Key Takeaways & Executive Findings
- •• The critical bimetallic phosphide layer (CBPL) exhibits high electrical conductivity and forms heterostructures with NiCo-LDH, improving the electrical conductivity of the hybrid cathode (NiCo-P1.0). • CBPL facilitates OH⁻ adsorption and synergizes with NiCo-LDH in electrode reactions, delivering extra energy. • NiCo-P1.0 cathode delivers 286.64 mAh g⁻¹ at 1C with a retention of 72.22% at 40C, and the assembled NiCo-P1.0//Zn battery achieves energy density/power density of 503.62 Wh kg⁻¹/18.62 kW kg⁻¹. • The flexible quasi-solid-state pouch cell maintains stable output after deformation, validating practicality.
Abstract
Nickel-based cathodes in aqueous nickel-zinc batteries typically suffer from sluggish reaction kinetics and limited energy density. In situ introduction of metal phosphides and rational construction of heterostructures can effectively promote electron/ion transport. However, the complex evolution of phosphidation and intractable phosphidizing degree greatly affect the composition of active phase, active sites, charge transfer rate, and ion adsorption strength of cathodes. Herein, the critical bimetallic phosphide layer (CBPL) is constructed on the NiCo-layered double hydroxide (NiCo-LDH) skeleton by a controllable anion-exchange strategy, yielding a novel nanohybrid cathode (NiCo-P1.0, 1.0 representing the mass ratio of Na2H2PO2 to NiCo-LDH). The high-conductivity CBPL with the inner NiCo-LDH forms extensive heterostructures, effectively regulating the electronic structure via charge transfer, thereby improving electrical conductivity. Remarkably, the CBPL exhibits unexpected electrochemical activity and synergizes with NiCo-LDH for electrode reactions, ultimately delivering extra energy. Benefiting from the bifunctional CBPL, NiCo-P1.0 delivers an optimal capacity of 286.64 mAh g−1 at 1C (1C = 289 mAh g−1) and superb rate performance (a capacity retention of 72.22% at 40C). The assembled NiCo-P1.0//Zn battery achieves ultrahigh energy/power density (503.62 Wh kg−1/18.62 kW kg−1, based on the mass loading of active material on the cathode), and the flexible quasi-solid-state pouch cell validates its practicality. This work demonstrates the superiority of bifunctional CBPL for surface modification, providing an effective and scalable compositing strategy in achieving high-performance cathodes for aqueous batteries.
1. Introduction
With the gradual depletion of non-renewable energy sources and the inducing environmental crisis, the development of advanced and highly efficient energy storage units is of great significance [1]. Among numerous energy storage devices, aqueous zinc batteries (ZBs) are recognized as one of the most viable options for energy storage owing to their high energy density, intrinsic safety, and simple as well as inexpensive manufacturing process [2, 3]. As a member of the ZBs systems, nickel-zinc batteries (NZBs) have attracted extensive research interest due to their high discharge voltage (over 1.7 V) [4, 5].
There have been many successful studies about improving corrosion and dendrite problems for the zinc anode which mainly affect the safety and stability of batteries [6–8]. However, the nickel-based cathode, largely determining the upper-performance limit of NZBs, suffers from major obstacles: (1) limited energy density caused by the low utilization efficiency of the nickel cathode, (2) slow reaction kinetics due to inherently retarded electrical conductivity and stacking of high impedance by-products from irreversible phase transitions, and (3) capacity degradation induced by structural collapse [9–11]. As a result, the development of NZBs has been severely limited.
To tackle these impediments, researchers have adopted a series of strategies for nickel-based cathodes, containing doping metal atoms.
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Leixin Wu, Linfeng Lv, Yibo Xiong, Wenwu Wang, Xiaoqiao Liao, Xiyao Huang, Ruiqi Song, Zhe Zhu, Yixue Duan, Lei Wang, Zeyu Ma, Jiangwang Wang, Fazal ul Nisa, Kai Yang, Muhammad Tahir, Longbing Qu, Wenlong Cai, Liang He (2025). Critical Bimetallic Phosphide Layer Enables Fast Electron Transfer and Extra Energy Supply for Flexible Quasi-Solid-State Zinc Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01784-3
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Frequently Asked Questions
What is the critical bimetallic phosphide layer (CBPL) and how is it constructed?
The critical bimetallic phosphide layer (CBPL) is a high-conductivity layer constructed on the NiCo-layered double hydroxide (NiCo-LDH) skeleton via a controllable anion-exchange strategy, yielding a novel nanohybrid cathode (NiCo-P1.0).
How does the CBPL improve the performance of nickel-zinc batteries?
The CBPL forms heterostructures with NiCo-LDH, improving electrical conductivity and facilitating OH⁻ adsorption. It synergizes with NiCo-LDH in electrode reactions, delivering extra energy and enhancing capacity and rate performance.
What are the key performance metrics of the NiCo-P1.0 cathode?
The NiCo-P1.0 cathode delivers a capacity of 286.64 mAh g⁻¹ at 1C with a retention of 72.22% at 40C. The assembled NiCo-P1.0//Zn battery achieves an energy density of 503.62 Wh kg⁻¹ and a power density of 18.62 kW kg⁻¹.
What is the significance of the flexible quasi-solid-state pouch cell?
The flexible quasi-solid-state pouch cell maintains stable output after deformation, demonstrating the practicality of the CBPL-modified cathode for flexible energy storage applications.
What is the main contribution of this work?
This work demonstrates the superiority of bifunctional CBPL for surface modification, providing an effective and scalable compositing strategy to achieve high-performance cathodes for aqueous batteries.
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