Multidentate Chelation Enables High-Efficiency Mn2+ Storage in Polyimide Covalent Organic Framework for Aqueous All Mn-Ion Battery,Advanced Energy Materials

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Multidentate Chelation Enables High-Efficiency Mn2+ Storage in Polyimide Covalent Organic Framework for Aqueous All Mn-Ion Battery
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-08-17 , DOI: 10.1002/aenm.202301631
Lejuan Cai ₁ , Lisha Lu ₂ , Yingying Lan ₁ , Youming Zhang ₁ , Jianlin Wang ₂ , Zijia Lin ₁ , Renjie Li ₁ , Fan Zhang ₁ , Jie Yu ₁ , Wengang Lu _{2,

3} , Xuedong Bai _{1,

2,

3} , Wenlong Wang _{1,

2,

3}

Affiliation

Aqueous divalent manganese ions (Mn²⁺) have recently emerged as a promising candidate for the development of multivalent ion rechargeable batteries. Here, a multidentate chelation strategy is demonstrated for high-efficiency Mn²⁺ storage in a polyimide covalent organic framework (PI-COF) anode based on the understanding of Mn²⁺ coordination chemistry. In contrast to other multivalent cations, Mn²⁺ can bond with two adjacent enolized carbonyl groups and the triazine ring to form a novel multidentate chelation configuration in charged PI-COF lattice. As such, a large Mn²⁺ storage capacity of 120 mAh g⁻¹ at 0.2 A g⁻¹ along with great cycling stability can be achieved in PI-COF. Ex situ characterization and first-principles calculations further identify the occurrence of polydentate Mn²⁺ coordination and its critical role in stabilizing the enolized PI-COF intermediates. Notably, an all Mn-ion prototype cell assembly is demonstrated by coupling a PI-COF/Mn²⁺ anode with a high-voltage cathode based on MnO₂/Mn²⁺ conversion reaction. The well-designed cell exhibits a stable discharge plateau of 1.28 V and an impressive capacity of 115 mAh g⁻¹ at the current density of 0.2 A g⁻¹. This work highlights the utility of coordination chemistry for achieving highly efficient energy storage by optimizing the matching between energy-carrying ions and organic host materials.

中文翻译：

多齿螯合可在水系全锰离子电池的聚酰亚胺共价有机框架中高效存储 Mn2+

含水二价锰离子（Mn ²⁺）最近已成为开发多价离子可充电电池的有希望的候选者。^{在此，基于对 Mn 2+}配位化学的理解，证明了多齿螯合策略可在聚酰亚胺共价有机骨架 (PI-COF) 阳极中高效存储 Mn ²⁺。与其他多价阳离子相比，Mn ²⁺可以与两个相邻的烯醇化羰基和三嗪环键合，在带电的PI-COF晶格中形成新型多齿螯合构型。因此，在0.2 A g ^-1下，Mn²⁺存储容量为120 mAh g ^-1PI-COF 可以实现出色的循环稳定性。^{非原位表征和第一原理计算进一步确定了多齿Mn 2+}配位的发生及其在稳定烯醇化PI-COF中间体中的关键作用。值得注意的是，通过将 PI-COF/Mn ^{2+阳极与基于 MnO}₂ /Mn ²⁺转化反应的高压阴极耦合来演示全锰离子原型电池组件。精心设计的电池在0.2 A g ⁻¹的电流密度下表现出1.28 V的稳定放电平台和115 mAh g ^{−1的令人印象深刻的容量}。这项工作强调了配位化学通过优化载能离子和有机主体材料之间的匹配来实现高效能量存储的效用。

更新日期：2023-08-17

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