Co-Based Metal–Organic Frameworks With Dual Redox Active Centers for Lithium-Ion Batteries With High Capacity and Excellent Rate Capability,Advanced Energy Materials

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Co-Based Metal–Organic Frameworks With Dual Redox Active Centers for Lithium-Ion Batteries With High Capacity and Excellent Rate Capability
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-09-09 , DOI: 10.1002/aenm.202402489
Lihong Su ₁ , Jin Chen ₁ , Jianzhong Zhou ₁ , Junjie Liu ₂ , Zhongli Hu ₁ , Sha Li ₃ , Xuebu Hu ₁ , Liang liang Xu ₄ , Li Zhang ₂

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Small molecule organic materials are widely used as anode materials for lithium-ion batteries (LIBs) due to their high reversible capacity, designable structure, and environmental friendliness. However, they suffer from poor intrinsic electronic conductivity, severe dissolution, and low initial coulombic efficiency. Recently, metal–organic frameworks (MOFs) have demonstrated in metal-ion batteries, outperforming some small molecule organic materials in terms of both cycling stability and rate capability. Herein, the first rational design and synthesis of a new cobalt-based MOF (CoBPDCA), are reported employing cobalt(II) nitrate as the metal source and small organic molecules (2,2-bipyridyl-4,4-dicarboxylic acid, BPDCA) as the ligands, which shows exceptional chemical stability and impressive electron conductivity. Most importantly, CoBPDCA electrodes deliver a high reversible capacity of 1112.9 mAh g⁻¹ at 0.05 C (1 C = 1000 mA g⁻¹) and outstanding high-rate durability (166.3 mAh g⁻¹ after 2500 cycles at 10 C). Employing a series of spectroscopic and morphological characterizations and density functional theory (DFT) calculations, it is revealed that these impressively electrochemical performances are contributed to the dual active redox centers of Co cations and BPDCA ligands (CN and CO groups), and the superb electron conductivity. This work might provide a new strategy and a deeper understanding of the other MOFs' development for LIBs.

中文翻译：

具有双氧化还原活性中心的共基金属-有机框架，用于锂离子电池，具有高容量和出色的倍率能力

小分子有机材料因其高可逆容量、可设计结构和环境友好性而被广泛用作锂离子电池（LIB）的负极材料。然而，它们的本征电子导电性差、溶解严重和初始库仑效率低。最近，金属有机框架（MOF）已在金属离子电池中得到证明，在循环稳定性和倍率能力方面都优于一些小分子有机材料。在此，报道了一种新的钴基 MOF （CoBPDCA）的首次合理设计和合成，以硝酸钴（II）为金属源，有机小分子（2,2-联吡啶基-4,4-二羧酸，BPDCA）作为配体，表现出优异的化学稳定性和令人印象深刻的电子导电性。最重要的是，CoBPDCA 电极在 0.05 C 下提供 1112.9 mAh g ⁻¹ 的高可逆容量（1 C = 1000 mA g ⁻¹ ）和出色的高倍率耐用性（在 10 C 下循环 2500 次后 166.3 mAh g ⁻¹ ）。采用一系列光谱和形态学表征以及密度泛函理论（DFT）计算，揭示了这些令人印象深刻的电化学性能有助于钴阳离子和 BPDCA 配体（CN 和 CO 基团）的双活性氧化还原中心以及极好的电子导电性。这项工作可能为其他 MOF 对 LIBS 的发展提供新的策略和更深入的理解。

更新日期：2024-09-09

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