ABSTRACT
Zinc ion hybrid capacitors (ZIHCs) are encouraging energy storage devices for large-scale applications. Nevertheless, the electrochemical performance of ZIHCs is often limited by the cathode materials which show low energy density and rate capability practically. One of the efficient strategies to overcome these challenges is the development of advanced carbon cathode materials with abundant physi/chemisorption sites. Herein, we develop a sulfate template strategy to prepare sulfur and oxygen doped carbon nanosheets (SOCNs) as a potential cathode active material for ZIHCs. The as-prepared SOCNs exhibit porous architectures with a large surface area of 1877 m2 g-1, substantial structural defects, and high heteroatom-doped contents (O: 7.9 at%, S: 0.7 at%). These exceptional features are vital to enhancing Zn ion storage. Consequently, the SOCN cathode shows a high capacity of 151 mAh g-1 at 0.1 A g-1, high cycle stability with 83% capacity retention at 5 A g-1 after 4000 cycles, and a superior energy density of 103.1 Wh kg-1. We also investigate the dynamic adsorption/desorption behaviors of Zn ions and anions of the ZIHCs carbon electrodes during the process of charge and discharge by ex-situ experiments. This work highlights the significance of the integration with a large specific surface area and bountiful heteroatoms in carbon electrodes for achieving high-performance ZIHCs.
ABSTRACT
Porous carbon is the most promising cathode material for Zn-ion hybrid capacitors (ZIHCs), but is limited by insufficient active adsorption sites and slow ion diffusion kinetics during charge storage. Herein, a pore construction-pore expansion strategy for synthesizing multi-channel hollow carbon nanofibers (MCHCNF) is proposed, in which the sacrificial template-induced multi-channel structure eliminates the diffusion barrier for enhancing ion diffusion kinetics, and the generated ultrahigh surface area and high-density defective structures effectively increase the quantity of active sites for charge storage. Additionally, a graphene-like shell structure formed on the carbon nanofiber surface facilitates fast electron transport, and the highly matchable pore size of MCHCNF with electrolyte-ions favors the accommodation of charge carriers. These advantages lead to the optimized ZIHCs exhibit high capacity (191.4 mAh g-1 ), high energy (133.1 Wh kg-1 ), along with outstanding cycling stability (93.0% capacity retention over 15000 cycles). Systematic ex situ characterizations reveal that the dual-adsorption of anions and cations synergistically ensures the outstanding electrochemical performance, highlighting the importance of the highly-developed porous structure of MCHCNF. This work not only provides a promising strategy for improving the capacitive capability of porous materials but also sheds light on charge storage mechanisms and rational design for advanced energy storage devices.
ABSTRACT
Constructing carbon electrodes with abundant heteroatoms and appropriate graphitic interlayer spacing remains a major challenge for achieving high gravimetric and volumetric potassium storage capacities with fast kinetics. Herein, we constructed 3D graphene-like N, F dual-doped carbon sheets induced by Ni template (N, F-CNS-Ni) with dense structure and rich active sites, providing a promising approach to address the facing obstacles. Highly reversible K-ion insertion/extraction is realized in the graphitic carbon structure, and K-adsorption capability is enhanced by introducing N/F heteroatoms. As a result, the N, F-CNS-Ni electrode exhibits ultrahigh gravimetric and volumetric capacities of 404.5 mA h g-1 and 281.3 mA h cm-3 at 0.05 A/g, respectively, and a superb capacity of 259.3 mA h g-1 with a capacity retention ratio of 90 % even after 600 cycles at 5 A/g. This work presents a simple Ni-based template method to prepare graphene-like carbon nanosheets with high packing density and rich heteroatoms, and offers mechanism insight for achieving superior K-ion storage.
