Directional regulation on single-molecule redox-targeting reaction in neutral zinc-iron flow batteries

IF 38.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Joule Pub Date : 2024-10-22 DOI:10.1016/j.joule.2024.09.015

Yichong Cai, Hang Zhang, Tidong Wang, Shibo Xi, Yuxi Song, Sida Rong, Jin Ma, Zheng Han, Chee Tong John Low, Qing Wang, Ya Ji

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Abstract

Aqueous redox flow batteries (ARFBs) are promising long-duration energy storage systems but struggle with low-energy density due to the inherent properties of liquid electrolytes. Herein, we report a [Fe(CN)₆]^3−/4−-LiMn_xFe_{1 − x}PO₄/Zn flow battery utilizing redox-targeting (RT) electrochemical-chemical loop, exhibiting an outstanding energy density of 118.3 Wh L⁻¹, surpassing blank RFB by 5.6 times. Remarkably, the RT reaction between redox mediator [Fe(CN)₆]^3−/4− and solid energy booster LiMn_xFe_{1 − x}PO₄ is directionally regulated, clearly revealing the quantitative relation between capacity enhancement and potential difference. Moreover, unprecedented Coulombic efficiency (99.9%), solid booster utilization (78.4%), and capacity retention (99.8% per cycle) are achieved at 10 mA cm⁻². Intriguingly, operando synchrotron X-ray absorption spectroscopy unveils the reversible changes of the Fe–O and Fe–Fe bonds in the [Fe(CN)₆]^3−/4−-LiMn_xFe_{1 − x}PO₄ RT system during real-time monitoring. This work suggests an appealing way for capacity enhancement in ARFBs and provides profound insight into the fundamental chemistry of the RT reaction in safe, energy-dense batteries.

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中性锌-铁液流电池中单分子氧化还原定向反应的定向调节

水氧化还原液流电池（ARFB）是一种前景广阔的长效储能系统，但由于液态电解质的固有特性，其能量密度较低。在此，我们报告了一种利用氧化还原靶向（RT）电化学循环的[Fe(CN)6]3-/4--LiMnxFe1 - xPO4/Zn液流电池，其能量密度高达118.3 Wh L-1，是空白液流电池的5.6倍。值得注意的是，氧化还原介质[Fe(CN)6]3-/4-与固体增能剂 LiMnxFe1 - xPO4 之间的 RT 反应是定向调节的，清楚地揭示了容量增强与电位差之间的定量关系。此外，在 10 mA cm-2 的条件下，还实现了前所未有的库仑效率（99.9%）、固体增能剂利用率（78.4%）和容量保持率（每周期 99.8%）。有趣的是，在实时监测过程中，操作同步辐射 X 射线吸收光谱揭示了[Fe(CN)6]3-/4--LiMnxFe1 - xPO4 RT 系统中 Fe-O 和 Fe-Fe 键的可逆变化。这项工作为提高 ARFB 的容量提供了一种有吸引力的方法，并对安全、高能量电池中 RT 反应的基本化学原理提供了深刻的见解。

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来源期刊

Joule Energy-General Energy

CiteScore

53.10

自引率

2.00%

发文量

198

期刊介绍： Joule is a sister journal to Cell that focuses on research, analysis, and ideas related to sustainable energy. It aims to address the global challenge of the need for more sustainable energy solutions. Joule is a forward-looking journal that bridges disciplines and scales of energy research. It connects researchers and analysts working on scientific, technical, economic, policy, and social challenges related to sustainable energy. The journal covers a wide range of energy research, from fundamental laboratory studies on energy conversion and storage to global-level analysis. Joule aims to highlight and amplify the implications, challenges, and opportunities of novel energy research for different groups in the field.