基于预嵌入碘离子的锌碘电池高效电荷存储，电化学反应势垒降低和多碘化物自穿梭效应抑制,Advanced Functional Materials

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基于预嵌入碘离子的锌碘电池高效电荷存储，电化学反应势垒降低和多碘化物自穿梭效应抑制
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-01-31 , DOI: 10.1002/adfm.202211979
Wenzheng Gao ₁ , Situo Cheng ₁ , Yaxiong Zhang ₁ , Erqing Xie ₁ , Jiecai Fu ₁

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水系锌碘电池由于其高能量/功率密度和安全性而被认为是一种有前途的储能系统。然而，聚碘化物穿梭会导致严重的活性质量损失，从而导致较低的库仑效率并限制循环寿命。在此，提出了一种将碘离子预嵌入普鲁士蓝 (PBI) 中的新型结构限制策略。DFT计算和电化学表征表明，铁碘键的形成降低了预嵌入位点后续碘离子的电化学反应能垒，改善了I-^氧化反应动力学过程，抑制了聚碘自穿梭。PBI//Zn 电池表现出低 Tafel 斜率（155 mV dec ^-1). 此外，紫外-可见光谱证实所提出的策略抑制了聚碘化物的自穿梭。因此，PBI//Zn 电池实现了高碘化物利用率和库仑效率（在 0.2 A g ^{-1 时为 242 mAh g -1}^， CEs ≈ 100%），以及 197.2 mAh g ^-1的高多重性能，即使在10 A g ^-1（初始容量的 82%）。^{PBI//Zn 电池还具有出色的循环稳定性，在 4 A g -1}下 1500 次循环后容量保持率为 94% 。^{该器件在 5538 W kg -1}的功率密度下表现出 142 Wh kg ^-1的高能量密度。

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Efficient Charge Storage in Zinc–Iodine Batteries based on Pre-Embedded Iodine-Ions with Reduced Electrochemical Reaction Barrier and Suppression of Polyiodide Self-Shuttle Effect

Aqueous zincIodine batteries are considered as a promising energy storage system due to their high energy/power density, and safety. However, polyiodide shuttling leads to severe active mass loss, which results in lower Coulombic efficiency and limits the cyclic life. Herein, a novel structure-limiting strategy to pre-embed iodide ions into Prussian blue (PBI) is proposed. The DFT calculations and electrochemical characterization reveal that the formation of FerrumIodine bond reduces the electrochemical reaction energy barrier of subsequent iodide-ions at the pre-embedding sites, improves the I⁻ oxidation reaction kinetic process, and suppresses the polyiodide self-shuttle. The PBI//Zn batteries exhibit a low Tafel slope (155 mV dec⁻¹). Moreover, UV–vis spectroscopy confirms that the proposed strategy suppresses the polyiodide self-shuttle. As a result, the PBI//Zn battery achieves high iodide utilization and Coulomb efficiency (242 mAh g⁻¹ at 0.2 A g⁻¹, CEs ≈ 100%), as well as high multiplicity performance of 197.2 mAh g⁻¹ even at 10 A g⁻¹(82% of initial capacity). The PBI//Zn battery also renders excellent cyclic stability with a capacity retention of 94% at 4 A g⁻¹ after 1500 cycles. The device exhibits a high energy density of 142 W h kg⁻¹ at a power density of 5538 W kg⁻¹.

更新日期：2023-01-31

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