RESUMO
Fabricating electrical double-layer capacitors (EDLCs) with high energy density for various applications has been of great interest in recent years. However, activated carbon (AC) electrodes are restricted to a lower operating voltage because they suffer from instability above a threshold potential window. Thus, they are limited in their energy storage. The deposition of inorganic compounds' atomic layer deposition (ALD) aiming to enhance cycling performance of supercapacitors and battery electrodes can be applied to the AC electrode materials. Here, we report on the investigation of zinc oxide (ZnO) coating strategy in terms of different pulse times of precursors, ALD cycles, and deposition temperatures to ensure high electrical conductivity and capacitance retention without blocking the micropores of the AC electrode. Crystalline ZnO phase with its optimal forming condition is obtained preferably using a longer precursor pulse time. Supercapacitors comprising AC electrodes coated with 20 cycles of ALD ZnO at 70 °C and operated in TEABF4/acetonitrile organic electrolyte show a specific capacitance of 23.13 F g-1 at 5 mA cm-2 and enhanced capacitance retention at 3.2 V, which well exceeds the normal working voltage of a commercial EDLC product (2.7 V). This work delivers an additional feasible approach of using ZnO ALD modification of AC materials, enhancing and promoting stable EDLC cells under high working voltages.
RESUMO
Designing the mesopore-dominated activated carbon electrodes has witnessed a significant breakthrough in enhancing the electrolyte breakdown voltage and energy density of supercapacitors. Herein, we designed N-doped mesoporous-dominated hierarchical activated carbon (N-dfAC) from the dragon fruit peel, an abundant biomass precursor, under the synergetic effect of KOH as the activating agent and melamine as the dopant. The electrode with the optimum N-doping content (3.4 at. %) exhibits the highest specific capacitance of 427 F g-1 at 5 mA cm-2 and cyclic stability of 123% capacitance retention until 50000 charge-discharge cycles at 500 mA cm-2 in aqueous 6 M KOH electrolytes. We designed a 4 V symmetric coin cell supercapacitor cell, which exhibits a remarkable specific energy and specific power of 112 W h kg-1 and 3214 W kg-1, respectively, in organic electrolytes. The cell also exhibits a significantly higher cycle life (109% capacitance retention) after 5000 GCD cycles at the working voltage of ≥3.5 V than commercial YP-50 AC (â¼60% capacitance retention). The larger Debye length of the diffuse ion layer permitted by the mesopores can explain the higher voltage window, and the polar N-doped species in the dfAC enhance capacitance and ion transport. The results endow a new path to design high-capacity and high-working voltage EDLCs from eco-friendly and sustainable biomass materials by properly tuning their pore structures.
RESUMO
Designing high voltage (>3â V) and stable electrochemical supercapacitors with low self-discharge is desirable for the applications in modern electronic devices. This work demonstrates a 4â V symmetric supercapacitor with stabilized cycling performance through atomic layer deposition (ALD) of alumina (Al2 O3 ) on the surface of activated carbon (AC). The 20-cycle ALD Al2 O3 coated AC delivers 84 % capacitance retention after 1000 charge/discharge cycles under 4â V, contrary to the bare AC cells having only 48 % retention. The extended cycling life is associated with the thickened Stern layer and suppressed oxygen functional group. The self-discharge data also show that the Al2 O3 coating enables AC cells to maintain 53 % of charge retention after 12â h, which is more than twice higher than that of bare AC cells under the same test protocol of 4â V charging. The curve fitting analysis reveals that ALD coating induced slow self-discharge dominated by ion diffusion mechanism, thus enhancing the AC surface energy.