Cyclodextrin Metal–Organic Framework Functionalized Carbon Materials with Optimized Interface Electronics and Selective Supramolecular Channels for High‐Performance Lithium–Sulfur Batteries

作者：Bingxin Sun, Dan Wang, Yuxuan Jiang, Rui Wang, Lulu Lyu, Guowang Diao, Wang Zhang, Huan Pang · 发表于：Advanced Materials · 年份：2024 · DOI：10.1002/adma.202415633 · 被引用次数：100 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Advanced battery technologies research

S). Here, a microenvironment regulation strategy with optimized interface electronics and selective supramolecular channels, is proposed to enhance LiPS reaction kinetics through Lewis basic γ-cyclodextrin metal-organic framework (γ-CDMOF). To validate this concept, γ-CDMOF is rapidly synthesized on 3D graphene foam (GF) via a microwave-assisted method, resulting in a γ-CDMOF/GF cathode for high-performance Li-S batteries. A range of analytical techniques combined with density functional theory (DFT) calculations confirm that introducing a Lewis basic supramolecular microenvironment mitigates the LiPSs shuttle effect, enhances polysulfide capture, and improves sulfur redox conversion. Additionally, COMSOL simulations reveal that the γ-CDMOF framework and oxygen sites significantly reduce volumetric expansion stress during the LiPS solid-liquid phase transition. Impressively, the γ-CDMOF/GF cathode exhibits exceptional performance, including a high specific capacity (1253.01 mAh g⁻¹ at 0.1C), excellent rate performance (589.68 mAh g⁻¹ at 5C), and long cycle life (over 1200 cycles). This study introduces a new concept of supramolecular microenvironment regulation and interfacial interaction strategy, offering a unique approach for the development of multifunctional electrode materials.