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The development of hydrogel electrolytes plays a critical role in high-performance flexible supercapacitor devices. Herein, a composite hydrogel electrolyte of polyacrylic acid (PAA) and graphene oxide (GO) has been successfully prepared, where the oxygen-containing functional groups of GO may crosslink and form hydrogen bonds with carboxyl on the molecular chain of PAA, thereby significantly enhancing the mechanical properties of a PAA-based gel electrolyte. The tensile strength increases from 4.0 MPa for pristine PAA gel to 6.1 MPa for PAA/GO composite gel, with the elongation at break rising from 1556% to 1950%. Meanwhile, GO promotes the transportation of electrolyte ions, which are favorable for enhancing the ionic conductivity of the PAA hydrogel. As a result, the assembled supercapacitor based on PAA/GO composite hydrogel electrolyte shows enhanced capacitance retention of 64.3% at a large current density of 20 A g−1 and excellent cycling stability over 10,000 cycles at 5 A g−1. Furthermore, the fabricated flexible supercapacitor devices could maintain outstanding electrochemical performance at various bending angles of 0–90°, indicating a promising prospect for the PAA/GO hydrogel electrolyte in flexible wearable fields. [ABSTRACT FROM AUTHOR]

2D MXenes have emerged as promising supercapacitor electrode materials due to their metallic conductivity, pseudo‐capacitive mechanism, and high density. However, layer‐restacking is a bottleneck that restrains their ionic kinetics and active site exposure. Herein, a carbon dots‐intercalated strategy is proposed to fabricate flexible MXene film electrodes with both large ion‐accessible active surfaces and high density through gelation of calcium alginate (CA) within the MXene nanosheets followed by carbonization. The formation of CA hydrogel within the MXene nanosheets accompanied by evaporative drying endow the MXene/CA film with high density. In the carbonization process, the CA‐derived carbon dots can intercalate into the MXene nanosheets, increasing the interlayer spacing and promoting the electrolytic diffusion inside the MXene film. Consequently, the carbon dots‐intercalated MXene films exhibit high volumetric capacitance (1244.6 F cm−3 at 1 A g−1), superior rate capability (662.5 F cm−3 at 1000 A g−1), and excellent cycling stability (93.5% capacitance retention after 30 000 cycles) in 3 m H2SO4. Additionally, an all‐solid‐state symmetric supercapacitor based on the carbon dots‐intercalated MXene film achieves a high volumetric energy density of 27.2 Wh L−1. This study provides a simple yet efficient strategy to construct high‐volumetric performance MXene film electrodes for advanced supercapacitors. [ABSTRACT FROM AUTHOR]

Summary: Energy storage devices (ESD) are getting significant attention regarding their ability to reduce fossil fuel usage. Batteries and electrochemical supercapacitors are two well‐known ESDs with supercapacitors preferred for their high energy discharge potential. The metal oxides (MOs) with robust redox characteristics are ideal candidates for supercapacitors, although their capacitance still lacks behind the theoretical values. Here, partial reduced or oxygen‐deficient MOs have been identified have proven promising to reach the desired capacitance. The introduction of oxygen vacancies into MOs can effectively enhance their electrochemical properties without altering the inherent characteristics of MOs. This review discusses the recent progress on new oxygen‐deficient MOs and their performance as a supercapacitor. The importance of oxygen vacancy is described, followed by the traditional synthesis route to producing MOs. The present pathways for generating oxygen vacancies and their analytical assessment are covered in‐depth, followed by a section on the most advanced analytical techniques for detecting and interpreting the creation of such vacancies. The influence of oxygen vacancies on the supercapacitive performance of the most researched MOs is provided with the challenges and prospects of oxygen‐deficient MOs in supercapacitor application. [ABSTRACT FROM AUTHOR]

MXenes have emerged as promising electrode materials for supercapacitors based on their metallic conductivity, good hydrophilicity, rich surface chemistry, and excellent mechanical characteristics. However, the strong interlayer van der Waals forces induce significant layer restacking, which restrict complete exposure of MXenes' surface active sites, impeding electron/ion transport and resulting in poor electrochemical performances. Herein, a porous MXene/carbon nanotube (CNT) film was prepared through a simple alkali-induced process. The developed porosity and the introduction of CNTs can effectively suppress the restacking of MXene nanosheets, promoting the effective utilization of the surface active sites of the MXene and facilitating fast ion/electron transportation. Consequently, the porous MXene/CNT film exhibited a high specific capacitance of 401.4 F g-1 at 1 A g-1 and a sustained capacitance of 336.2 F g-1 at an ultrahigh current density of 1000 A g-1, corresponding to an 83.8% capacitance retention. Furthermore, the film electrode demonstrated outstanding cycling stability, with a capacitance retention of 99.0% after 20,000 cycles at 100 A g-1, showing its significant potential for supercapacitor applications. [ABSTRACT FROM AUTHOR]