established, and the analytical solutions for thermal-acoustic radiation from a graphene thin film are obtained. The sound pressure of the graphene film generator on different substrates is measured, and the measurement data is compared with the theoretical results. The frequency response from the experimental results is consistent with the theoretical ones, while the measured values are slightly lower than the theoretical ones. Therefore, the accuracy of the proposed theoretical model is verified. It is shown that thermal-acoustic radiation from a graphene thin film reveals a wide frequency response. The sound pressure level increases with the frequency in the low frequency range, while the sound pressure varies smoothly with frequency in the high frequency range. Thus it can be used as excellent thermal generator. When the thermal effusivity of the substrate is smaller, then the sound pressure of grapheme films will be higher. Furthermore, the sound pressure decreases with the increase of heat capacity per unit area of grapheme films. Results will contribute to the mechanism of graphene films generator and its applications in the design of loudspeaker and other related areas.

2D materials via liquid exfoliation:a review on fabrication and applications

Since graphene was discovered, the study of two-dimensional(2D) materials with atomic thickness has become a hot spot. To prepare different 2D materials,different methods have been groped, such as mechanical exfoliation, chemical vapor deposition(CVD), liquid-phase exfoliation. This review mainly introduced the sonication liquid-phase exfoliation, an effective method to prepare 2D materials. Compared with mechanical exfoliation and CVD methods, liquid-phase exfoliation is convenient and costeffective and provides high yield. We focused on both theoretical and experimental details of this method. This method was reviewed according to the development of 2D materials from graphene, h-BN to transition metal chalcogenides(TMDs) and black phosphorus nanosheets.We discussed the applications of liquid-exfoliated 2D materials including micro- and nanoelectrical devices,photoelectric devices, and energy storage devices.

Pyrolyzed bacterial cellulose/graphene oxide sandwich interlayer for lithium–sulfur batteries

Herein, a facile strategy for the synthesis of sandwich pyrolyzed bacterial cellulose（PBC）/graphene oxide（GO） composite was reported simply by utilizing the large-scale regenerated biomass bacterial cellulose as precursor. The unique and delicate structure where three-dimensional interconnected bacterial cellulose（BC） network embedded in two-dimensional GO skeleton could not only work as an effective barrier to retard polysulfide diffusion during the charge/discharge process to enhance the cyclic stability of the Li–S battery, but also offer a continuous electron transport pathway for the improved rate capability.As a result, by utilizing pure sulfur as cathodes, the Li–S batteries assembled with PBC/GO interlayer can still exhibit a capacity of nearly 600 mAh·g^-1 at 3C and only 0.055% capacity decay per cycle can be observed over 200 cycles. Additionally, the cost-efficient and environmentfriendly raw materials may enable the PBC/GO sandwich interlayer to be an advanced configuration for Li–S batteries.

Improved performance of Li-Se battery based on a novel dual functional CNTs@graphene/CNTs cathode construction

A dual functional CNTs@graphene/CNTs cathode for Li–Se battery was constructed by a CNTs@graphene network and a CNTs interlayer. CNTs were first integrated with graphene to form a three-dimensional（3D） framework and work together as a conductive matrix for Se confinement. The optimized composite cathode delivers a high initial capacity of 575 mAh·g^-1 at 0.5 A·g^-1 and good rate capacity with a retained capacity of 479 mAh·g^-1 at 2.0 A·g^-1（73% of the capacity at 0.2 A·g^-1）. CNTs were further served as an interlayer to confine the diffusion of polyselenides by constructing a thin CNTs layer outside the CNTs@graphene network. An improved initial capacity of 616 mAh·g^-1 at 0.5 A·g^-1 is achieved with a retained capacity of 538 mAh·g^-1 after 80 cycles, indicating the effective dual function of CNTs in this novel cathode construction and great application potential for Li–Se battery.

Photodetectors based on two dimensional materials

Two-dimensional（2D） materials with unique properties have received a great deal of attention in recent years. This family of materials has rapidly established themselves as intriguing building blocks for versatile nanoelectronic devices that offer promising potential for use in next generation optoelectronics, such as photodetectors. Furthermore, their optoelectronic performance can be adjusted by varying the number of layers. They have demonstrated excellent light absorption, enabling ultrafast and ultrasensitive detection of light in photodetectors,especially in their single-layer structure. Moreover, due to their atomic thickness, outstanding mechanical flexibility, and large breaking strength, these materials have been of great interest for use in flexible devices and strain engineering. Toward that end, several kinds of photodetectors based on 2D materials have been reported. Here, we present a review of the state-of-the-art in photodetectors based on graphene and other 2D materials, such as the graphene, transition metal dichalcogenides, and so on.