Zinc–air batteries (ZABs) are promising as energy storage devices owing to their high energy density and the safety of electrolytes. Construction of abundant triple‐phase boundary (TPB) effectively facilitates cathode reactions occurring at TPB. Herein, a wood‐derived integral air electrode containing Co/CoO nanoparticles and nitrogen‐doped carbonized wood (Co/CoO@NWC) is constructed with a dual catalytic function. The potential gap between oxygen reduction and evolution is shortened to 0.77 V. Liquid ZABs using Co/CoO@NWC as cathode exhibit high discharge specific capacity (800 mAh gZn−1), low charge–discharge gap (0.84 V), and long‐term cycling stability (270 h). Co/CoO@NWC also shows distinguished catalytic activity and stability in all‐solid‐state ZABs. The inherent layered porous and pipe structures of wood are well maintained in catalytically active carbon. The different hydrophilicity of carbonized wood and Co/CoO endow abundant TPBs for battery reaction. The Co/CoO located on TPB provides main active sites for oxygen reactions. The inherent pipe structures of wood carbon and the interaction between Co/CoO and NWC effectively prevent nanoparticles from aggregation. The design and preparation of this monolithic electrocatalyst contribute to the broad‐scale application of ZABs and promote the development of next‐generation biomass‐based storage devices.
One challenge facing the development of air electrodes for Zn-air batteries (ZABs) is the embedment of active sites into carbon, which requires cracks and blends between powder and membrane and results in low energy efficiency during manufacturing and utilization. Herein, a surface phosphorization-monolithic strategy is proposed to embed CoO nanoparticles into paulownia carbon plate (P-CoO@PWC) as monolithic electrodes. Benefiting from the retention of natural transport channels, P-CoO@PWC-2 is conducive to the construction of three-phase interface structure for efficient mass transfer and high electrical conductivity. The electrode exhibits remarkable catalytic activities for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) with a small overpotential gap (E OER − E ORR = 0.68 V). Density functional theory calculations reveal that the incorporation of P on P-CoO@PWC-2 surface adjusts the electronic structure to promote the dissociation of water and the activation of oxygen, thus inducing catalytic activity. The monolithic P-CoO@PWC-2 electrode for quasi-solid-state or aqueous ZABs has excellent specific power, low charge-discharge voltage gap (0.83 V), and long-term cycling stability (over 700 cycles). This work serves as a new avenue for transforming abundant biomass into high-value energy-related engineering products.
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