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

被引：14

作者：

Cai, Lejuan ^{[1
]}

Lu, Lisha ^{[2
,3
,4
]}

Lan, Yingying ^{[1
]}

Zhang, Youming ^{[1
]}

Wang, Jianlin ^{[2
,3
]}

Lin, Zijia ^{[1
]}

Li, Renjie ^{[1
]}

Zhang, Fan ^{[1
]}

Yu, Jie ^{[1
]}

Lu, Wengang ^{[2
]}

Bai, Xuedong ^{[1
,2
,3
,4
]}

Wang, Wenlong ^{[1
,2
,3
,4
]}

机构：

[1] Songshan Lake Mat Lab, Dongguan 523808, Guangdong, Peoples R China

[2] Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China

[3] Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China

[4] Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100190, Peoples R China

来源：

ADVANCED ENERGY MATERIALS | 2023年 / 13卷 / 37期

基金：

中国国家自然科学基金;

关键词：

all Mn-ion batteries; coordination chemistry; covalent organic framework; multidentate chelation; organic electrodes; PERFORMANCE;

D O I：

10.1002/aenm.202301631

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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.

引用

页数：10