Resolving Deactivation of Low-Spin Fe Sites by Redistributing Electron Density toward High-Energy Sodium Storage

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2023-11-13 DOI:10.1021/acs.nanolett.3c03065

Mingwei Jiang, Zhidong Hou, Honghao Ma, Jinjin Wang, Wei Hua, Lingbo Ren, Yu Zhang*, Chunguang Wei, Feiyu Kang and Jian-Gan Wang*,

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Abstract

Prussian blue (PB) has been an emerging class of cathode material for sodium-ion batteries due to its low cost and high theoretical capacity. However, their working voltage and capacity are substantially restricted due to the deactivation of low-spin Fe sites. Herein, we demonstrate a universal strategy to activate the low-spin Fe sites of PB by hybridizing them with the π–π conjugated electronic conductors. The redistribution of electron density between π–π conjugated conductors and PB effectively promotes the participation of low-spin Fe sites in sodium storage. Consequently, the low-spin Fe-induced plateau is greatly aroused, resulting in a high specific capacity of 148.4 mAh g^–1 and remarkable energy density of 444.2 Wh kg^–1. In addition, the excellent structural stability enables superior cycling stability over 2500 cycles and outstanding rate performance. The work will provide fundamental insight into activating the low-spin Fe sites of PB for advanced battery technologies.

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通过重新分配电子密度来解决低自旋铁位的失活问题。

普鲁士蓝(PB)由于其低廉的成本和较高的理论容量而成为钠离子电池正极材料中的一种新兴材料。然而，由于低自旋铁位失活，它们的工作电压和容量受到很大限制。在这里，我们展示了一种通用的策略，通过π-π共轭电子导体杂化来激活PB的低自旋铁位。π-π共轭导体与PB之间电子密度的重新分布有效地促进了低自旋铁位参与钠的储存。因此，低自旋铁诱导的平台被极大地激发，从而产生148.4 mAh g-1的高比容量和444.2 Wh kg-1的显著能量密度。此外，优异的结构稳定性使其具有超过2500次循环的优越循环稳定性和出色的速率性能。这项工作将为激活PB的低自旋铁位点为先进的电池技术提供基本的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.