Interfacial Charge Redistribution–Driven Two‐Electron Conversion in Ni0.85Se@Mo‐Doped NiCo‐LDH for High‐Power Electrochemical Energy Storage

Why It Matters

The breakthrough demonstrates that precise interfacial engineering and defect control can dramatically boost both energy and power metrics of supercapacitors, narrowing the performance gap with batteries and enabling faster, longer‑lasting grid‑scale storage solutions.

Key Takeaways

• Ni0.85Se core provides fast electron transport and mechanical strength
• Mo‑doped NiCo‑LDH shell creates oxygen vacancies for extra redox sites
• Interfacial charge redistribution enables efficient two‑electron transfer
• 540.8 mAh g⁻¹ at 1 A g⁻¹, 81.8% retention at 32 A g⁻¹
• Hybrid supercapacitor delivers 128.5 Wh kg⁻¹ at 750 W kg⁻¹, 10k‑cycle stability

Pulse Analysis

High‑power electrochemical storage hinges on electrode materials that can move ions and electrons at lightning speed while storing ample charge. Traditional carbon‑based supercapacitors excel in power but fall short on energy density, whereas battery electrodes offer energy at the expense of rate capability. By integrating a conductive Ni0.85Se core with a Mo‑doped NiCo‑LDH shell directly onto a hydrophilic carbon cloth, the researchers created a continuous conductive network that also introduces abundant active sites, addressing both power and energy constraints in a single architecture.

The key to the material’s performance lies in its engineered interfacial chemistry. Mo doping generates oxygen vacancies within the NiCo‑LDH lattice, altering the electronic structure and fostering charge redistribution across the core‑shell boundary. Density functional theory calculations confirm that this redistribution lowers the activation barrier for a two‑electron redox reaction, effectively turning what is typically a single‑electron process into a multi‑electron pathway. In‑situ Raman spectroscopy and relaxation‑time analyses verify rapid charge transfer and reversible phase transitions, translating the theoretical advantage into measurable capacity gains.

When assembled into a hybrid supercapacitor, the heterostructure delivers 128.5 Wh kg⁻¹ at a respectable 750 W kg⁻¹, rivaling many lithium‑ion batteries while retaining supercapacitor‑level cyclability—over 10,000 cycles with less than 20% loss. Such metrics suggest a viable route for grid‑scale applications where both quick response and long‑term durability are essential. The scalable carbon‑cloth substrate and straightforward hydrothermal synthesis further enhance commercial appeal, positioning this interfacial engineering strategy as a template for future high‑power, high‑energy storage technologies.