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A new method to prepare graphene-based fibers with ultrahigh tensile strength, conductivity, and increased elongation is reported. It includes wet-spinning the mixture of GO aqueous dispersion with phenolic resin solution in a newly developed coagulation bath, followed by annealing. The introduced phenolic carbon increased densification of graphene fibers through reducing defects and increased interfacial interaction among graphene sheets by forming new C-C bonds, thus resulting in the increasing of stiffness, toughness, and conductivity simultaneously.

The energy and power performance of lithium (Li)-ion batteries is significantly reduced at low-temperature conditions, which is mainly due to the slow diffusion of Li-ions in graphite anode. Here, it is demonstrated that the effective utilization of the surface-controlled charge storage mechanism through the transition from layered graphite to 3D crumpled graphene (CG) dramatically improves the Li-ion charge storage kinetics and structural stability at low-temperature conditions. The structure-controlled CG anode prepared via a one-step aerosol drying process shows a remarkable rate-capability by delivering ≈206 mAh g-1 at a high current density of 10 A g-1 at room temperature. At an extremely low temperature of −40 °C, CG anode still exhibits a high capacity of ≈154 mAh g-1 at 0.01 A g-1 with excellent rate-capability and cycling stability. A combination of electrochemical studies and density functional theory (DFT) reveals that the superior performance of CG anode stems from the dominant surface-controlled charge storage mechanism at various defect sites. This study establishes the effective utilization of the surface-controlled charge storage mechanism through structure-controlled graphene as a promising strategy to improve the charge storage kinetics and stability under low-temperature conditions.

Soft energy storage devices, such as supercapacitors, are an essential component for powering integrated soft microsystems. However, conventional supercapacitors are mainly manufactured using hard/brittle materials that easily crack and eventually delaminate from the current collector by mechanical deformation. Therefore, to realize all-soft supercapacitors, the electrodes should be soft, stretchable, and highly conductive without compromising the electrochemical performance. This paper presents all-soft supercapacitors for integrated soft microsystems based on gallium–indium liquid metal (eutectic gallium–indium alloy, EGaIn) electrodes with integrated functionalized carbon nanotubes (CNTs). Oxygen functional groups on the surface of the CNTs ensure strong adhesion between the functionalized CNTs and the thin native oxide layer on the surface of EGaIn, which enables delamination-free soft and stretchable electrodes even under mechanical deformation. The electrochemical performances of fabricated all-soft supercapacitors in a parallel-plate arrangement were investigated without and with applied mechanical deformation. The fabricated supercapacitors exhibit areal capacitances as high as 12.4 mF cm–2 and show nearly unchanged performance under 30% applied strain. They maintain >95% of their original capacitance after >4200 charging and discharging cycles with a periodic applied strain of 30%. Finally, fabricated supercapacitors have been successfully integrated with a commercial light-emitting diode to demonstrate an integrated soft microsystem.