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A Pyrazine-Pyridinamine Covalent Organic Framework as a Low Potential Anode for Highly Durable Aqueous Calcium-Ion Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-11-13 , DOI: 10.1002/aenm.202302495 Chunfang Wang 1, 2, 3 , Ran Li 4 , Yuchao Zhu 2 , Yaxin Wang 2 , Yilun Lin 2 , Leheng Zhong 2 , Hui Chen 2 , Zijie Tang 2 , Hongfei Li 2, 5 , Feng Liu 1, 3 , Chunyi Zhi 2, 3, 6 , Haiming Lv 2, 6
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-11-13 , DOI: 10.1002/aenm.202302495 Chunfang Wang 1, 2, 3 , Ran Li 4 , Yuchao Zhu 2 , Yaxin Wang 2 , Yilun Lin 2 , Leheng Zhong 2 , Hui Chen 2 , Zijie Tang 2 , Hongfei Li 2, 5 , Feng Liu 1, 3 , Chunyi Zhi 2, 3, 6 , Haiming Lv 2, 6
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Rechargeable aqueous calcium-ion batteries (CIBs) are promising for reliable large-scale energy storage. However, they face significant challenges, primarily stemming from suboptimal anodes, resulting in unfavorable voltage profiles, limited capacity, and diminished durability, all of which hinder the development of CIBs. Here, a covalent organic framework (PTHAT-COF) featuring repeated pyrazine and pyridinamine units, employed as the anode material for aqueous CIBs, is introduced. This innovative approach results in a remarkably flat ultralow potential plateau ranging from −0.6 to −1.05 V (vs Ag/AgCl), attributed to the high level of the lowest unoccupied molecular orbital. Furthermore, the PTHAT-COF anode exhibits outstanding rate performance (152.3 mAh g−1 @ 1 A g−1), exceptional long-term cycling stability, and remarkable capacity retention (10 000 cycles with 89.9% retention). Mechanistic studies, including experimental and theoretical calculations, reveal that C═N active sites reversibly trap Ca2+ ions via chemisorption during the discharging/charging process. The PTHAT-COF demonstrates exceptional structural stability throughout cycling. Finally, by pairing PTHAT-COF with a high-voltage manganese-based Prussian blue cathode, a complete aqueous CIB with a voltage interval of 2.2 V is achieved, exhibiting extraordinary durability (10 000 cycles with 83.6% retention). This research illuminates the potential of organic anode materials in aqueous batteries to achieve higher battery voltages.
中文翻译：
吡嗪-吡啶胺共价有机骨架作为高耐用水系钙离子电池的低电位阳极
可充电水性钙离子电池（CIB）有望用于可靠的大规模能源存储。然而，它们面临着重大挑战，主要是由于阳极不理想，导致电压分布不利、容量有限和耐用性下降，所有这些都阻碍了 CIB 的发展。在此，引入了一种具有重复吡嗪和吡啶胺单元的共价有机骨架（PTHAT-COF），用作水性 CIB 的阳极材料。这种创新方法产生了非常平坦的超低电位平台，范围从-0.6到-1.05 V（相对于Ag/AgCl），这归因于最低未占据分子轨道的高水平。此外，PTHAT-COF负极表现出出色的倍率性能（152.3 mAh g −1 @ 1 A g −1）、出色的长期循环稳定性和显着的容量保持率（10 000次循环，保持率89.9%）。包括实验和理论计算在内的机理研究表明，C=N活性位点在放电/充电过程中通过化学吸附可逆地捕获Ca 2+离子。PTHAT-COF 在整个循环过程中表现出卓越的结构稳定性。最后，通过将 PTHAT-COF 与高压锰基普鲁士蓝阴极配对，实现了电压间隔为 2.2 V 的完整水性 CIB，表现出非凡的耐用性（10 000 次循环，保留率为 83.6%）。这项研究阐明了有机阳极材料在水性电池中实现更高电池电压的潜力。
更新日期：2023-11-13
中文翻译：
吡嗪-吡啶胺共价有机骨架作为高耐用水系钙离子电池的低电位阳极
可充电水性钙离子电池（CIB）有望用于可靠的大规模能源存储。然而，它们面临着重大挑战，主要是由于阳极不理想，导致电压分布不利、容量有限和耐用性下降，所有这些都阻碍了 CIB 的发展。在此，引入了一种具有重复吡嗪和吡啶胺单元的共价有机骨架（PTHAT-COF），用作水性 CIB 的阳极材料。这种创新方法产生了非常平坦的超低电位平台，范围从-0.6到-1.05 V（相对于Ag/AgCl），这归因于最低未占据分子轨道的高水平。此外，PTHAT-COF负极表现出出色的倍率性能（152.3 mAh g −1 @ 1 A g −1）、出色的长期循环稳定性和显着的容量保持率（10 000次循环，保持率89.9%）。包括实验和理论计算在内的机理研究表明，C=N活性位点在放电/充电过程中通过化学吸附可逆地捕获Ca 2+离子。PTHAT-COF 在整个循环过程中表现出卓越的结构稳定性。最后，通过将 PTHAT-COF 与高压锰基普鲁士蓝阴极配对，实现了电压间隔为 2.2 V 的完整水性 CIB，表现出非凡的耐用性（10 000 次循环，保留率为 83.6%）。这项研究阐明了有机阳极材料在水性电池中实现更高电池电压的潜力。
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