Significantly raising tetracyanoquinodimethane electrode performance in zinc-ion battery at low temperatures by eliminating impurities,Battery Energy

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Significantly raising tetracyanoquinodimethane electrode performance in zinc-ion battery at low temperatures by eliminating impurities
Battery Energy ( IF 9.0 ) Pub Date : 2023-02-09 , DOI: 10.1002/bte2.20220050
Shuchan Wang ₁ , Wenwen Deng ₁ , Zhiyuan Geng ₁ , Peiyuan Li ₁ , Naiqi Hu ₁ , Limin Zhu ₂ , Wei Sun ₃ , Chang M. Li ₁

Affiliation

Applications of organic compounds-based electrodes in aqueous zinc-ion batteries (AZIBs) at low temperatures are severely restricted by the freezing of aqueous electrolytes and the inferior dynamic behavior of organic electrodes below zero. Herein, tetracyanoquinodimethane (TCNQ) was purified by the sublimation method and used as a cathode in AZIBs to investigate electrochemical Zn storage performance in comparison with nonpurified TCNQ at a temperature range of 25°C to −40°C. Nuclear magnetic resonance and elemental analysis prove increased purity in purified TCNQ (p-TCNQ), whereas scanning electron microscope and Brunner−Emmet−Teller data verify reduced particle size and increased surface area of p-TCNQ. Kinetic analysis demonstrates that p-TCNQ is a more surface-controlled electrode process than TCNQ and offers much higher ionic diffusivity than the latter at various temperatures. Molecular dynamics simulation validates that the existence of impurity increases the absorption energy of TCNQ in a TCNQ//Zn system that is unfavorable to Zn migration. Comprehensive analysis, including ex situ X-ray diffraction, Fourier transform infrared, Raman, and electron spin-resonance spectroscopy characterization confirm the high reversibility of transformation between C≡N and −C═N groups in p-TCNQ. This work provides a simple, environmentally friendly strategy to fabricate a high-performance AZIB at low temperatures while offering fundamental chemistry insight into organic electrode performance, thus possessing universal significance.

中文翻译：

通过去除杂质显着提高锌离子电池中四氰基醌二甲烷电极的低温性能

基于有机化合物的电极在低温下水系锌离子电池（AZIB）中的应用受到水系电解质冻结和有机电极低于零的较差动态行为的严重限制。在此，四氰基喹啉二甲烷 (TCNQ) 通过升华法纯化并用作 AZIB 的阴极，以研究在 25°C 至 -40°C 的温度范围内与未纯化的 TCNQ 相比的电化学 Zn 存储性能。核磁共振和元素分析证明纯化的 TCNQ (p-TCNQ) 的纯度增加，而扫描电子显微镜和 Brunner-Emmet-Teller 数据证实 p-TCNQ 的粒径减小和表面积增加。动力学分析表明，p-TCNQ 是一种比 TCNQ 更受表面控制的电极过程，并且在各种温度下提供比后者高得多的离子扩散率。分子动力学模拟证实，杂质的存在增加了TCNQ//Zn体系中TCNQ的吸收能，不利于Zn的迁移。综合分析，包括非原位 X 射线衍射、傅里叶变换红外、拉曼和电子自旋共振光谱表征，证实了 p-TCNQ 中 C≡N 和 -C=N 基团之间转变的高度可逆性。这项工作提供了一种简单、环保的策略来在低温下制造高性能 AZIB，同时提供对有机电极性能的基础化学洞察，因此具有普遍意义。

更新日期：2023-02-09

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