Co-Solvent Electrolyte Engineering for Stable Anode-Free Zinc Metal Batteries.

Anode-free metal batteries can in principle offer higher energy density, but this requires them to have extraordinary Coulombic efficiency (>99.7%). Although Zn-based metal batteries are promising for stationary storage, the parasitic side reactions make anode-free batteries difficult to achieve in practice. In this work, a salting-in-effect-induced hybrid electrolyte is proposed as an effective strategy that enables both a highly reversible Zn anode and good stability and compatibility toward various cathodes. The as-prepared electrolyte can also work well under a wide temperature range (i.e., from -20 to 50 °C). It is demonstrated that in the presence of propylene carbonate, triflate anions are involved in the Zn2+ solvation sheath structure, even at a low salt concentration (2.14 M). The unique solvation structure results in the reduction of anions, thus forming a hydrophobic solid electrolyte interphase. The waterproof interphase along with the decreased water activity in the hybrid electrolyte effectively prevents side reactions, thus ensuring a stable Zn anode with an unprecedented Coulombic efficiency (99.93% over 500 cycles at 1 mA cm-2). More importantly, we design an anode-free Zn metal battery that exhibits excellent cycling stability (80% capacity retention after 275 cycles at 0.5 mA cm-2). This work provides a universal strategy to design co-solvent electrolytes for anode-free Zn metal batteries.

Surface and Interface Engineering of Zn Anodes in Aqueous Rechargeable Zn-Ion Batteries.

Rechargeable zinc-ion batteries (ZIBs) have shown great potential as an alternative to lithium-ion batteries. The ZIBs utilize Zn metal as the anode, which possesses many advantages such as low cost, high safety, eco-friendliness, and high capacity. However, on the other hand, the Zn anode also suffers from many issues, including dendritic growth, corrosion, and passivation. These issues are largely related to the surface and interface properties of the Zn anode. Many efforts have therefore been devoted to the modification of the Zn anode, aiming to eliminate the above-mentioned problems. This review gives a comprehensive summary on the mechanism behind these issues as well as the recent progress on Zn anode modification with focus on the strategies of surface and interface engineering, covering the design and application of both the Zn anode supports and surface protective layers, along with abundant examples. In addition, the promising research directions and perspective on these strategies are also presented.

Aqueous Zinc-Ion Storage in MoS2 by Tuning the Intercalation Energy.

Aqueous Zn-ion batteries present low-cost, safe, and high-energy battery technology but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn2+ storage materials through intercalation energy tuning. Using MoS2 as a model system, we show both experimentally and theoretically that even hosts with an originally poor Zn2+ diffusivity can allow fast Zn2+ diffusion. Through simple interlayer spacing and hydrophilicity engineering that can be experimentally achieved by oxygen incorporation, the Zn2+ diffusivity is boosted by 3 orders of magnitude, effectively enabling the otherwise barely active MoS2 to achieve a high capacity of 232 mAh g-1, which is 10 times that of its pristine form. The strategy developed in our work can be generally applied for enhancing the ion storage capacity of metal chalcogenides and other layered materials, making them promising cathodes for challenging multivalent ion batteries.

MXene Derived Metal-Organic Frameworks.

Synthesis of nanoscale metal-organic frameworks (MOFs) is a highly challenging task because conventional soluble metal salt precursors are not easy to manipulate spatially, thus normally leading to bulk MOFs. In the present work, V2CTx MXene is demonstrated for the first time as a metal precursor to fabricate two-dimensional (2D) MOF nanosheets, whose thickness (6 to 18 nm) can be tuned by varying the reaction temperature. The highly electronegative surface atoms of MXene and sufficient accessible attacking sites for ligands are responsible for the evolution of 2D MOF nanosheets. Moreover, highly oriented and smooth MOF thin films have been grown based on these nanosheets using a convenient spin coating process. With the impregnation of nonvolatile H3PO4, the MOF thin film exhibits a proton-conducting property. This study demonstrates that high-quality 2D MOF sheets and thin films are enabled by 2D MXene precursors. We believe that the high-quality MOF films prepared in this study pave the way for many device applications.

Efficient Overall Water-Splitting Electrocatalysis Using Lepidocrocite VOOH Hollow Nanospheres.

Herein we report the control synthesis of lepidocrocite VOOH hollow nanospheres and further their applications in electrocatalytic water splitting for the first time. By tuning the surface area of the nanospheres, the optimal performance can be achieved with low overpotentials of 270 mV for the oxygen evolution reaction (OER) and 164 mV for the hydrogen evolution reaction (HER) at 10 mA cm-2 in 1 m KOH, respectively. Furthermore, when used as both the anode and cathode for overall water splitting, a low cell voltage of 1.62 V is required to reach the current density of 10 mA cm-2 , making the VOOH hollow nanospheres an efficient alternative to water splitting.

MXene-Coated Membranes for Autonomous Solar-Driven Desalination.

Clean water supply in off-grid locations remains a stumbling stone for socio-economic development in remote areas where solar energy is abundant. In this regard, several technologies have already introduced various solutions to the off-grid freshwater predicament; however, most of them are either costly or complex to operate. Nonetheless, photothermal membrane distillation (PMD) has emerged as a promising candidate with great potential to be autonomously driven by solar energy. Instead of using energy-intensive bulk feed heating in conventional MD systems, PMD membranes can directly harvest the incident solar light at the membrane interface as an alternative driving energy resource for the desalination process. Because of its excellent photothermal properties and stability in ionic environments, herein, Ti3C2Tx MXene was coated onto commercial polytetrafluoroethylene (PTFE) membranes to allow for a self-heated PMD process. An average water vapor flux of 0.77 kg/m2 h with an excellent temporal response under intermitting lighting and a photothermal efficiency of 65.3% were achieved by the PMD membrane under one-sun irradiation for a feed salinity of 0.36 g/L. Naturally, the efficiency of the process decreased with higher feed concentrations due to the reduction of the evaporation rate and the scattering of incident sunlight toward the membrane photothermal surface, especially at rates above 10 g/L. Notably, with such performance, 1 m2 of the MXene-coated PMD membrane can fulfill the recommended daily potable water intake for a household, that is, ca. 6 L/day.

MXenes for Rechargeable Batteries Beyond the Lithium-Ion.

Research on next-generation battery technologies (beyond Li-ion batteries, or LIBs) has been accelerating over the past few years. A key challenge for these emerging batteries has been the lack of suitable electrode materials, which severely limits their further developments. MXenes, a new class of 2D transition metal carbides, carbonitrides, and nitrides, are proposed as electrode materials for these emerging batteries due to several desirable attributes. These attributes include large and tunable interlayer spaces, excellent hydrophilicity, extraordinary conductivity, compositional diversity, and abundant surface chemistries, making MXenes promising not only as electrode materials but also as other components in the cells of emerging batteries. Herein, an overview and assessment of the utilization of MXenes in rechargeable batteries beyond LIBs, including alkali-ion (e.g., Na+ , K+ ) storage, multivalent-ion (e.g., Mg2+ , Zn2+ , and Al3+ ) storage, and metal batteries are presented. In particular, the synthetic strategies and properties of MXenes that enable MXenes to play various roles as electrodes, metal anode protective layers, sulfur hosts, separator modification layers, and conductive additives in these emerging batteries are discussed. Moreover, a perspective on promising future research directions on MXenes and MXene-based materials, ranging from material design and processing, fundamental understanding of the reaction mechanisms, to device performance optimization strategies is provided.

Selective Toluene Detection with Mo2CTx MXene at Room Temperature.

MXenes are a promising class of two-dimensional materials with several potential applications, including energy storage, catalysis, electromagnetic interference shielding, transparent electronics, and sensors. Here, we report a novel Mo2CTx MXene sensor for the successful detection of volatile organic compounds (VOCs). The proposed sensor is a chemiresistive device fabricated on a Si/SiO2 substrate using photolithography. The impact of various MXene process conditions on the performance of the sensor is evaluated. The VOCs, such as toluene, benzene, ethanol, methanol, and acetone, are studied at room temperature with varying concentrations. Under optimized conditions, the sensor demonstrates a detection limit of 220 ppb and a sensitivity of 0.0366 Ω/ppm at a toluene concentration of 140 ppm. It exhibits an excellent selectivity toward toluene against the other VOCs. Ab initio simulations demonstrate selectivity toward toluene in line with the experimental results.

MXene-Derived Ferroelectric Crystals.

This study demonstrates the first synthesis of MXene-derived ferroelectric crystals. Specifically, high-aspect-ratio potassium niobate (KNbO3 ) ferroelectric crystals is successfully synthesized using 2D Nb2 C, MXene, and potassium hydroxide (KOH) as the niobium and potassium source, respectively. Material analysis confirms that a KNbO3 orthorhombic phase with Amm2 symmetry is obtained. Additionally, ferroelectricity in KNbO3 is confirmed using standard ferroelectric, dielectric, and piezoresponse force microscopy measurements. The KNbO3 crystals exhibit a saturated polarization of ≈21 µC cm-2 , a remnant polarization of ≈17 µC cm-2 , and a coercive field of ≈50 kV cm-1 . This discovery illustrates that the 2D nature of MXenes can be exploited to grow ferroelectric crystals.

Two-Dimensional Ti3C2Tx MXene Membranes as Nanofluidic Osmotic Power Generators.

Salinity-gradient is emerging as one of the promising renewable energy sources but its energy conversion is severely limited by unsatisfactory performance of available semipermeable membranes. Recently, nanoconfined channels, as osmotic conduits, have shown superior energy conversion performance to conventional technologies. Here, ion selective nanochannels in lamellar Ti3C2Tx MXene membranes are reported for efficient osmotic power harvesting. These subnanometer channels in the Ti3C2Tx membranes enable cation-selective passage, assisted with tailored surface terminal groups, under salinity gradient. A record-high output power density of 21 W·m-2 at room temperature with an energy conversion efficiency of up to 40.6% is achieved by controlled surface charges at a 1000-fold salinity gradient. In addition, due to thermal regulation of surface charges and ionic mobility, the MXene membrane produces a large thermal enhancement at 331 K, yielding a power density of up to 54 W·m-2. The MXene lamellar structure, coupled with its scalability and chemical tunability, may be an important platform for high-performance osmotic power generators.