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通过调节电子密度增强活性铁位点的硫氧化还原转化用于先进锂硫电池

Enhancing Sulfur Redox Conversion of Active Iron Sites by Modulation of Electronic Density for Advanced Lithium-Sulfur Battery.

作者信息

Zhang Fanchao, Tang Zihuan, Zhang Tengfei, Xiao Hong, Zhuang Huifeng, Liang Xiao, Zheng Lirong, Gao Qiuming

机构信息

Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, Beijing Advanced Innovation Center for Biomedical Engineering, School of Chemistry, Beihang University, Beijing, 100191, P. R. China.

The State Key Laboratory of Refractories and Metallurgy, Institute of Advanced Materials and Nanotechnology, Wuhan University of Science and Technology, Wuhan, 430081, P. R. China.

出版信息

Small Methods. 2023 Oct;7(10):e2300519. doi: 10.1002/smtd.202300519. Epub 2023 Jun 21.

DOI:10.1002/smtd.202300519
PMID:37344352
Abstract

Despite lithium-sulfur (Li-S) batteries possessing ultrahigh energy density as great promising energy storage devices, the suppressing shuttle effect and improving sulfur redox reaction (SROR) are vital for their practical application. Developing high-activity electrocatalysts for enhancing the SROR kinetics is a major challenge for the application of Li-S batteries. Herein, single-molecule iron phthalocyanine species are anchored on the N and P dual-doped porous carbon nanosheets (Fe-NPPC) via axial Fe-N coordination to optimize the electronic structure of active centers. The Fe-NPPC can promote the catalytic conversion of polysulfides by modulation of the electronic density in active moieties, endowing the Li-S battery with a high reversible capacity of 1023 mAh g at 1 C as well as an ultralow capacity decay of 0.035% per cycle over 1500 cycles. Even with a high sulfur loading of 7.1 mg cm , the Li-S battery delivers a high areal capacity of 4.8 mAh cm after 150 cycles at 0.2 C. With further increasing the sulfur loading to 9.2 mg cm , an excellent areal capacity of up to 9.3 mAh cm is obtained at 0.1 C.

摘要

尽管锂硫(Li-S)电池作为极具前景的储能装置具有超高能量密度,但抑制穿梭效应和改善硫氧化还原反应(SROR)对其实际应用至关重要。开发用于增强SROR动力学的高活性电催化剂是Li-S电池应用面临的一项重大挑战。在此,单分子铁酞菁物种通过轴向Fe-N配位锚定在N和P双掺杂多孔碳纳米片(Fe-NPPC)上,以优化活性中心的电子结构。Fe-NPPC可通过调节活性部分的电子密度促进多硫化物的催化转化,使Li-S电池在1 C下具有1023 mAh g的高可逆容量,以及在1500次循环中每循环0.035%的超低容量衰减。即使在硫负载量高达7.1 mg cm²的情况下,Li-S电池在0.2 C下经过150次循环后仍具有4.8 mAh cm²的高面积容量。随着硫负载量进一步增加至9.2 mg cm²,在0.1 C下可获得高达9.3 mAh cm²的优异面积容量。

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