The rapidly growing demand for wearable and portable electronics has driven the recent revival of flexible Zn‐ion batteries (ZIBs). However, issues of dendrite growth and low the flexibility of Zn metal anode still impede their practical application. Herein, 3D nitrogen‐doped vertical graphene nanosheets in situ grown on carbon cloth (N‐VG@CC) are proposed to enable uniform Zn nucleation, thereby obtaining a dendrite‐free and robust Zn anode. The introduced zincopilic N‐containing groups in N‐VG effectively reduce the Zn nucleation overpotential by enhancing the interaction between Zn2+ ion and carbon substrate, as confirmed by density functional theory calculations, thus achieving uniform distribution of Zn nucleus. Moreover, the 3D nanosheet arrays can homogenize electric distribution, which optimizes the subsequence Zn deposition process and realizes the highly reversible Zn plating/stripping process. Consequently, the as‐prepared Zn@N‐VG@CC anode exhibits an improved overall electrochemical performance compared with Zn@CC. As a proof‐of‐concept application, the high‐performance Zn@N‐VG@CC electrodes are successfully employed as anodes for coin and flexible quasi‐solid‐state ZIBs together with MnO2@N‐VG@CC (deposited MnO2 nanosheets on N‐VG@CC) as cathodes. More importantly, the flexible ZIB exhibits impressive cycling stability with 80% capacity retention after 300 cycles and outstanding mechanical flexibility, indicating a promising potential for portable and wearable electronics.
Extensive efforts have been devoted to construct a fiber-shaped energystorage device to fulfill the increasing demand for power consumption of textile-based wearable electronics. Despite the myriad of available material selections and device architectures, it is still fundamentally challenging to develop eco-friendly fiber-shaped aqueous rechargeable batteries (FARBs) on a single-fiber architecture with high energy density and long-term stability. Here, we demonstrate flexible and high-voltage coaxialfiber aqueous rechargeable zinc-ion batteries (CARZIBs). By utilizing a novel spherical zinc hexacyanoferrate with prominent electrochemical performance as cathode material, the assembled CARZIB offers a large capacity of 100.2 mAh cm −3 and a high energy density of 195.39 mWh cm −3 , outperforming the state-of-the-art FARBs. Moreover, the resulting CARZIB delivers outstanding flexibility with the capacity retention of 93.2% after bending 3000 times. Last, high operating voltage and output current are achieved by the serial and parallel connection of CARZIBs woven into the flexible textile to power high-energy-consuming devices. Thus, this work provides proof-of-concept design for next-generation wearable energy-storage devices.
The Al effect on the electrochemical properties of layered double hydroxides (LDHs) is not properly probed, although it is demonstrated to notably promote the capacitive behavior of LDHs. Herein, ternary NiCo 2 Al x layered double hydroxides with varying levels of Al stoichiometry are purposely developed, grown directly on mechanically flexible and electrically conducting carbon cloth (CC@NiCo 2 Al x -LDH). Al plays a significant role in determining the structure, morphology, and electrochemical behavior of NiCo 2 Al x -LDHs. At an increasing level of Al in NiCo 2 Al x -LDHs, there is a steady evolution from 1D nanowire to 2D nanosheets. The CC@NiCo 2 Al-LDH at an appropriate level of Al and with the nanowire-nanosheet mixed morphology exhibits both significantly enhanced electrochemical performance and excellent structural stability, with about a 2.3-fold capacitance of NiCo 2 -OH. When applied as the anode in a flexible asymmetric supercapacitor (ASC), the CC@NiCo 2 Al-LDH gives rise to a remarkable energy density of 44 Wh kg −1 at the power density of 462 W kg −1 , together with remarkable cyclic stability with 91.2% capacitance retention over 15 000 charge-discharge cycles. The present study demonstrates a new pathway to significantly improve the electrochemical performance and stability of transition metal LDHs, which are otherwise unstable in structure and poorly performing in both rate and cycling capability.
The emergence of fiber-shaped supercapacitors (FSSs) has led to a revolution in portable and wearable electronic devices. However, obtaining high energy density FSSs for practical applications is still a key challenge. This article exhibits a facile and effective approach to directly grow well-aligned three-dimensional vanadium nitride (VN) nanowire arrays (NWAs) on carbon nanotube (CNT) fiber with an ultrahigh specific capacitance of 715 mF/cm in a three-electrode system. Benefiting from their intriguing structural features, we successfully fabricated a prototype asymmetric coaxial FSS (ACFSS) with a maximum operating voltage of 1.8 V. From core to shell, this ACFSS consists of a CNT fiber core coated with VN@C NWAs as the negative electrode, NaSO poly(vinyl alcohol) (PVA) as the solid electrolyte, and MnO/conducting polymer/CNT sheets as the positive electrode. The novel coaxial architecture not only fully enables utilization of the effective surface area and decreases the contact resistance between the two electrodes but also, more importantly, provides a short pathway for the ultrafast transport of axial electrons and ions. The electrochemical results show that the optimized ACFSS exhibits a remarkable specific capacitance of 213.5 mF/cm and an exceptional energy density of 96.07 μWh/cm, the highest areal capacitance and areal energy density yet reported in FSSs. Furthermore, the device possesses excellent flexibility in that its capacitance retention reaches 96.8% after bending 5000 times, which further allows it to be woven into flexible electronic clothes with conventional weaving techniques. Therefore, the asymmetric coaxial architectural design allows new opportunities to fabricate high-performance flexible FSSs for future portable and wearable electronic devices.
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