High-Performance Foam-Shaped Strain Sensor Based on Carbon Nanotubes and Ti3C2Tx MXene for the Monitoring of Human Activities.

The flexible strain sensor is of significant importance in wearable electronics, since it can help monitor the physical signals from the human body. Among various strain sensors, the foam-shaped ones have received widespread attention owing to their light weight and gas permeability. However, the working range of these sensors is still not large enough, and the sensitivity needs to be further improved. In this work, we develop a high-performance foam-shaped strain sensor composed of Ti3C2Tx MXene, multiwalled carbon nanotubes (MWCNTs), and thermoplastic polyurethane (TPU). MXene sheets are adsorbed on the surface of a composite foam of MWCNTs and TPU (referred to as TPU/MWCNTs foam), which is prefabricated by using a salt-templating method. The obtained TPU/MWCNTs@MXene foam works effectively as a lightweight, easily processable, and sensitive strain sensor. The TPU/MWCNTs@MXene device can deliver a wide working strain range of ∼100% and an outstanding sensitivity as high as 363 simultaneously, superior to the state-of-the-art foam-shaped strain sensors. Moreover, the composite foam shows an excellent gas permeability and suitable elastic modulus close to those of skin, indicating its being highly comfortable as a wearable sensor. Owing to these advantages, the sensor works effectively in detecting both subtle and large human movements, such as joint motion, finger motion, and vocal cord vibration. In addition, the sensor can be used for gesture recognition, demonstrating its perspective in human-machine interaction. Because of the high sensitivity, wide working range, gas permeability, and suitable modulus, our foam-shaped composite strain sensor may have great potential in the field of flexible and wearable electronics in the near future.

Site-Selective Transformation for Preparing Tripod-like NiCo-Sulfides@Carbon Boosts Enhanced Areal Capacity and Cycling Reliability.

Flexible power supply systems for future wearable electronics desperately require high areal capacity (Ca) and robust cycling reliability due to the limited surface area of the human body. Transition metal sulfides are preferred as cathode materials for their improved conductivity and rich redox centers, yet their practical applications are severely hindered by the sluggish charge transport kinetics and unavoidable capacity decay due to the phase transformation during charge/discharge processes. Herein, we develop a site-selective transformation strategy for preparing tripod-like NiCo-sulfides@carbon (T-NCS@C) arrays on carbon cloth. The mass loading of active materials is balanced with charge (electron and ion) transport efficiency. The optimized T-NCS@C delivers a superior Ca of 494 µA h/cm2 (corresponding to 235 mA h/g) at 3 mA/cm2. Due to the protection of the carbon layer that is derived from transformed metal-organic framework (MOF) sheath, the T-NCS@C displays excellent stability with 92% retention over 5000 charge/discharge cycles. The flexible full cell adopting Fe2O3 as the anode and T-NCS@C as the cathode exhibits an improved Ea (areal energy density) of 389 µW h/cm2 at a Pa (areal power density) of 4.22 mW/cm2 together with robust cycling reliability.

Ammonium Intercalation Induced Expanded 1T-Rich Molybdenum Diselenides for Improved Lithium Ion Storage.

Transition metal dichalcogenides (TMDs), particularly molybdenum diselenides (MoSe2), have the merits of their unique two-dimensional (2D) layered structures, large interlayer spacing (∼0.64 nm), good electrical conductivities, and high theoretical capacities when applied in lithium-ion batteries (LIBs) as anode materials. However, MoSe2 remains suffering from inferior stability as well as unsatisfactory rate capability because of the unavoidable volume expansion and sluggish charge transport during lithiation-delithiation cycles. Herein, we develop a simultaneous reduction-intercalation strategy to synthesize expanded MoSe2 (e-MoSe2) with an interlayer spacing of 0.98 nm and a rich 1T phase (53.7%) by rationally selecting the safe precursors of ethylenediamine (NH2C2H4NH2), selenium dioxide (SeO2), and sodium molybdate (Na2MoO4). It is noteworthy that NH2C2H4NH2 can effectively reduce SeO2 and MoO42- forming MoSe2 nanosheets; in the meantime, the generated ammonium (NH4+) efficiently intercalates between MoSe2 layers, leading to charge transfer, thus stabilizing 1T phases. The obtained e-MoSe2 exhibits high capacities of 778.99 and 611.40 mAh g-1 at 0.2 and 1 C, respectively, together with excellent cycling stability (retaining >90% initial capacity at 0.2 C over 100 charge-discharge cycles). It is believed that the material design strategy proposed in this paper provides a favorable reference for the synthesis of other transition metal selenides with improved electrochemical performance for battery applications.

Recent Advances in Molybdenum-Based Materials for Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries as power supply systems possessing a theoretical energy density of as high as 2600 Wh kg-1 are considered promising alternatives toward the currently used lithium-ion batteries (LIBs). However, the insulation characteristic and huge volume change of sulfur, the generation of dissolvable lithium polysulfides (LiPSs) during charge/discharge, and the uncontrollable dendrite formation of Li metal anodes render Li-S batteries serious cycling issues with rapid capacity decay. To address these challenges, extensive efforts are devoted to designing cathode/anode hosts and/or modifying separators by incorporating functional materials with the features of improved conductivity, lithiophilic, physical/chemical capture ability toward LiPSs, and/or efficient catalytic conversion of LiPSs. Among all candidates, molybdenum-based (Mo-based) materials are highly preferred for their tunable crystal structure, adjustable composition, variable valence of Mo centers, and strong interactions with soluble LiPSs. Herein, the latest advances in design and application of Mo-based materials for Li-S batteries are comprehensively reviewed, covering molybdenum oxides, molybdenum dichalcogenides, molybdenum nitrides, molybdenum carbides, molybdenum phosphides, and molybdenum metal. In the end, the existing challenges in this research field are elaborately discussed.

Mechanistic insight in site-selective and anisotropic etching of prussian blue analogues toward designable complex architectures for efficient energy storage.

Engineering coordination compounds, e.g., prussian blue (PB) and its analogues (PBAs), with designable complex nanostructures via chemical etching holds great opportunities for improving energy storage performances by adjusting topological geometry, selectively exposing active sites, tuning electronic properties and enhancing accessible surface area. Unfortunately, it remains ambiguous particularly on site-selective and anisotropic etching behaviors. Herein, for the first time, we propose that two distinct regions are formed inside NiCo PBA (NCP) cubes due to the competition between classical ion-by-ion crystallization and non-classical crystallization based on aggregation. Such a unique structure ultimately determines not only the etching position but also the anisotropic pathway by selectively exposing unprotected Ni sites. According to this principle, complex PBA architectures, including nanocages, open nanocubes (constructed by six cones sharing the same apex), nanocones, and chamfer nanocubes can be intentionally obtained. After thermal annealing, NCP nanocones are converted to morning glory-like porous architectures composed of NiO/NiCo2O4 heterostructures with a mean particle size of 5 nm, which show improved rate performance and cycling stability.

Microstructure Design of Carbonaceous Fibers: A Promising Strategy toward High-Performance Weaveable/Wearable Supercapacitors.

Fiber-based supercapacitors (FSCs) possess great potential as an ideal type of power source for future weaveable/wearable electronics and electronic-textiles. The performance of FSCs is, without doubt, primarily determined by the properties of fibrous electrodes. Carbonaceous fibers, e.g., commercial carbon fibers, newly developed graphene fibers, and carbon nanotube fibers, are deemed as promising materials for weaveable/wearable supercapacitors owing to their exotic properties including high tensile strength and robustness, excellent electrical conductivity, good flexibility, and environmental stability. Nevertheless, bare carbonaceous fiber normally exhibits low capacitance originating from electric double-layer capacitance, which remains unsatisfactory for efficiently powering wearable and portable devices. Numerous efforts have been devoted to tailoring fiber properties by hybridizing pseudocapacitive materials, and impressive progress has been achieved thus far. Herein, the microstructures of pristine carbonaceous fibers are introduced in detail, and the recent advances in rational nano/microstructure design of their hybrids, which provides the feasibility to achieve the synergistic interaction between conductive agents and pseudocapacitive nanomaterials but are normally overlooked, are comprehensively reviewed. Besides, the challenges in developing high-performance fibrous electrodes are also elaborately discussed.

Solution-Processed Sensing Textiles with Adjustable Sensitivity and Linear Detection Range Enabled by Twisting Structure.

Wearable strain sensors are emerging rapidly for their promising applications in human motion detection for diagnosis, healthcare, training instruction, and rehabilitation exercise assessment. However, it remains a bottleneck in gaining comfortable and breathable devices with the features of high sensitivity, linear response, and tunable detection range. Textiles possess fascinating advantages of good breathability, aesthetic property, tailorability, and excellent mechanical compliance to conformably attach to human body. As the meandering loops in a textile can be extended in different directions, it provides plenty of room for exploring ideal sensors by tuning a twisting structure with rationally selected yarn materials. Herein, textile sensors with twisting architecture are designed via a solution-based process by using a stable water-based conductive ink that is composed of polypyrrole/polyvinyl alcohol nanoparticles with a mean diameter of 50 nm. Depending on the predesigned twisting models, the thus-fabricated textile sensors show adjustable performances, exhibiting a high sensitivity of 38.9 with good linearity and a broad detection range of 200%. Such sensors can be integrated into fabrics and conformably attached to skin for monitoring subtle (facial expressions, breathing, and speaking) and large (stretching, jumping, running and jogging, and sign language) human motions. As a proof-of-concept application, by integrating with a wireless transmitter, the signals detected by our sensors during exercise (e.g., running) can be remotely received and displayed on a smartphone. It is believed that the integration of our textile sensors with selected twisting models into a cloth promises full-range motion detection for wearable electronics and human-machine interfaces.

Electrostatically Assembling 2D Nanosheets of MXene and MOF-Derivatives into 3D Hollow Frameworks for Enhanced Lithium Storage.

As an essential member of 2D materials, MXene (e.g., Ti3 C2 Tx ) is highly preferred for energy storage owing to a high surface-to-volume ratio, shortened ion diffusion pathway, superior electronic conductivity, and neglectable volume change, which are beneficial for electrochemical kinetics. However, the low theoretical capacitance and restacking issues of MXene severely limit its practical application in lithium-ion batteries (LIBs). Herein, a facile and controllable method is developed to engineer 2D nanosheets of negatively charged MXene and positively charged layered double hydroxides derived from ZIF-67 polyhedrons into 3D hollow frameworks via electrostatic self-assembling. After thermal annealing, transition metal oxides (TMOs)@MXene (CoO/Co2 Mo3 O8 @MXene) hollow frameworks are obtained and used as anode materials for LIBs. CoO/Co2 Mo3 O8 nanosheets prevent MXene from aggregation and contribute remarkable lithium storage capacity, while MXene nanosheets provide a 3D conductive network and mechanical robustness to facilitate rapid charge transfer at the interface, and accommodate the volume expansion of the internal CoO/Co2 Mo3 O8 . Such hollow frameworks present a high reversible capacity of 947.4 mAh g-1 at 0.1 A g-1 , an impressive rate behavior with 435.8 mAh g-1 retained at 5 A g-1 , and good stability over 1200 cycles (545 mAh g-1 at 2 A g-1 ).

Identifying the active site of ultrathin NiCo LDH as an efficient peroxidase mimic with superior substrate affinity for sensitive detection of hydrogen peroxide.

Nanozymes have been extensively investigated to imitate protein enzymes in biomimetic chemistry and the identification of the active site is believed to be the pre-requisite before one can effectively regulate their activity. Herein, ultrathin NiCo LDH nanosheets are synthesized via a fast co-precipitation at room temperature and can be stably dispersed in water without any additives of surfactants or organic solvents. By tuning the ratio between Ni and Co in LDH nanosheets, the activity is tuned and their peroxidase-like activity is determined by Co sites that show higher affinity to both 3,3',5,5'-tetramethylbenzidine (TMB) and hydrogen peroxide (H2O2) due to the strong Lewis acidity of Co3+ and the low redox potential of Co3+/Co2+. Together with their small crystallite size, ultra-thin thickness and tunable composition, NiCo LDH is used as a nanozyme for highly sensitive colorimetric detection of H2O2 and the limit of detection (LOD) reaches 0.48 µM.