Self-Healable, Self-Adhesive and Degradable MXene-Based Multifunctional Hydrogel for Flexible Epidermal Sensors.

Conductive hydrogels have garnered significant interest in the realm of wearable flexible sensors due to their close resemblance to human tissue, wearability, and precise signal acquisition capabilities. However, the concurrent attainment of an epidermal hydrogel sensor incorporating reliable self-healing capabilities, biodegradability, robust adhesiveness, and the ability to precisely capture subtle electrophysiological signals poses a daunting and intricate challenge. Herein, an innovative MXene-based composite hydrogel (PBM hydrogel) with exceptional self-healing, self-adhesive, and versatile functionality is engineered through the integration of conductive MXene nanosheets into a well-structured poly(vinyl alcohol) (PVA) and bacterial cellulose (BC) hydrogel three-dimensional (3D) network, utilizing multiple dynamic cross-linking synergistic repeated freeze-thaw strategy. The hydrogel harnesses the presence of dynamically reversible borax ester bonds and multiple hydrogen bonds between its constituents, endowing it with rapid self-healing efficiency (97.8%) and formidable self-adhesive capability. The assembled PBM hydrogel epidermal sensor possesses a rapid response time (10 ms) and exhibits versatility in detecting diverse external stimuli and human movements such as vocalization, handwriting, joint motion, Morse code signals, and even monitoring infusion status. Additionally, the PBM hydrogel sensor offers the added advantage of swift degradation in phosphate-buffered saline solution (within a span of 56 days) and H2O2 solution (in just 53 min), maintaining an eco-friendly profile devoid of any environmental pollution. This work lays the groundwork for possible uses in electronic skins, interactions between humans and machines, and the monitoring of individualized healthcare.

Topological Engineering Electrodes with Ultrafast Oxygen Transport for Super-Power Sodium-Oxygen Batteries.

Sodium-oxygen battery has attracted tremendous interest due to its extraordinary theoretical specific energy (1605 Wh kg-1 NaO2) and appealing element abundance. However, definite mechanistic factors governing efficient oxygen diffusion and consumption inside electrolyte-flooded air cathodes remain elusive thus precluding a true gas diffusion electrode capable of high discharge current (i.e., several mA cm-2) and superior output power. Herein, 3D-printing technology is adopted to create gas channels with tailored channel size and structure to demystify the diffusion-limited oxygen delivery process. It is revealed that as the clogging discharging products increase, large channel size, and interconnected channel structure are essential to guaranteeing fast O2 diffusion. Moreover, to further encourage O2 diffusion, a bio-inspired breathable cathode with progressively branching channels that balances between O2 passage and reaction is 3D printed. This elaborated 3D electrode allows a sodium-oxygen cell to deliver an impressive discharging current density of up to 4 mA cm-2 and an output power of 8.4 mW cm-2, giving rise to an outstanding capacity of 18.4 mAh cm-2. The unraveled mystery of oxygen delivery enabled by 3D printing points to a valuable roadmap for the rational design of metal-air batteries toward practical applications.

Densifiable Ink Extrusion for Roll-To-Roll Fiber Lithium-Ion Batteries with Ultra-High Linear and Volumetric Energy Densities.

Conventional bulky and rigid planar architecting power systems are difficult to satisfy the growing demand for wearable applications. 1D fiber batteries bearing appealing features of miniaturization, adaptability, and weavability represent a promising solution, yet challenges remain pertaining to energy density and scalability. Herein, an ingenious densifiable functional ink is invented to fabricate scalable, flexible, and high-mass-loading fiber lithium-ion batteries (LIBs) by adopting a fast ink-extrusion technology. In the formulated ink, pyrrole-modified reduced graphene oxide is elaborately introduced and exerts multiple influences; it not only assembles carbon nanotubes and poly(vinylidene fluoride-co-hexafluoropropylene) to compose a sturdy, conductive, and agglomeration-free 3D network that realizes an ultra-high content (75 wt%) of the active materials and endows the electrode excellent flexibility but also serves as a capillary densification inducer, encouraging an extremely large linear mass loading (1.01 mg cm-1 per fiber) and packing density (782.1 mg cm-3 ). As a result, the assembled fiber LIBs deliver impressive linear and volumetric energy densities with superb mechanical compliance, demonstrating the best performance among all the reported extruded fiber batteries. This work highlights a highly effective and facile approach to fabricate high-performance fiber energy storage devices for future practical wearable applications.

Surface-Adaptive Capillarity Enabling Densified 3D Printing for Ultra-High Areal and Volumetric Energy Density Supercapacitors.

Endowing supercapacitors with higher energy density is of great practical significance but remains extremely challenging. In this work, an innovative densified 3D printing enabled by a surface-adaptive capillarity strategy is proposed for the first time. The printable ink formulated with pyrrole surface-modified reduced graphene oxide renders the printed electrodes excellent surface tension regulability to the subsequent capillary densification, creating an intensely condensed electrode with well-maintained structural integrity. Furthermore, simultaneous in situ nitrogen doping and hierarchical micro-meso porosity are readily realized upon post-carbonization, encouraging enhanced capacitance and fast reaction dynamics. As a result, the printed symmetric supercapacitor delivers a double leap in areal and volumetric energy densities in both aqueous and organic electrolytes, a rarely achieved yet gravely desired attribute for 3D printed energy storage devices.

Supercritical CO2 Assisted Solvothermal Preparation of CoO/Graphene Nanocomposites for High Performance Lithium-Ion Batteries.

Supercritical CO2 (scCO2) is often used to prepare graphene/metal oxide nanocomposite anodes for high performance lithium-ion batteries (LIBs) by the assisted solvothermal method due to its low viscosity, high diffusion, zero surface tension and good surface wettability. However, the formation mechanism of metal oxides and the combination mechanism between metal oxides and graphene in this system are superficial. In this work, a cobalt monoxide/graphene (CoO/G) nanocomposite is fabricated via the scCO2 assisted solvothermal method followed by thermal treatment. We elucidate the mechanism that amorphous intermediates obtain by the scCO2 assisted solvothermal method, and then ultrafine CoO nanoparticles are crystallized during the heat treatment. In addition, scCO2 can promote CoO to be tightly fixed on the surface of graphene nanosheets by interfacial chemical bonds, which can effectively improve its cycle stability and rate performance. As expected, the CoO/G composites exhibit higher specific capacity (961 mAh g-1 at 100 mA g-1), excellent cyclic stability and rate capability (617 mAh g-1 after 500 cycles at 1000 mA g-1) when applied as an anode of LIB.

Tunable Hollow Nanoreactors for In Situ Synthesis of GeP Electrodes towards High-Performance Sodium Ion Batteries.

The practical application of germanium phosphide (GeP) in battery systems is seriously impeded referring to the sluggish reaction kinetics and severe volume change. Nanostructure design that elaborately resolves the above issues is highly desired but still remains a big challenge. Herein, unique hollow nanoreactors assembled with nitrogen-doped carbon networks for in situ synthesis of the GeP electrodes are proposed for the first time. Such nanoreactors form a self-supported conductive network, ensuring sufficient electrolyte infiltration and fast electron transport. They restrain crystal growth and accommodate the volume expansion of GeP simultaneously. Reaction kinetics and confinement effect are optimized through nanoreactor size regulation. The optimized GeP electrode has high reversible capacities and outstanding cyclability and rate performance for sodium storage, outperforming most previously reported phosphides.

Rational Design of Porous Covalent Triazine-Based Framework Composites as Advanced Organic Lithium-Ion Battery Cathodes.

In an effort to explore the use of organic high-performance lithium ion battery cathodes as an alternative to resolve the current bottleneck hampering the development of their inorganic counterparts, a rational strategy focusing on the optimal composition of covalent triazine-based frameworks (CTFs) with carbon-based materials of varied dimensionalities is delineated. Two-dimensional reduced graphene oxide (rGO) with a compatible structural conformation with the layered CTF is the most suitable scaffold for the tailored mesopores in the polymeric framework, providing outstanding energy storage ability. Through facile ionothermal synthesis and structure engineering, the obtained CTF-rGO composite possesses a high specific surface area of 1357.27 m²/g, and when used as a lithium ion battery cathode it delivers a large capacity of 235 mAh/g in 80 cycles at 0.1 A/g along with a stable capacity of 127 mAh/g over 2500 cycles at 5 A/g. The composite with modified pore structure shows drastically improved performance compared to a pristine CTF, especially at large discharge currents. The CTF-rGO composite with excellent capacity, stability, and rate performance shows great promise as an emerging high-performance cathode that could revolutionize the conventional lithium-ion battery industry.

Facile Synthesis of Nanosized Lithium-Ion-Conducting Solid Electrolyte Li1.4Al0.4Ti1.6(PO4)3 and Its Mechanical Nanocomposites with LiMn2O4 for Enhanced Cyclic Performance in Lithium Ion Batteries.

Nanoparticles of fast lithium-ion-conducting solid electrolyte Li1.4Al0.4Ti1.6(PO4)3 (LATP) are prepared by a modified citric-acid-assisted sol-gel method that involves a two-step heat treatment in which the dry gel is calcined first in argon and then in air. The obtained LATP exhibits smaller particle size (down to 40 nm) with a narrower size distribution and less aggregation than LATP prepared by a conventional sol-gel method because of a polymeric network that preserves during LATP crystallization. It has a high relative density of 97.0% and a high room-temperature conductivity of 5.9 × 10-4 S cm-1. The as-prepared superfine LATP is further used to composite with a spinel LiMn2O4 cathode in lithium ion batteries by simple grinding. This noncoating speckled layer over the LiMn2O4 particle surface has a minimal effect on the electronic conductivity of the electrode while offering excellent ionic conductivity. The cycling stability and rate capability of LiMn2O4 are greatly improved at both ambient and elevated temperatures. After 100 cycles at 25 and 55 °C, the capacity retentions are 96.0% and 89.0%, respectively, considerably higher than the values of pristine LiMn2O4 (61.0% at 25 °C; 51.5% at 55 °C) and mechanical LiMn2O4 composite with LATP made by a conventional sol-gel method (85.0% at 25 °C; 71.4% at 55 °C).