Energy Storage Mechanism in Supercapacitors with Porous Graphdiynes: Effects of Pore Topology and Electrode Metallicity

作者：Tangming Mo, Zhenxiang Wang, Liang Zeng, Ming Chen, Alexei A. Kornyshev, Mingcai Zhang, Yongqing Zhao, Guang Feng · 发表于：Advanced Materials · 年份：2023 · DOI：10.1002/adma.202301118 · 被引用次数：58 · 研究领域：Supercapacitor Materials and Fabrication、Advancements in Battery Materials、Electrocatalysts for Energy Conversion

Porous graphdiynes are a new class of porous 2D materials with tunable electronic structures and various pore structures. They have potential applications as well-defined nanostructured electrodes and can provide platforms for understanding energy storage mechanisms underlying supercapacitors. Herein, the effect of stacking structure and metallicity on energy storage with such electrodes is investigated. Simulations reveal that supercapacitors based on porous graphdiynes of AB stacking structure can achieve both higher double-layer capacitance and ionic conductivity than AA stacking. This phenomenon is ascribed to more intense image forces in AB stacking, leading to a breakdown of ionic ordering and the formation of effective "free ions". Macroscale analysis shows that doped porous graphdiynes can deliver outstanding gravimetric and volumetric energy and power densities due to their enhanced quantum capacitance. These findings pave the way for designing high-performance supercapacitors by regulating pore topology and metallicity of electrode materials.