Hierarchical Spatial Confinement Unlocking the Storage Limit of MoS2 for Flexible High-Energy Supercapacitors.

Molybdenum sulfide (MoS2) is a promising electrode material for supercapacitors; however, its limited Mo/S edge sites and intrinsic inert basal plane give rise to sluggish active electronic states, thus constraining its electrochemical performance. Here we propose a hierarchical confinement strategy to develop ethylene molecule (EG)-intercalated Co-doped sulfur-deficient MoS2 (Co-EG/SV-MoS2) for efficient and durable K-ion storage. Theoretical analyses suggest that the intercalation-confined EG and lattice-confined Co can enhance the interfacial K-ion storage capacity while reducing the K-ion diffusion barrier. Experimentally, the intercalated EG molecules with mildly reducing properties induced the creation of sulfur vacancies, expanded the interlayer spacing, regulated the 2H-1T phase transition, and strengthened the structural grafting between layers, thereby facilitating ion diffusion and ensuring structural durability. Moreover, the Co dopants occupying the initial Mo sites initiated charge transfer, thus activating the basal plane. Consequently, the optimized Co-EG/SV-MoS2 electrode exhibited a substantially improved electrochemical performance. Flexible supercapacitors assembled with Co-EG/SV-MoS2 delivered a notable areal energy density of 0.51 mW h cm-2 at 0.84 mW cm-2 with good flexibility. Furthermore, supercapacitor devices were integrated with a strain sensor to create a self-powered system capable of real-time detection of human joint motion.

In Situ Construction of the Fe-Cu Hydroxide Interlocking Structure with Solution-Derived Cu/Ag Current Collectors for Flexible Symmetric Supercapacitors.

The current collector serves as a crucial element in supercapacitors, acting as a medium between the electrode material and the substrate. Due to its excellent conductivity, a metal collector is typically favored. Enhancing the binding strength between the collector and the substrate as well as between the collector and the electrode material has emerged as a critical factor for enhancing the capacitance performance. In this study, a Ag film with a grass root-like structure was initially grown on a PI substrate through the surface modification and ion exchange (SMIE) process. This Ag interlocking structure contributes to strong binding between the PI substrate and Ag without compromising the mechanical properties of the Ag film. To further enhance the electrochemical properties at low scan rates, electroless-plated Cu was subsequently deposited on the Ag film to form the Cu/Ag current collector. Moreover, the Cu within the Cu/Ag current collector served as a precursor for the growth of FeOOH-Cu(OH)2 via a two-step in situ method. The resulting FeOOH-Cu(OH)2/Cu/Ag structure as a whole is binder-free. Supercapacitors employing symmetric FeOOH-Cu(OH)2/Cu/Ag structures were assembled, and their energy storage properties were investigated. The solution-based low-temperature process used in this study offers the potential for cost-effective and large-scale applications.