水溶液鋅離子儲能裝置用高倍率二維聚芳醯亞胺共價有機骨架陽極
作者:
小柯機器人發布時間:2020/11/14 16:34:37
可再充式水溶液鋅離子儲能裝置是下一代儲能技術中非常有前途的一種候選裝置。然而,缺乏具有低電位窗口的高可逆Zn2+儲存陽極材料仍然是人們關注的主要問題。
研究人員研製了一種具有高動力學Zn2+儲存能力的二維聚芳醯亞胺共價有機骨架(PI-COF)陽極。PI-COF的孔道結構良好,具有很高的內建氧化還原活性羰基和低勢壘的離子擴散。所構建的PI-COF陽極具有特定的容量(332 C g–1或92 mAh g–1,0.7 a g–1),高速率容量(7Ag–1時為79.8%),長循環壽命(4000次循環中為85%)。原位拉曼光譜研究和第一性原理計算闡明了醯亞胺羰基可逆形成帶負電荷的烯醇酸鹽的Zn2+兩步儲存機理。採用PI-COF陽極與MnO2陰極耦合的方法製備了無枝晶全鋅離子裝置,其具有優良的能量密度(23.9~66.5 Wh kg–1)和超級電容器級功率密度(133~4782 W kg–1)。
該研究驗證了共價有機骨架作為Zn2+儲能陽極的可行性,為構建可靠的水儲能裝置提供了良好的前景。
附:英文原文
Title: A High-Rate Two-Dimensional Polyarylimide Covalent Organic Framework Anode for Aqueous Zn-Ion Energy Storage Devices
Author: Minghao Yu, Naisa Chandrasekhar, Ramya Kormath Madam Raghupathy, Khoa Hoang Ly, Haozhe Zhang, Evgenia Dmitrieva, Chaolun Liang, Xihong Lu, Thomas D. Kühne, Hossein Mirhosseini, Inez M. Weidinger, Xinliang Feng
Issue&Volume: November 9, 2020
Abstract: Rechargeable aqueous Zn-ion energy storage devices are promising candidates for next-generation energy storage technologies. However, the lack of highly reversible Zn2+-storage anode materials with low potential windows remains a primary concern. Here, we report a two-dimensional polyarylimide covalent organic framework (PI-COF) anode with high-kinetics Zn2+-storage capability. The well-organized pore channels of PI-COF allow the high accessibility of the build-in redox-active carbonyl groups and efficient ion diffusion with a low energy barrier. The constructed PI-COF anode exhibits a specific capacity (332 C g–1 or 92 mAh g–1 at 0.7 A g–1), a high rate capability (79.8% at 7 A g–1), and a long cycle life (85% over 4000 cycles). In situ Raman investigation and first-principle calculations clarify the two-step Zn2+-storage mechanism, in which imide carbonyl groups reversibly form negatively charged enolates. Dendrite-free full Zn-ion devices are fabricated by coupling PI-COF anodes with MnO2 cathodes, delivering excellent energy densities (23.9 ~ 66.5 Wh kg–1) and supercapacitor-level power densities (133 ~ 4782 W kg–1). This study demonstrates the feasibility of covalent organic framework as Zn2+-storage anodes and shows a promising prospect for constructing reliable aqueous energy storage devices.
DOI: 10.1021/jacs.0c07992
Source: https://pubs.acs.org/doi/10.1021/jacs.0c07992