Engineering Self‐Supported Hydrophobic–Aerophilic Air Cathode with CoS/Fe₃S₄ Nanoparticles Embedded in S, N Co‐Doped Carbon Plate Arrays for Long‐Life Rechargeable Zn–Air Batteries

Abstract

The highly sluggish kinetics of oxygen reduction/evolution reactions (ORR/OER) at air cathodes lead to problems such as low power density and unsatisfactory cycling life with rechargeable Zn–air batteries (RZABs). To engineer the reaction kinetics at the air cathodes, a hydrophobic–aerophilic strategy is developed to fabricate a self‐supported air cathode based on CoS/Fe3S4 nanoparticles encapsulated in S, N co‐doped carbon plate arrays (CoS/Fe3S4@SNCP). It is experimentally shown that the in situ growth of bimetallic sulfides nanoparticles on the carbon plate arrays improves the intrinsic electrocatalytic activity and electron conduction of the air cathode. Meanwhile, the ab initio molecular dynamics simulations reveal that the hydrophobic–aerophilic surface can repel water molecules to create abundant solid–liquid–gas three‐phase reaction interfaces as well as to expose Fe‐sites, which consequently promote the diffusion of reactive molecules/ions across the interface and the oxygen adsorption. As a result, the CoS/Fe3S4@SNCP electrode exhibits excellent OER and ORR activities with a smaller potential gap of 0.65 V. For the engineered hydrophobicity of the catalyst, the RZAB demonstrates a high power density of 272 mW cm−2, a narrow discharge/charge gap of 0.75 V at 10 mA cm−2, and long‐term cycling stability over 1400 h, outperforming its hydrophilic CoS@SNCP counterparts.

Modulation of bulk and surface electronic structures for oxygen evolution by Cr, P co-doped Co3S4

“…Cr, P-Co 3 S 4 showed a lower system resistance ( R S ) (1.43 Ω) in comparison with the as-prepared catalysts and the corresponding EIS parameters were presented in Table S5 (ESI†). 20 The conductivity test proved the best conductivity of Cr, P-Co 3 S 4 and the leading role of Cr in the enhanced conductivity (Table S6, ESI†). Electrochemical stability is one of the important parameters in the evaluation of electrocatalysts.…”

Heterointerface promoted trifunctional electrocatalysts for all temperature high-performance rechargeable Zn–air batteries

“…Increased electrical transport requires high-energy rechargeable batteries that safely operate under harsh conditions and a wide range of temperatures. [1][2][3][4] Lithium-ion batteries (LIBs) suffer from limited capacity/power/energy, poor rate performances, and a short cycle life owing to the temperaturesensitive electrode dynamics and electrolyte freezing points with severe dendritic growth and lithium precipitation. 5,6 Zinc-air batteries (ZABs) are considered as the most promising next-generation green power devices featuring high theoretical energy density (1086 Wh kg À1 ), zero carbon emissions, low cost of electrode materials, earth abundance, and intrinsic safety.…”

“…5,6 Zinc-air batteries (ZABs) are considered as the most promising next-generation green power devices featuring high theoretical energy density (1086 Wh kg À1 ), zero carbon emissions, low cost of electrode materials, earth abundance, and intrinsic safety. [1][2][3][4]7,8 ZABs can reveal feasibility against widetemperature environments due to the ultralow and ultrahigh a Department of Materials Science and Chemical Engineering, Hanyang University, activation energies for the anode and cathode reactions resulting in temperature impervious electrode kinetics according to the Arrhenius equation. 9 However, ZABs suffer from poor reversibility, poor charging/discharging rates with high/low charge-discharge voltages, limited electrochemical and thermodynamic stability mainly because of the sluggish electrochemical oxygen reduction/evolution reaction (ORR/OER), and poor ion transport properties of the electrolytes.…”

(FeSe2 + CoSe2) Nanoparticles Anchored on 3D Porous Ultrathin Carbon Nanosheets for High-Activity Oxygen Evolution Reaction

“…3 Up to now, although IrO 2 and RuO 2 are still the most sophisticated OER catalysts, their widespread utilization has been greatly restricted by their scarcity of supplies and high cost. 4 Therefore, substantial research into cost-effective transition metal-based catalysts to replace IrO 2 and RuO 2 has been launched recently. 5 Nowadays, transition metal selenides have been demonstrated to be an excellent electrocatalyst toward OER due to the higher electrical conductivity compared to transition metal oxides, which significantly enhances the charge transportation, accelerating the reaction kinetics and improving the effectiveness of energy conversion during electrochemical processes.…”

“…Up to now, although IrO 2 and RuO 2 are still the most sophisticated OER catalysts, their widespread utilization has been greatly restricted by their scarcity of supplies and high cost . Therefore, substantial research into cost-effective transition metal-based catalysts to replace IrO 2 and RuO 2 has been launched recently .…”