Nano-carbon supported B/N-coordinated Fe single atoms with a tuned electronic structure for long lifespan zinc–iodine batteries†

IF 30.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yong Li, Aoyang Zhu, Guodong Peng, Jun He, Hongqiang Li, Dedong Jia, Guanjie He, Jieshan Qiu and Xiaojun He
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Abstract

Single-atom catalysts (SACs) have great potential to boost the sluggish iodine redox kinetics and alleviate the polyiodide shuttle in aqueous zinc–iodine (Zn–I2) batteries. Nevertheless, it is a big challenge to improve the catalytic activity of traditional metal nitrogen (M–N4) SACs by adjusting the microenvironment to enhance iodine redox kinetics. Herein, asymmetric B/N-coordinated Fe single atoms (Fe–B2N2) immobilized on carbon nanotube forests (denoted as Fe-SAs@BNCF) are prepared by a one-pot calcination method and used as the iodine host in Zn–I2 batteries. Theoretical calculation results have revealed that the B sites function to increase the electron density by disrupting the symmetrical electron distribution around the Fe sites compared to traditional Fe–N4. Correspondingly, the as-synthesized Fe–B2N2 SACs significantly improve polyiodide adsorption and electrocatalytic activities in Zn–I2 batteries. Moreover, carbon nanotube forests provide more adsorption sites for polyiodides. Consequently, the Zn–I2 batteries with Fe-SAs@BNCF as a host enable a superb long lifespan (78% retention over 60 000 cycles at 5 A g−1) and a high rate capability (147 mA h g−1 at 10 A g−1). This work provides a promising strategy for designing advanced I2 cathodes with asymmetric single atoms for long-life Zn–I2 batteries.

Abstract Image

具有调谐电子结构的纳米碳负载B/ n配位铁单原子用于长寿命锌碘电池
单原子催化剂(SACs)在改善水相锌-碘(Zn-I2)电池中碘氧化还原动力学和缓解多碘离子穿梭方面具有很大的潜力。然而,如何通过调节微环境增强碘氧化还原动力学来提高传统金属氮(M-N4) SACs的催化活性是一个很大的挑战。本文采用一锅烧结法将不对称B/ n配位铁单原子(Fe- b2n2)固定在碳纳米管森林(表示为Fe-SAs@BNCF)上,并将其用作锌- i2电池的碘载体。理论计算结果表明,与传统的Fe- n4相比,B位通过破坏Fe位周围的对称电子分布来增加电子密度。相应地,合成的Fe-B2N2 SACs显著提高了Zn-I2电池对多碘化物的吸附和电催化活性。此外,碳纳米管森林为多碘化物提供了更多的吸附位点。因此,以Fe-SAs@BNCF为主体的锌- i2电池具有超长的使用寿命(在5 A g−1下超过60,000次循环保持78%)和有效的倍率能力(在10 A g−1下147 mAh g−1)。这项工作为设计具有不对称单原子的先进I2阴极提供了一种有前途的策略,用于长寿命锌-I2电池。
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
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
期刊介绍: Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).
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