Highly Sensitive Temperature-Pressure Bimodal Aerogel with Stimulus Discriminability for Human Physiological Monitoring.

Multimodal sensor with high sensitivity, accurate sensing resolution, and stimuli discriminability is very desirable for human physiological state monitoring. A dual-sensing aerogel is fabricated with independent pyro-piezoresistive behavior by leveraging MXene and semicrystalline polymer to assemble shrinkable nanochannel structures inside multilevel cellular walls of aerogel for discriminable temperature and pressure sensing. The shrinkable nanochannels, controlled by the melt flow-triggered volume change of semicrystalline polymer, act as thermoresponsive conductive channels to endow the pyroresistive aerogel with negative temperature coefficient of resistance of -10.0% °C-1 and high accuracy within 0.2 °C in human physiological temperature range of 30-40 °C. The flexible cellular walls, working as pressure-responsive conductive channels, enable the piezoresistive aerogel to exhibit a pressure sensitivity up to 777 kPa-1 with a detectable pressure limit of 0.05 Pa. The pyro-piezoresistive aerogel can detect the temperature-dependent characteristics of pulse pressure waveforms from artery vessels under different human body temperature states.

Biomimetic Dual Absorption-Adsorption Networked MXene Aerogel-Pump for Integrated Water Harvesting and Power Generation System.

Harvesting atmospheric water and converting it into electricity play vital roles in advancing next-generation energy conversion systems. However, the current water harvester systems suffer from a weak water capture ability and poor recyclability due to high diffusion barriers and low sorption kinetics, which significantly limit their practical application. Herein, we drew inspiration from the natural "Pump effect" observed in wood and successfully developed a dual "absorption-adsorption" networked MXene aerogel atmospheric water harvester (MAWH) through ice templating and confining LiCl processes, thereby serving multiple purposes of clean water production, passive dehumidification, and power generation. The MAWH benefits from the dual H-bond network of MXene and cellulose nanocrystals (absorption network) and the hygroscopic properties of lithium chloride (adsorption network). Furthermore, its aligned wood-like channel structure efficiently eliminates water nucleation near the 3D network, resulting in fast moisture absorption. The developed MAWH demonstrates a high moisture absorption ability of 3.12 g g-1 at 90% relative humidity (RH), featuring rapid vapor transport rates and durable cyclic performance. When compared with commercial desiccants such as the 4A molecular sieve and silica gel, the MAWH can reduce the RH from 80% to 20% within just 6 h. Most notably, our integrated MAWH-based water harvesting-power generation system achieves a high voltage of ∼0.12 V at 77% RH, showcasing its potential for practical application. These developed MAWHs are considered as high-performance atmospheric water harvesters in the water collection and power generation field.

Cation-induced Ti3C2Tx MXene@melamine sponge aerogels with large layer spacing and high strength for high-performance supercapacitors.

The self-assembled aerogels are considered as an efficient strategy to address the aggregation and restacking of Ti3C2Tx MXene nanosheets for high-performance supercapacitors. However, the low mechanical strength of the MXene aerogel results in the structural collapse of the self-standing supercapacitor electrode materials. Herein, a low-cost melamine sponge (MS) absorbed different cations (H+, K+, Mg2+, Fe2+, Co2+, Ni2+ and Al3+), serves as a carrier and crosslinker for loading MXene hydrogel induced by the absorbed cations on the skeleton surface and the pores of MS, resulting in the high loading mass MXene aerogels with high mechanical strength. The experimental results show that the Mg-Ti3C2Tx@MS aerogel exhibits the maximum area capacitance of 702.22 mF cm-2 at 3 mA cm-2, and the area capacitance is still 603.12 mF cm-2 even at 100 mA cm-2, indicating the high rate capability with a capacitance retention of 85.89 %. It is worth noting that the constructed asymmetric supercapacitor with activated carbon achieves high energy densities of 104.53 µWh cm-2 and 93.87 µWh cm-2 at 800 µW cm-2 and 7999 µW cm-2, respectively. Furthermore, the asymmetric supercapacitor shows the high cycling stability with 90.2 % capacity retention after 10,000 cycles. This work provides a feasible strategy to prepare Ti3C2Tx MXene aerogels with large layer spacing and high strength for high-performance supercapacitors.

Maximizing Electron Channels Enabled by MXene Aerogel for High-Performance Self-Healable Flexible Electronic Skin.

Among the increasingly popular miniature and flexible smart electronics, two-dimensional materials show great potential in the development of flexible electronics owing to their layered structures and outstanding electrical properties. MXenes have attracted much attention in flexible electronics owing to their excellent hydrophilicity and metallic conductivity. However, their limited interlayer spacing and tendency for self-stacking lead to limited changes in electron channels under external pressure, making it difficult to exploit their excellent surface metal conductivity. We propose a strategy for rapid gas foaming to construct interlayer tunable MXene aerogels. MXene aerogels with rich interlayer network structures generate maximized electron channels under pressure, facilitating the effective utilization of the surface metal properties of MXene; this forms a self-healable flexible pressure sensor with excellent sensing properties such as high sensitivity (1,799.5 kPa-1), fast response time (11 ms), and good cycling stability (>25,000 cycles). This pressure sensor has applications in human body detection, human-computer interaction, self-healing, remote monitoring, and pressure distribution identification. The maximized electron channel design provides a simple, efficient, and scalable method to effectively exploit the excellent surface metal conduction of 2D materials.

Self-supported CsPbBr3/Ti3C2Tx MXene aerogels towards efficient photocatalytic CO2 reduction.

Aerogels, especially MXene aerogels, are an ideal multifunctional platform for developing efficient photocatalysts for CO2 reduction because they are featured by abundant catalytic sites, high electrical conductivity, high gas absorption ability and self-supported structure. However, the pristine MXene aerogel has almost no ability to utilize light, which requires additional photosensitizers to assist it in achieving efficient light harvesting. Herein, we immobilized colloidal CsPbBr3 nanocrystals (NCs) onto the self-supported Ti3C2Tx (where Tx represents surface terminations such as fluorine, oxygen, and hydroxyl groups) MXene aerogels for photocatalytic CO2 reduction. The resultant CsPbBr3/Ti3C2Tx MXene aerogels exhibit a remarkable photocatalytic activity toward CO2 reduction with total electron consumption rate of 112.6 µmol g-1h-1, which is 6.6-fold higher than that of the pristine CsPbBr3 NC powders. The improvement of the photocatalytic performance is presumably attributed to the strong light absorption, effective charge separation and CO2 adsorption in the CsPbBr3/Ti3C2Tx MXene aerogels. This work presents an effective perovskite-based photocatalyst in aerogel form and opens a new avenue for their solar-to-fuel conversions.

Scalable Fabrication of Ti3C2Tx MXene/RGO/Carbon Hybrid Aerogel for Organics Absorption and Energy Conversion.

High aspect ratio two-dimensional Ti3C2Tx MXene flakes with extraordinary mechanical, electrical, and thermal properties are ideal candidates for assembling elastic and conductive aerogels. However, the scalable fabrication of large MXene-based aerogels remains a challenge because the traditional preparation method relies on supercritical drying techniques such as freeze drying, resulting in poor scalability and high cost. Herein, the use of porous melamine foam as a robust template for MXene/reduced graphene oxide aerogel circumvents the volume shrinkage during its natural drying process. Through this approach, we were able to produce large size (up to 600 cm3) MXene-based aerogel with controllable shape. In addition, the aerogels possess an interconnected cellular structure and display resilience up to 70% of compressive strain. Some key features also include high solvent absorption capacity (∼50-90 g g-1), good photothermal conversion ability (an average evaporation rate of 1.48 kg m-2 h-1 for steam generation), and an excellent electrothermal conversion rate (1.8 kg m-2 h-1 at 1 V). More importantly, this passive drying process provides a scalable, convenient, and cost-effective approach to produce high-performance MXene-based aerogels, demonstrating the feasibility of commercial production of MXene-based aerogels toward practical applications.

Superelastic Ti3C2Tx MXene-Based Hybrid Aerogels for Compression-Resilient Devices.

Superelastic aerogels with excellent electrical conductivity, reversible compressibility, and high durability hold great potential for varied emerging applications, ranging from wearable electronics to multifunctional scaffolds. In the present work, superelastic MXene/reduced graphene oxide (rGO) aerogels are fabricated by mixing MXene and GO flakes, followed by a multistep reduction of GO, freeze-casting, and finally an annealing process. By optimizing both the composition and reducing conditions, the resultant aerogel shows a reversible compressive strain of 95%, surpassing all current reported values. The conducting MXene/rGO network provides fast electron transfer and stable structural integrity under compression/release cycles. When assembled into compressible supercapacitors, 97.2% of the capacitance was retained after 1000 compression/release cycles. Moreover, the high conductivity and porous structure also enabled the fabrication of a piezoresistive sensor with high sensitivity (0.28 kPa-1), wide detection range (up to 66.98 kPa), and ultralow detection limit (∼60 Pa). It is envisaged that the superelasticity of MXene/rGO aerogels offers a versatile platform for utilizing MXene-based materials in a wide array of applications including wearable electronics, electromagnetic interference shielding, and flexible energy storage devices.

Three-Dimensional MOFs@MXene Aerogel Composite Derived MXene Threaded Hollow Carbon Confined CoS Nanoparticles toward Advanced Alkali-Ion Batteries.

MXene combining high metal-like conductivity, high hydrophilicity, and abundant surface functional groups has been recognized as a class of versatile two-dimensional materials for many applications. However, the aggregation of MXene nanosheets from interlayer van der Waals force and hydrogen bonds represents a major problem that severely limits their practical use. Here, we report an aerogel structure of MOFs@MXene, in which the in situ formed MOF particles can effectively prevent the accumulation of MXene, enabling a three-dimensional (3D) hierarchical porous conductive network to be composed with an ultralight feature. Subsequently, a 3D porous MXene aerogel threaded hollow CoS nanobox composite ((CoS NP@NHC)@MXene) derived from the MOFs@MXene aerogel precursor was synthesized, and the highly interconnected MXene network and hierarchical porous structure coupled with the ultrafine nanocrystallization of the electrochemically active phase of CoS yield the hybrid system with excellent electron and ion transport properties. Benefiting from the synergistic effect of the components, the (CoS NP@NHC)@MXene composite manifests outstanding electrochemistry properties as electrode materials for all of the lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), and potassium-ion batteries (PIBs). It demonstrated the excellent cycle stability and high capacities of 1145.9 mAh g-1 at 1 A g-1 after 800 cycles and 574.1 mAh g-1 at 5 A g-1 after 1000 cycles for LIBs, 420 mAh g-1 at 2 A g-1 after 650 cycles for SIBs, and 210 mAh g-1 at 2 A g-1 after 500 cycles for PIBs. First-principle calculations confirmed that the (CoS NP@NHC)@MXene hybrid could enhance the charge transfer reaction kinetics, particularly at the interface. More importantly, the excellent rate performance under high mass loading and the high volumetric energy and power density of the entire electrode represent the potential of (CoS NP@NHC)@MXene composites for applications to practical electrochemical energy storage devices. The synthesis method reported in this Article is versatile and can be easily extended to produce other porous MXene-aerogel-based materials for various applications.

Anisotropic Electromagnetic Absorption of Aligned Ti3C2Tx MXene/Gelatin Nanocomposite Aerogels.

Assembling Ti3C2Tx MXene nanosheets into three-dimensional (3D) architecture with controllable alignment is of great importance for electromagnetic wave absorption (EMA) application. However, it is a great challenge to realize it due to the weak van der Waals interconnection between MXene nanosheets. Herein, we propose to introduce gelatin molecules as a "chemical glue" to fabricate the 3D Mxene@gelatin (M@G) nanocomposite aerogel using a unidirectional freeze casting method. The Ti3C2Tx MXene nanosheets are well aligned in the M@G nanocomposite aerogel, yielding much enhanced yet anisotropic mechanical properties. Due to the unidirectional aligned microstructure, the M@G nanocomposite aerogel shows significantly anisotropic EMA properties. M@G-45 shows a -59.5 dB minimum reflection loss (RLmin) at 14.04 GHz together with a 6.24 GHz effective absorption bandwidth in the parallel direction (relative to the direction of unidirectional freeze casting). However, in the vertical direction of the same M@G aerogel, RLmin is shifted to a much lower frequency (4.08 GHz) and the effective absorption bandwidth decreases to 0.86 GHz. The anisotropic electromagnetic energy dissipation mechanism was deeply investigated, and the impendence match plays a critical role for electromagnetic wave penetration. Our lightweight M@G nanocomposite aerogel with controllable MXene alignment is very promising in EMA application.

Vertically Aligned Janus MXene-Based Aerogels for Solar Desalination with High Efficiency and Salt Resistance.

Solar desalination is an effective way of converting solar energy to heat for seawater purification. The structure of absorbers and salt resistance are two crucial parameters for water transport and desalination stability. Here, we designed a vertically aligned Janus MXene aerogel (VA-MXA) with hydrophobic upper layer and hydrophilic bottom layer. Compared with irregular porous channels, such regulatable and well-ordered vertical array structure gives competitive advantage in the capillary water transport, light absorption, and vapor escape. MXene, which possesses a theoretical light-to-heat conversion efficiency of 100%, combined with the Janus structure, can efficiently convert light to heat and prevent the photothermal layer from "direct bulk water contact" with the hydrophobic upper layer, thus decreasing heat loss, while the hydrophilic bottom layer submerged in water can quickly pump water upward through the vertically aligned channels with low transport resistance and, meanwhile, enable effective inhibition of salt crystallization due to rapid dissolution with continuously pumping water. With a vertically aligned and Janus structure by flexible design, the Janus VA-MXA exhibited a high conversion efficiency (87%) and stable water yield for 15 days (∼1.46 kg·m-2·h-1) under 1 sun. About 6 L·m-2 of freshwater was output daily from seawater.

Highly Electrically Conductive Three-Dimensional Ti3C2T x MXene/Reduced Graphene Oxide Hybrid Aerogels with Excellent Electromagnetic Interference Shielding Performances.

Two-dimensional transition-metal carbides/carbonitrides (MXenes) with both superb electrical conductivity and hydrophilicity are promising for fabricating multifunctional nanomaterials and nanocomposites. However, the construction of three-dimensional (3D) and lightweight MXene macroscopic assemblies with excellent electrical conductivity and mechanical performances has not been realized due to the weak gelation capability of MXene sheets. Herein, we demonstrate an efficient approach for constructing highly conductive 3D Ti3C2T x porous architectures by graphene oxide assisted hydrothermal assembly followed by directional freezing and freeze-drying. The resultant hybrid aerogels exhibit aligned cellular microstructure, in which the graphene sheets serve as the inner skeleton, while the compactly attached Ti3C2T x sheets present as shells of the cell walls. The porous and highly conductive architecture (up to 1085 S m-1) is highly efficient in endowing epoxy nanocomposite with a high electrical conductivity of 695.9 S m-1 and an outstanding electromagnetic interference (EMI)-shielding effectiveness of more than 50 dB in the X-band at a low Ti3C2T x content of 0.74 vol %, which are the best results for polymer nanocomposites with similar loadings of MXene so far. The successful assembly methodology of 3D and porous architectures of Ti3C2T x would greatly widen the practical applications of MXenes in the fields of EMI shielding, supercapacitors, and sensors.