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Multiscale control of MnO2 growth via [WO6]-perturbed [MnO6] assembly toward a favorable balance between capacitance and rate performance

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Abstract

Although pseudocapacitive manganese dioxide (MnO2) integrates the high-power merit of carbonaceous materials with the high-energy merit of battery-type materials, it still has a long way to go in achieving a more satisfactory balance of higher energy and power density, and in decoupling the relationship of structural characteristics with energy storage performance. To realize such goals, a bottom-up [WO6]-perturbed [MnO6] assembly strategy has been developed here due to their similar structure, yet mismatched lattice parameters. This facile protocol is capable of finely controlling the morphology and crystal structure of MnO2 by adjusting its internal [WO6] concentration. Therefore, the as-prepared Wx–MnO2 is treated as an ideal platform to scrutinize the correlations of the structure with the energy storage performance. The operando Raman spectra and finite element analysis have fully demonstrated the superiority of the locally ordered defects-enriched structure of W0.02–MnO2, which could reach a favorable balance between the ion diffusion equilibrium time and the number of active sites. As a result, the W0.02–MnO2 is able to deliver a high capacitance of 292 F·g−1 at a current density of 1 A·g−1 and a remarkable rate performance with a 60% capacity retention at a current density of 50 A·g−1. The further unveiled structure–performance relationship provides a guideline for the design of better pseudocapacitive energy storage devices.

Graphical Abstract

摘要

二氧化锰（MnO2）因结合了碳基材料的高功率密度与电池型材料的高能量密度优点，是一种极具潜力的赝电容型材料。目前，研究的主要方向是实现功率密度和能量密度之间更好的平衡，并解耦其结构与性能之间的构效关系。本研究采用了一种称为“自下而上”的策略，通过引入[WO6]扰动[MnO6]的组装来精确调整MnO2的结构。由于[WO6]和[MnO6]具有相似的结构单元但不同的晶格参数，通过调节MnO2内部的[WO6]浓度，可以精确控制所得产物的形貌、晶型和内部缺陷。原位拉曼光谱和有限元分析的结果表明：适度的[WO6]浓度（W0.02–MnO2）导致的局部有序、缺陷富集的结构，使得活性位点数量和离子扩散平衡时间达到最佳平衡。因此，该样品在1 A·g−1的电流密度下提供了292 F·g−1的高比电容，并在50 A·g−1的电流密度下保持着60%的容量。这项研究不仅提供了一种性能优越的储能材料，还揭示了结构-性能之间的关系，为下一代赝电容材料的设计提供了理论指导。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 22105164 and 21875205), the National Natural Science Foundation of Hebei Province (No. B2022203009), Hebei Province Foundation for the National Natural Science Foundation (No. 206Z4404G), and the subsidy for Hebei Key Laboratory of Applied Chemistry after Operation Performance (No. 22567616H). The authors also acknowledge Dr. Ning Dang from Xihua University for the help of COMSOL simulation.

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  1. Hebei Key Laboratory of Applied Chemistry, Yanshan University, Qinhuangdao, 066004, China

    Jin-Kang Liu, Tian-Shuo Yang, Zhi-Bin Ren, Adekunle-Adedapo Obisanya, Xin-Yi Tan, Yan-Di Rao, Jun-Shuang Zhou, Fa-Ming Gao & Jian-Ren Wang

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Liu, JK., Yang, TS., Ren, ZB. et al. Multiscale control of MnO2 growth via [WO6]-perturbed [MnO6] assembly toward a favorable balance between capacitance and rate performance. Rare Met. 43, 1658–1671 (2024). https://doi.org/10.1007/s12598-023-02542-3

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