2D Nanomaterials for Cancer Theranostic Applications

2D nanomaterials with unique nanosheet structures, large surface areas, and extraordinary physicochemical properties have attracted tremendous interest. In the area of nanomedicine, research on graphene and its derivatives for diverse biomedical applications began as early as 2008. Since then, many other types of 2D nanomaterials, including transition metal dichalcogenides, transition metal carbides, nitrides and carbonitrides, black phosphorus nanosheets, layered double hydroxides, and metal–organic framework nanosheets, have been explored in the area of nanomedicine over the past decade. In particular, a large surface area makes 2D nanomaterials highly efficient drug delivery nanoplatforms. The unique optical and/or X-ray attenuation properties of 2D nanomaterials can be harnessed for phototherapy or radiotherapy of cancer. Furthermore, by integrating 2D nanomaterials with other functional nanoparticles or utilizing their inherent physical properties, 2D nanomaterials may also be engineered as nanoprobes for multimodal imaging of tumors. 2D nanomaterials have shown substantial potential for cancer theranostics. Herein, the latest progress in the development of 2D nanomaterials for cancer theranostic applications is summarized. Current challenges and future perspectives of 2D nanomaterials applied in nanomedicine are also discussed.     

Flexible and High‐Performance All‐2D Photodetector for Wearable Devices

Emerging novel applications at the forefront of innovation horizon raise new requirements including good flexibility and unprecedented properties for the photoelectronic industry. On account of diversity in transport and photoelectric properties, 2D layered materials have proven as competent building blocks toward next‐generation photodetectors. Herein, an all‐2D Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector is fabricated with pulsed‐laser deposition. It is sensitive to broadband wavelength from ultraviolet (370 nm) to near‐infrared (808 nm). In addition, it exhibits great durability to bend, with intact photoresponse after 100 bend cycles. Upon 370 nm illumination, it achieves a high responsivity of 115 A W^?1, a large external quantum efficiency of 3.9 × 10⁴%, and a superior detectivity of 4.1 × 10¹¹ Jones. They are among the best figures‐of‐merit of state‐of‐the‐art 2D photodetectors. The synergistic effect of SnS's strong light–matter interaction, efficient carrier separation of Bi₂Te₃–SnS interface, expedite carrier injection across Bi₂Te₃–SnS interface, and excellent carrier collection of Bi₂Te₃ topological insulator electrodes accounts for the superior photodetection properties. In summary, this work depicts a facile all‐in‐one fabrication strategy toward a Bi₂Te₃‐SnS‐Bi₂Te₃ photodetector. More importantly, it reveals a novel all‐2D concept for construction of flexible, broadband, and high‐performance photoelectronic devices by integrating 2D layered metallic electrodes and 2D layered semiconducting channels.     

Cellulose‐Based Nanomaterials for Energy Applications

Cellulose is the most abundant natural polymer on earth, providing a sustainable green resource that is renewable, degradable, biocompatible, and cost effective. Recently, nanocellulose‐based mesoporous structures, flexible thin films, fibers, and networks are increasingly developed and used in photovoltaic devices, energy storage systems, mechanical energy harvesters, and catalysts components, showing tremendous materials science value and application potential in many energy‐related fields. In this Review, the most recent advancements of processing, integration, and application of cellulose nanomaterials in the areas of solar energy harvesting, energy storage, and mechanical energy harvesting are reviewed. For solar energy harvesting, promising applications of cellulose‐based nanostructures for both solar cells and photoelectrochemical electrodes development are reviewed, and their morphology‐related merits are discussed. For energy storage, the discussion is primarily focused on the applications of cellulose‐based nanomaterials in lithium‐ion batteries, including electrodes (e.g., active materials, binders, and structural support), electrolytes, and separators. Applications of cellulose nanomaterials in supercapacitors are also reviewed briefly. For mechanical energy harvesting, the most recent technology evolution in cellulose‐based triboelectric nanogenerators is reviewed, from fundamental property tuning to practical implementations. At last, the future research potential and opportunities of cellulose nanomaterials as a new energy material are discussed.     

2D MoS2 Neuromorphic Devices for Brain‐Like Computational Systems

Hardware implementation of artificial synapses/neurons with 2D solid‐state devices is of great significance for nanoscale brain‐like computational systems. Here, 2D MoS₂ synaptic/neuronal transistors are fabricated by using poly(vinyl alcohol) as the laterally coupled, proton‐conducting electrolytes. Fundamental synaptic functions, such as an excitatory postsynaptic current, paired‐pulse facilitation, and a dynamic filter for information transmission of biological synapse, are successfully emulated. Most importantly, with multiple input gates and one modulatory gate, spiking‐dependent logic operation/modulation, multiplicative neural coding, and neuronal gain modulation are also experimentally demonstrated. The results indicate that the intriguing 2D MoS₂ transistors are also very promising for the next‐generation of nanoscale neuromorphic device applications.     

3D Heteroatom‐Doped Carbon Nanomaterials as Multifunctional Metal‐Free Catalysts for Integrated Energy Devices

Sustainable and cost‐effective energy generation has become crucial for fulfilling present energy requirements. For this purpose, the development of cheap, scalable, efficient, and reliable catalysts is essential. Carbon‐based heteroatom‐doped, 3D, and mesoporous electrodes are very promising as catalysts for electrochemical energy conversion and storage. Various carbon allotropes doped with a variety of heteroatoms can be utilized for cost‐effective mass production of electrode materials. 3D porous carbon electrodes provide multiple advantages, such as large surface area, maximized exposure to active sites, 3D conductive pathways for efficient electron transport, and porous channels to facilitate electrolyte diffusion. However, it is challenging to synthesize and functionalize isotropic 3D carbon structures. Here, various synthesis processes of 3D porous carbon materials are summarized to understand how their physical and chemical properties together with heteroatom doping dictate the electrochemical catalytic performance. Prospects of attractive 3D carbon structural materials for energy conversion and efficient integrated energy systems are also discussed.     

Bioinspired 2D Nanomaterials for Sustainable Applications

The increasing demand for constructing ecological civilization and promoting socially sustainable development has encouraged scientists to develop bioinspired materials with required properties and functions. By bringing science and nature together, plenty of novel materials with extraordinary properties can be created by learning the best from natural species. In combination with the exceptional features of 2D nanomaterials, bioinspired 2D nanomaterials and technologies have delivered significant achievements. Here, the progress over the past decade in bioinspired 2D photonic structures, energy nanomaterials, and superwetting materials, is summarized, together with the challenges and opportunities in developing bioinspired materials for sustainable energy and environmental technologies.     

Self‐Formed Channel Devices Based on Vertically Grown 2D Materials with Large‐Surface‐Area and Their Potential for Chemical Sensor Applications

2D layered materials with sensitive surfaces are promising materials for use in chemical sensing devices, owing to their extremely large surface‐to‐volume ratios. However, most chemical sensors based on 2D materials are used in the form of laterally defined active channels, in which the active area is limited to the actual device dimensions. Therefore, a novel approach for fabricating self‐formed active‐channel devices is proposed based on 2D semiconductor materials with very large surface areas, and their potential gas sensing ability is examined. First, the vertical growth phenomenon of SnS₂ nanocrystals is investigated with large surface area via metal‐assisted growth using prepatterned metal electrodes, and then self‐formed active‐channel devices are suggested without additional pattering through the selective synthesis of SnS₂ nanosheets on prepatterned metal electrodes. The self‐formed active‐channel device exhibits extremely high response values (>2000% at 10 ppm) for NO₂ along with excellent NO₂ selectivity. Moreover, the NO₂ gas response of the gas sensing device with vertically self‐formed SnS₂ nanosheets is more than two orders of magnitude higher than that of a similar exfoliated SnS₂‐based device. These results indicate that the facile device fabrication method would be applicable to various systems in which surface area plays an important role.     

In‐Plane Isotropic/Anisotropic 2D van der Waals Heterostructures for Future Devices

Mono‐ to few‐layers of 2D semiconducting materials have uniquely inherent optical, electronic, and magnetic properties that make them ideal for probing fundamental scientific phenomena up to the 2D quantum limit and exploring their emerging technological applications. This Review focuses on the fundamental optoelectronic studies and potential applications of in‐plane isotropic/anisotropic 2D semiconducting heterostructures. Strong light–matter interaction, reduced dimensionality, and dielectric screening in mono‐ to few‐layers of 2D semiconducting materials result in strong many‐body interactions, leading to the formation of robust quasiparticles such as excitons, trions, and biexcitons. An in‐plane isotropic nature leads to the quasi‐2D particles, whereas, an anisotropic nature leads to quasi‐1D particles. Hence, in‐plane isotropic/anisotropic 2D heterostructures lead to the formation of quasi‐1D/2D particle systems allowing for the manipulation of high binding energy quasi‐1D particle populations for use in a wide variety of applications. This Review emphasizes an exciting 1D–2D particles dynamic in such heterostructures and their potential for high‐performance photoemitters and exciton–polariton lasers. Moreover, their scopes are also broadened in thermoelectricity, piezoelectricity, photostriction, energy storage, hydrogen evolution reactions, and chemical sensor fields. The unique in‐plane isotropic/anisotropic 2D heterostructures may open the possibility of engineering smart devices in the nanodomain with complex opto‐electromechanical functions.     

Multifunctional Cellular Materials Based on 2D Nanomaterials: Prospects and Challenges

Recent advances in emerging 2D nanomaterial‐based cellular materials (2D‐CMs) open up new opportunities for the development of next generation cellular solids with exceptional properties. Herein, an overview of the current research status of 2D‐CMs is provided and their future opportunities are highlighted. First, the unique features of 2D nanomaterials are introduced to illustrate why these nanoscale building blocks are promising for the development of novel cellular materials and what the new features of 2D nanoscale building blocks can offer when compared to their 0D and 1D counterparts. An in‐depth discussion on the structure–property relationships of 2D‐CMs is then provided, and the remarkable functions that can be achieved by engineering their cellular architecture are highlighted. Additionally, the use of 2D‐CMs to tackle key challenges in different practical applications is demonstrated. In conclusion, a personal perspective on the challenges and future research directions of 2D‐CMs is given.     

Recent Advances in 2D Inorganic Nanomaterials for SERS Sensing

Surface‐enhanced Raman spectroscopy is a powerful and sensitive analytical tool that has found application in chemical and biomolecule analysis and environmental monitoring. Since its discovery in the early 1970s, a variety of materials ranging from noble metals to nanostructured materials have been employed as surface enhanced Raman scattering (SERS) substrates. In recent years, 2D inorganic materials have found wide use in the development of SERS‐based chemical sensors owing to their unique thickness dependent physico‐chemical properties with enhanced chemical‐based charge‐transfer processes. Here, recent advances in the application of various 2D inorganic nanomaterials, including graphene, boron nitride, semiconducting metal oxides, and transition metal chalcogenides, in chemical detection via SERS are presented. The background of the SERS concept, including its basic theory and sensing mechanism, along with the salient features of different nanomaterials used as substrates in SERS, extending from monometallic nanoparticles to nanometal oxides, is comprehensively discussed. The importance of 2D inorganic nanomaterials in SERS enhancement, along with their application toward chemical detection, is explained in detail with suitable examples and illustrations. In conclusion, some guidelines are presented for the development of this promising field in the future.     

Chemical Patterning of High‐Mobility Semiconducting 2D Bi2O2Se Crystals for Integrated Optoelectronic Devices

Patterning of high‐mobility 2D semiconducting materials with unique layered structures and superb electronic properties offers great potential for batch fabrication and integration of next‐generation electronic and optoelectronic devices. Here, a facile approach is used to achieve accurate patterning of 2D high‐mobility semiconducting Bi₂O₂Se crystals using dilute H₂O₂ and protonic mixture acid as efficient etchants. The 2D Bi₂O₂Se crystal after chemical etching maintains a high Hall mobility of over 200 cm² V^?1 s^?1 at room temperature. Centimeter‐scale well‐ordered arrays of 2D Bi₂O₂Se with tailorable configurations are readily obtained. Furthermore, integrated photodetectors based on 2D Bi₂O₂Se arrays are fabricated, exhibiting excellent air stability and high photoresponsivity of ≈2000 A W^?1 at 532 nm. These results are one step towards the practical application of ultrathin 2D integrated digital and optoelectronic circuits.     

Regulating the Electrical Behaviors of 2D Inorganic Nanomaterials for Energy Applications

Recent years have witnessed great developments in inorganic 2D nanomaterials for their unique dimensional confinement and diverse electronic energy bands. Precisely regulating their intrinsic electrical behaviors would bring superior electrical conductivity, rendering 2D nanomaterials ideal candidates for active materials in electrochemical applications when combined with the excellent reaction activity from the inorganic lattice. This Concept focuses on highly conducting inorganic 2D nanomaterials, including intrinsic metallic 2D nanomaterials and artificial highly conductive 2D nanomaterials. The intrinsic metallicity of 2D nanomaterials is derived from their closely packed atomic structures that ensure maximum overlapping of electron orbitals, while artificial highly conductive 2D nanomaterials could be achieved by designed methodologies of surface modification, intralayer ion doping, and lattice strain, in which atomic‐scale structural modulation plays a vital role in realizing conducting behaviors. Benefiting from fast electron transfer, high reaction activity, as well as large surface areas arising from the 2D inorganic lattice, highly conducting 2D nanomaterials open up prospects for enhancing performance in electrochemical catalysis and electrochemical capacitors. Conductive 2D inorganic nanomaterials promise higher efficiency for electrochemical applications of energy conversion and storage.     

Hybridized 2D Nanomaterials Toward Highly Efficient Photocatalysis for Degrading Pollutants: Current Status and Future Perspectives

Organic pollutants including industrial dyes and chemicals and agricultural waste have become a major environmental issue in recent years. As an alternative to simple adsorption, photocatalytic decontamination is an efficient and energy‐saving technology to eliminate these pollutants from water environment, utilizing the energy of external light, and unique function of photocatalysts. Having a large specific surface area, numerous active sites, and varied band structures, 2D nanosheets have exhibited promising applications as an efficient photocatalyst for degrading organic pollutants, particularly hybridization with other functional components. The novel hybridization of 2D nanomaterials with various functional species is summarized systematically with emphasis on their enhanced photocatalytic activities and outstanding performances in environmental remediation. First, the mechanism of photocatalytic degradation is given for discussing the advantages/shortcomings of regular 2D materials and identifying the importance of constructing hybrid 2D photocatalysts. An overview of several types of intensively investigated 2D nanomaterials (i.e., graphene, g‐C₃N₄, MoS₂, WO₃, Bi₂O₃, and BiOX) is then given to indicate their hybridized methodologies, synergistic effect, and improved applications in decontamination of organic dyes and other pollutants. Finally, future research directions are rationally suggested based on the current challenges.     

2D Transition‐Metal‐Dichalcogenide‐Nanosheet‐Based Composites for Photocatalytic and Electrocatalytic Hydrogen Evolution Reactions

Hydrogen (H₂) is one of the most important clean and renewable energy sources for future energy sustainability. Nowadays, photocatalytic and electrocatalytic hydrogen evolution reactions (HERs) from water splitting are considered as two of the most efficient methods to convert sustainable energy to the clean energy carrier, H₂. Catalysts based on transition metal dichalcogenides (TMDs) are recognized as greatly promising substitutes for noble‐metal‐based catalysts for HER. The photocatalytic and electrocatalytic activities of TMD nanosheets for the HER can be further improved after hybridization with many kinds of nanomaterials, such as metals, oxides, sulfides, and carbon materials, through different methods including the in situ reduction method, the hot‐injection method, the heating‐up method, the hydro(solvo)thermal method, chemical vapor deposition (CVD), and thermal annealing. Here, recent progress in photocatalytic and electrocatalytic HERs using 2D TMD‐based composites as catalysts is discussed.     

Self‐Assembled Nickel Pyrophosphate‐Decorated Amorphous Bimetal Hydroxides 2D‐on‐2D Nanostructure for High‐Energy Solid‐State Asymmetric Supercapacitor

To obtain a supercapacitor with a remarkable specific capacitance and rate performance, a cogent design and synthesis of the electrode material containing abundant active sites is necessary. In present work, a scalable strategy is developed for preparing 2D‐on‐2D nanostructures for high‐energy solid‐state asymmetric supercapacitors (ASCs). The self‐assembled vertically aligned microsheet‐structured 2D nickel pyrophosphate (Ni₂P₂O₇) is decorated with amorphous bimetallic nickel cobalt hydroxide (NiCo‐OH) to form a 2D‐on‐2D nanostructure arrays electrode. The resulting Ni₂P₂O₇/NiCo‐OH 2D‐on‐2D array electrode exhibits peak specific capacity of 281 mA hg^?1 (4.3 F cm^?2), excellent rate capacity, and cycling stability over 10 000 charge–discharge cycles in the positive potential range. The excellent electrochemical features can be attributed to the high electrical conductivity and 2D layered structure of Ni₂P₂O₇ along with the Faradic capacitance of the amorphous NiCo‐OH nanosheets. The constructed Ni₂P₂O₇/NiCo‐OH//activated carbon based solid‐state ASC cell operates in a high voltage window of 1.8 V with an energy density of 78 Wh kg^?1 (1.065 mWh cm^?3) and extraordinary cyclic stability over 10 000 charge–discharge cycles with excellent energy efficiency (75%–80%) over all current densities. The excellent electrochemical performance of the prepared electrode and solid‐state ASC device offers a favorable and scalable pathway for developing advanced electrodes.     

Structural Phase Transition Effect on Resistive Switching Behavior of MoS2‐Polyvinylpyrrolidone Nanocomposites Films for Flexible Memory Devices

The 2H phase and 1T phase coexisting in the same molybdenum disulfide (MoS₂) nanosheets can influence the electronic properties of the materials. The 1T phase of MoS₂ is introduced into the 2H‐MoS₂ nanosheets by two‐step hydrothermal synthetic methods. Two types of nonvolatile memory effects, namely write‐once read‐many times memory and rewritable memory effect, are observed in the flexible memory devices with the configuration of Al/1T@2H‐MoS₂‐polyvinylpyrrolidone (PVP)/indium tin oxide (ITO)/polyethylene terephthalate (PET) and Al/2H‐MoS₂‐PVP/ITO/PET, respectively. It is observed that structural phase transition in MoS₂ nanosheets plays an important role on the resistive switching behaviors of the MoS₂‐based device. It is hoped that our results can offer a general route for the preparation of various promising nanocomposites based on 2D nanosheets of layered transition metal dichalcogenides for fabricating the high performance and flexible nonvolatile memory devices through regulating the phase structure in the 2D nanosheets.     

In‐Plane Potential Gradient Induces Low Frictional Energy Dissipation during the Stick‐Slip Sliding on the Surfaces of 2D Materials

Understanding the nanoscale friction properties of 2D materials and further manipulating their friction behaviors is of great significance for the development of various micro/nanodevices. Recent studies, taking advantage of the close relationship between friction and surface charges, use an external out‐of‐plane electric field to control the interfacial friction. Nevertheless, friction increases with the application of the out‐of‐plane electric field in most cases. Here, an in‐plane potential gradient is applied for the investigation of the contribution of electric charges to friction on the surfaces of 2D materials. Experimental results show that the friction between an atomic force microscope tip and the flakes of 2D materials decreases with the application of the in‐plane potential gradient, and the higher the potential gradient, the greater the friction decrease. By comparing the in situ atomic‐level stick‐slip maps before and after the application of the in‐plane potential gradient, it is proposed that the promotion of low friction dissipative motion during the stick‐slip process owing to the presence of the potential gradient gives rise to the friction reduction. These results not only help to reveal the origin of friction, but also provide a novel way to manipulate friction through an electrically‐controlled sliding process.