Wafer-Scale Transfer of MXene Films with Enhanced Device Performance via 2D Liquid Intercalation.

Wafer-scale transfer processes of 2D materials significantly expand their application space in scalable microelectronic devices with excellent and tunable properties through van der Waals (vdW) stacking. Unlike many 2D materials, wafer-scale transfer of MXene films for vdW contact engineering has not yet been reported. With their rich surface chemistry and tunable properties, the transfer of MXenes can enable enormous possibilities in electronic devices using interface engineering. Taking advantage of the MXene hydrophilic surface, a straightforward, green, and fast process for the transfer of MXene films at the wafer scale (4-inch) is developed. Uniform vdW stacking of several types of large-area heterojunctions including MXene/MXene (Ti3C2Tx, Nb2CTx, and V2CTx), MXene/MoS2, and MXene/Au is further demonstrated. Multilayer support is applied to minimize damage or deformation in the transfer process of patterned Ti3C2Tx film. It allows us to fabricate thin film transistors and manipulate the MXene/MoS2 interface through the intercalation of various 2D liquids. Particularly noteworthy is the significant enhancement of the interfacial carrier transfer efficiency by ≈2 orders of magnitude using hydrogen iodide (HI) intercalation. This finding indicates a wide range of possibilities for interface engineering by transferring MXene films and employing liquid-assisted interfacial intercalation.

Anisotropic Superconducting Nb2 CTx MXene Processed by Atomic Exchange at the Wafer Scale.

Superconductivty has recently been induced in MXenes through surface modification. However, the previous reports have mostly been based on powders or cold-pressed pellets, with no known reports on the intrinsic superconsucting properties of MXenes at the nanoale. Here, it is developed a high-temperature atomic exchange process in NH3 atmosphere which induces superconductivity in either singleflakes or thin films of Nb2 CTx MXene. The exchange process between nitrogen atoms and fluorine, carbon, and oxygen atoms in the MXene lattice and related structural adjustments are studied using both experiments and density functional theory. Using either single-flake or thin-film devices, an anisotropic magnetic response of the 2D superconducting transformation has been successfully revealed. The anisotropic superconductivity is further demonstrated using superconducting thin films uniformly deposited over a 4 in. wafers, which opens up the possibility of scalable MXene-based superconducting devices.

Peptide Gel Electrolytes for Stabilized Zn Metal Anodes.

The rechargeable aqueous Zn ion battery (AZIB) is considered a promising candidate for future energy storage applications due to its intrinsic safety features and low cost. However, Zn dendrites and side reactions (e.g., corrosion, hydrogen evolution reaction, and inactive side product (Zn hydroxide sulfate) formation) at the Zn metal anode have been serious obstacles to realizing a satisfactory AZIB performance. The application of gel electrolytes is a common strategy for suppressing these problems, but the normally used highly cross-linked polymer matrix (e.g., polyacrylamide (PAM)) brings additional difficulties for battery assembly and recycling. Herein, we have developed a gel electrolyte for Zn metal anode stabilization, where a peptide matrix, a highly biocompatible material, is used for gel construction. Various experiments and simulations elucidate the sulfate anion-assisted self-assembly gel formation and its effect in stabilizing Zn metal anodes. Unlike polymer gel electrolytes, the peptide gel electrolyte can reversibly transform between gel and liquid states, thus facilitating the gel-involved battery assembly and recycling. Furthermore, the peptide gel electrolyte provides fast Zn ion diffusion (comparable to conventional liquid electrolyte) while suppressing side reactions and dendrite growth, thus achieving highly stable Zn metal anodes as validated in various cell configurations. We believe that our concept of gel electrolyte design will inspire more future directions for Zn metal anode protection based on gel electrolyte design.

Large-Area Metal-Semiconductor Heterojunctions Realized via MXene-Induced Two-Dimensional Surface Polarization.

Direct MXene deposition on large-area 2D semiconductor surfaces can provide design versatility for the fabrication of MXene-based electronic devices (MXetronics). However, it is challenging to deposit highly uniform wafer-scale hydrophilic MXene films (e.g., Ti3C2Tx) on hydrophobic 2D semiconductor channel materials (e.g., MoS2). Here, we demonstrate a modified drop-casting (MDC) process for the deposition of MXene on MoS2 without any pretreatment, which typically degrades the quality of either MXene or MoS2. Different from the traditional drop-casting method, which usually forms rough and thick films at the micrometer scale, our MDC method can form an ultrathin Ti3C2Tx film (ca. 10 nm) based on a MXene-introduced MoS2 surface polarization phenomenon. In addition, our MDC process does not require any pretreatment, unlike MXene spray-coating that usually requires a hydrophilic pretreatment of the substrate surface before deposition. This process offers a significant advantage for Ti3C2Tx film deposition on UV-ozone- or O2-plasma-sensitive surfaces. Using the MDC process, we fabricated wafer-scale n-type Ti3C2Tx-MoS2 van der Waals heterojunction transistors, achieving an average effective electron mobility of ∼40 cm2·V-1·s-1, on/off current ratios exceeding 104, and subthreshold swings of under 200 mV·dec-1. The proposed MDC process can considerably enhance the applications of MXenes, especially the design of MXene/semiconductor nanoelectronics.

MoS2 -Mediated Epitaxial Plating of Zn Metal Anodes.

Metal-based anodes (Li, Zn, etc.) are regarded as promising solutions for next-generation advanced batteries due to their high theoretical specific capacities. However, most of these metal anodes suffer from dendrite growth, which severely restricts their practical applications. Recently, epitaxial anode metal deposition by choosing a suitable substrate has received tremendous attention as an effective strategy to suppress dendrites. However, the epitaxial relationship between plated metal and the substrate has been a subject of debate. Herein, large-area, mono-orientated 2D material (MoS2 ) is used, for the first time, to electrodeposit truly epitaxial Zn anodes. The continuous (without edges) mono-orientated MoS2 films are shown to be an effective strategy for suppressing metal dendrites. In addition, the epitaxial nature of the electrodeposited Zn anode is proven by pole figure analysis, which provides the first demonstration of truly epitaxial Zn anode growth over large area as metal anode protection strategy through epitaxy.

A Sustainable NH4 + Ion Battery by Electrolyte Engineering.

Aqueous ammonium ion battery is a promising sustainable energy storage system. However, the side reactions originating from electrolytes (the water decomposition and host material dissolution) preclude its practical applications. Unlike the metal-based aqueous batteries, the idea of "ultrahigh concentrated electrolyte" is not feasible due to the strong hydrolysis of ammonium ions. Therefore, we propose an effective and sustainable strategy for the water hydrogen bond network modulation by adding sucrose into the electrolytes. The sucrose can form sucrose-water hydrogen bond networks to break the continuous water hydrogen bond network, thereby inhibiting water decomposition significantly. Moreover, the weak hydrogen bond interaction between ammonium and sucrose facilitates rapid ion migration, leading to an improved ionic conductivity. This work presents a new electrolyte modulating strategy for the practical application of aqueous ammonium ion batteries.

MXenes for Energy Harvesting.

Energy harvesting modules play an increasingly important role in the development of autonomous self-powered microelectronic devices. MXenes (i.e., 2D transition metal carbide/nitride) have recently emerged as promising candidates for energy applications due to their excellent electronic conductivity, large specific surface area, and tunable properties. Herein, a perspective on using MXenes to harvest energy from various sources in the environment is presented. First, the characteristics of MXenes that facilitate energy capturing are systematically introduced and the preparation strategies of MXenes and their derived nanostructures tailored toward such applications are summarized. Subsequently, the harvesting mechanism of different energy sources (e.g., solar energy, thermoelectric energy, triboelectric energy, piezoelectric energy, salinity-gradient energy, electrokinetic energy, ultrasound energy, and humidity energy) are discussed. Then, the recent progress of MXene-based nanostructures in energy harvesting, as well as their applications, is introduced. Finally, opinions on the existing challenges and future directions of MXene-based nanostructure for energy harvesting are presented.

Growth of 2D Materials at the Wafer Scale.

Wafer-scale growth has become a critical bottleneck for scaling up applications of van der Waal (vdW) layered 2D materials in high-end electronics and optoelectronics. Most vdW 2D materials are initially obtained through top-down synthesis methods, such as exfoliation, which can only prepare small flakes on a micrometer scale. Bottom-up growth can enable 2D flake growth over a large area. However, seamless merging of these flakes to form large-area continuous films with well-controlled layer thickness and lattice orientation is still a significant challenge. This review briefly introduces several vdW layered 2D materials covering their lattice structures, representative physical properties, and potential roles in large-scale applications. Then, several methods used to grow vdW layered 2D materials at the wafer scale are reviewed in depth. In particular, three strategies are summarized that enable 2D film growth with a single-crystalline structure over the whole wafer: growth of an isolated domain, growth of unidirectional domains, and conversion of oriented precursors. After that, the progress in using wafer-scale 2D materials in integrated devices and advanced epitaxy is reviewed. Finally, future directions in the growth and scaling of vdW layered 2D materials are discussed.

Controlled Deposition of Zinc-Metal Anodes via Selectively Polarized Ferroelectric Polymers.

Aqueous zinc-ion batteries are regarded as ideal candidates for stationary energy-storage systems due to their low cost and high safety. However, zinc can readily grow into dendrites, leading to limited cycling performance and quick failure of the batteries. Herein, a novel strategy is proposed to mitigate this dendrite problem, in which a selectively polarized ferroelectric polymer material (poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE))) is employed as a surface protective layer on zinc anodes. Such a polarized ferroelectric polymer layer can enable a locally concentrated zinc-ion distribution along the coated surface and thus enable the horizontal growth of zinc plates. As a result, symmetrical zinc batteries using such anodes exhibit long cycling lifespan at 0.2 mA cm-2 , 0.2 mAh cm-2 for 2000 h, and a high rate performance up to 15 mA cm-2 . Also, the full cell (including a Zn-MnO2 battery and a zinc-ion capacitor) based on this anode is demonstrated. This work provides a novel strategy to protect the zinc anode and even other metal anodes exploiting polymer ferroelectricity.

High-Yield Ti3 C2 Tx MXene-MoS2 Integrated Circuits.

It is very challenging to employ solution-processed conducting films in large-area ultrathin nanoelectronics. Here, spray-coated Ti3 C2 Tx MXene films as metal contacts are successfully integrated into sub-10 nm gate oxide 2D MoS2 transistor circuits. Ti3 C2 Tx films are spray coated on glass substrates followed by vacuum annealing. Compared to the as-prepared sample, vacuum annealed films exhibit a higher conductivity (≈11 000 S cm-1 ) and a lower work function (≈4.5 eV). Besides, the annealed Ti3 C2 Tx film can be patterned through a standard cleanroom process without peeling off. The annealed Ti3 C2 Tx film shows a better band alignment for n-type transport in MoS2 channel with small work function mismatch of 0.06 eV. The MoS2 film can be uniformly transferred on the patterned Ti3 C2 Tx surface and then readily processed through the cleanroom process. A large-area array of Ti3 C2 Tx MXene-MoS2 transistors is fabricated using different dielectric thicknesses and semiconducting channel sizes. High yield and stable performance for these transistor arrays even with an 8 nm-thick dielectric layer are demonstrated. Besides, several circuits are demonstrated, including rectifiers, negative-channel metal-oxide-semiconductor (NMOS) inverters, and voltage-shift NMOS inverters. Overall, this work indicates the tremendous potential for solution-processed Ti3 C2 Tx MXene films in large-area 2D nanoelectronics.