Synergistic Effect of Nitrogen–Sulfur Codoping on Honeycomb-like Carbon-Based High-Energy-Density Zinc-Ion Hybrid Supercapacitors

Abstract

Zn-ion hybrid supercapacitors (ZHSCs) are emerging charge storage devices that inherit many of the advantages of supercapacitors and batteries. However, problems such as unsatisfactory cycling stability and low energy density need to be solved urgently, which can be accomplished by developing cathode materials with excellent properties. Herein, we report the development of performance-enhanced ZHSCs obtained by incorporating N and S heteroatoms into orange peel-based hierarchical porous carbon (NS-OPC) to facilitate Zn 2+ adsorption. The results of ex situ photoelectron spectroscopy and X-ray diffraction demonstrated the presence of −OH and Zn 2+ chemisorbed and Zn 4 SO 4 (OH) 6 •5H 2 O during charging and discharging, respectively. Density functional theory calculations show that double doping can promote the chemisorption/desorption kinetics of Zn 2+ and thus promote the electrochemical charge storage of C materials. Impressively, when used to assemble ZHSCs, the device still has an energy density of 53.9 Wh kg −1 , a high power density of 6063.75 W kg −1 , and an 86.2% capacity retention after 10,000 cycles. This study not only provides a reasonable technique for developing superior C-based electrode materials but also contributes to the understanding of the charge storage process in heteroatom-doped C materials.

Coal-Based 2D Ultrathin N-Doped Hierarchical Porous Carbon Nanosheets Induced by Dual-Salt System of Na2CO3–K2CO3 for High-Performance Supercapacitors

“…We studied the charge storage dynamics of NCPNs-3 to reveal its energy storage mechanism, mainly distinguishing between diffusion- and capacitance-controlled processes. Typically, there is a formula between the peak current ( i ) and the scanning rate ( v ) as follows: log i = log a + b log v , where a and b are adjustable parameters and the b -value can be determined by fitting a line . Generally, If the b -value is 0.5, the diffusion process fully controls the electrochemical process, while if the b -value is 1, the capacitance fully controls it .…”

Ammonium persulfate assisted synthesis of ant-nest-like hierarchical porous carbons derived from chitosan for high-performance supercapacitors and zinc-ion hybrid capacitors

“…Among them, the sample with an added hydrothermal agent shows superior electrochemical performance, exhibiting the remarkable electrochemical reversibility of the synthesized antnest-like hierarchical 3D interconnected porous carbons. 39,54 As shown in Fig. 9d, the Nyquist plots of the fabricated ZIHCs reveal two distinct regions: a semicircular region indicative of charge transfer resistance at high frequencies, and a linear region at low frequencies A quick diffusion process of Zn 2+ / SO 4 2− ions in the cathode material and low charge transfer resistance are demonstrated by the steep slope and small semicircle that were found in the low frequency and high frequency zones, respectively.…”

“…The ZIHC calculation methods of the C g (F g −1 ), power density (W kg −1 ), and energy density (W h kg −1 ) of the supercapacitors are consistent with ref. 39.…”

“…AH-PCs//Zn displays peak energy densities of 137.61 W h kg −1 at a power density of 80 W kg −1 and 69.78 W h kg −1 at 16 000 W kg −1 , considerably surpassing the This journal is © The Royal Society of Chemistry 2024 energy densities of earlier reported ZIHCs (Table S6 †). 39,50,51,54,68,[71][72][73][74][75] Typically, rapid charging and discharging at elevated current densities can readily compromise the integrity of electrode materials, resulting in a swi decline in electrode capacity 38 Nonetheless, the ability to charge/discharge at high currents remains a crucial metric for energy storage systems. In this work, the assembled AH-PCs//Zn demonstrates complete capacitance retention (100%) and nearly perfect coulombic efficiency (close to 100%) aer 20 000 cycles at 20 A g −1 , showcasing outstanding cycling stability (Fig.…”

Biomass-Derived Carbon Materials for Advanced Metal-Ion Hybrid Supercapacitors: A Step Towards More Sustainable Energy

“…Recent advancements in DFT calculations have shed light on the energy barriers involved in the adsorption and desorption of Zn 2+ ions on doped carbon electrodes, which is crucial for optimizing the chemisorption kinetics in ZIHSCs [239]. The addition of nitrogen and sulfur heteroatoms to the carbon structure considerably impacts the energy barriers, leading to improved electrochemical performance.…”