Composite of CoS1.97 nanoparticles decorated CuS hollow cubes with rGO as thin film electrode for high-performance all solid flexible supercapacitors.

Stretchable flexible thin-film electrodes are extensively explored for developing new wearable energy storage devices. However, traditional carbon-based materials used in such independent electrodes have limited practical applications owing to their low energy storage capacity and energy density. To address this, a unique structure and remarkable mechanical stability thin-film flexible positive electrode comprising CoS1.97 nanoparticles decorated hollow CuS cubes and reduced graphene oxide (rGO), hereinafter referred to as CCSrGO, is prepared. Transition metal sulfide CoS1.97 and CuS shows high energy density owing to the synergistic effects of its active components. The electrode can simultaneously meet the high-energy density and safety requirements of new wearable energy storage devices. The electrode has excellent electrochemical performance (1380 F/g at 1 A/g) and ideal capacitance retention (93.8 % after 10,000 cycles) owing to its unique three-dimensional hollow structure and polymetallic synergies between copper and cobalt elements, which are attributed to their different energy storage mechanisms. Furthermore, a flexible asymmetric supercapacitor (FASC) was constructed using CCSrGO as the positive electrode and rGO as the negative electrode (CCSrGO//rGO), which delivers an energy density of 100 Wh kg-1 and a corresponding power density of 2663 W kg-1 within a voltage window of 0-1.5 V. The resulting FASC can power a light-emitting diode (LED) at different bending and twisting angles, exerting little effect on the capacitance. Therefore, the prepared CCSrGO//rGO FASC devices show great application prospects in energy storage.

Strong Ti3 C2 Tx MXene-Based Composite Films Fabricated through Bioinspired Bridging for Flexible Energy Storage Devices.

Flexible energy storage device is one of the most critical components as power source for wearable electronics. The emergence of MXenes, a growing family of 2D nanomaterials, has demonstrated a brand-new possibility for flexible energy storage. However, the fabrication of MXene films with satisfactory mechanical, electrical, and electrochemical reliabilities remains challenging due to the weak interlayer interactions and self-restacking of MXene sheets. Sequential bridging of polydopamine/polyethyleneimine-functionalized (PDA/PEI)-coated MXene sheets to induce synergistically covalent and hydrogen binding connections of MXene-based films is demonstrated here. By interrupting self-hydrogen bonding and π-π stacking interactions, the introduction of long-chain PEI can not only inhibit the massive aggregation of PDA, but also improve the continuity of the interconnection network of PDA/PEI between MXene layers. Hence, the as-prepared MXene/PDA/PEI composite film displays high mechanical strength (≈366 MPa) which achieves 12-fold improvement compared with pure MXene film, as well as superior energy storage capability (≈454 F g-1  at 5 mV s-1 ) and rate performance of ≈48% at 10 000 mV s-1 . This modulation of inserted polymer between MXene layers can provide an avenue for assembling high performance MXene films, and can even be extended to the fabrication of other 2D platelets for varied applications.

Compression-tolerant supercapacitor based on NiCo2O4/Ti3C2Tx MXene/reduced graphene oxide composite aerogel with insights from density functional theory simulations.

Compression-tolerant electrodes are critical for developing next-generation wearable energy storage devices. However, most of previous studies on compressible electrodes focus on carbon-based materials, whereas metal-based materials such as spinel metal oxide with faradaic nature have been rarely studied due to their lack of compressibility. Herein, NiCo2O4 (NCO) microtubes assembled by ultrathin and mesoporous nanosheets, are deposited on/into Ti3C2Tx MXene/reduced graphene oxide aerogel (MGA), an intrinsically compressible host template with high conductivity and specific surface areas. The optimized NCO/MGA-300 sample shows a reversible compressive strain of 60% and a superior durability. Density functional theory (DFT) calculations reveal that the NCO/MGA-300 heterojunction has high electronic conductivity, fast electron transfer ability, and low adsorption energy for OH- ions. As a result, the NCO/MGA-300 electrode exhibits superb electrochemical performance in terms of its high gravimetric capacitance (1633F g-1 at 1 A g-1), rate performance (1492F g-1 at 10 A g-1), and remarkable cycling stability of 86.6% after 10,000 charge-discharging cycles. Moreover, an assembled asymmetric supercapacitor based on compressible NCO/MGA-300 shows stable electrochemical performances under different compressive strains (20%. 40% and 60%), or after 100 compression-release cycles. This research finding demonstrates the possibility of metal-based electrode for wearable devices with high energy storage capability and good compressibility.

CuxO nanorod arrays shelled with CoNi layered double hydroxide nanosheets for enhanced oxygen evolution reaction under alkaline conditions.

Exploration of highly efficient and cost-effective oxygen evolution reaction (OER) electrocatalysts is of crucial importance for the development of water splitting. In recent years, Cu-based materials have been widely concerned in OER due to their non-toxicity, rich reserves and highest reversibility. Meanwhile, CuxO nanorods is easy to be prepared in industry. Herein, we report a fast preparation method to construct an integrated CuxO@CoNi-LDH electrocatalyst with a unique 1D nanowire-2D nanosheet hierarchical core-shell structure by electrodepositing CoNi-LDH nanosheet arrays directly onto CuxO nanorods (CuxO were in situ-created on the Cu foam) at a large deposition voltage of -3.0 V vs SCE. The unique heterogeneous core-shell nanostructure, large deposition amount of CoNi-LDH and the synergistic effects between CuxO core and CoNi-LDH shell can provide abundant active sites, rich open-channels and reduced charge transfer resistance (Rct) for effective oxygen release and facile electron transport. Consequently, the optimized CuxO@CoNi-LDH/CF exhibits a low overpotential of 207 mV in 1 M KOH solution at the current density of 10 mV cm-2 and a small Tafel slope of 50.1 mV dec-1. After 60 h of long-term stability test, the catalytic performance is only slightly weakened. This work demonstrates a new approach to design the high-performance LDH and Cu-related OER catalysts by constructing a unique hierarchical core-shell nanostructure.

In Situ Synthesis of CoCeSx Bimetallic Sulfide Nanoparticles on a Bi-Pyrene Terminated Molecular Wire Modified Graphene Surface for Supercapacitors.

The excellent electrical conductivity of graphene is due to its highly-conjugated structures. Manipulation of the electronic and mechanical properties of graphene can be achieved by controlling the destruction of its in-sheet conjugation system. Herein, we report the preparation of CoCeSx -SA@BPMW@RGO through π-π stacking interactions at the molecular level. In this study, sodium alginate was reacted with Co2+ and Ce3+ , and the composite was loaded onto a graphene surface. The graphene sheets were prepared using a bi-pyrene terminated molecular wire (BPMW) to avoid re-stacking of the grapheme sheets, thereby forming nanoscale spaces between sheets. The angle between the BPMW coplanar pyrene group and the phenyl group was 33.2°, and the graphene layer is supported in an oblique direction. Finally, a three-dimensional porous composite was obtained after annealing and vulcanization. The obtained CoCeSx -SA@BPMW@RGO exhibited excellent electrical conductivity and remarkable cycle stability. When the current density was 1 A g-1 , its specific capacitance was as high as 1004 F g-1 . BPMW modifies graphene through the synergistic effect of π-π stacking interaction and special structure to obtain excellent electrochemical performance. Moreover, a solid-state asymmetric supercapacitor device was fabricated based on the synthesized CoCeSx -SA@BPMW@RGO hybrid, which exhibited a power density of 979 W kg-1 at an energy density of 23.96 Wh kg-1 .