Enhanced Transformation Kinetics of Polysulfides Enabled by Synergistic Catalysis of Functional Graphitic Carbon Nitride for High-Performance Li-S Batteries

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Peng Chen, Tianyu Huang, Tianyu Wei, Bing Ding, Hui Dou, Xiaogang Zhang
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Abstract

The introduction of an electrocatalyst to accelerate the kinetics of lithium polysulfides (LiPSs) reduction/oxidation is beneficial to enhance the capacity of sulfur cathode and inhibit the shuttling effect of LiPSs. However, current electrocatalysts mainly focus on the metal-based active sites to reduce the reaction barriers, and there remains a great challenge in developing light-weighted metal-free catalysts. In this work, 1D graphitic carbon nitride nanorods (g-C3N4-NRs) with carboxyl (─COOH) and acylamide (─CONH2) functional groups are designed as metal-free electrocatalysts for lithium-sulfur batteries to accelerate the transport of Li+ and the conversion of LiPSs. The density functional theory (DFT) calculations prove that the existence of ─COOH group realizes the adsorption of LiPSs and accelerates the transport of Li+, while the ─CONH2 groups reduce the reaction energy barrier of S8 to Li2S. In addition, in situ UV–vis and Li2S nucleation/dissociation experiments also verify that g-C3N4-NRs achieve rapid adsorption and transformation of LiPSs under the synergistic action of ─COOH and ─CONH2 functional groups. Consequently, the sulfur cathode based on the g-C3N4-NRs-PP separator remains at a specific capacity of 700.3 mAh g−1 after 70 cycles at 0.2 C, at 0 °C. This work provides a new strategy for breaking through the bottleneck of metal-free catalysts for high-performance lithium-sulfur batteries.

Abstract Image

功能化石墨氮化碳协同催化高性能锂硫电池中多硫化物的强化转化动力学
引入电催化剂加速多硫化锂还原/氧化动力学,有利于提高硫阴极容量,抑制多硫化锂的穿梭效应。然而,目前电催化剂主要集中在金属基活性位点上,以降低反应障碍,开发轻质无金属催化剂仍然存在很大的挑战。在这项工作中,设计了具有羧基(─COOH)和酰基酰胺(─CONH2)官能团的1D石墨氮化碳纳米棒(g-C3N4-NRs)作为锂硫电池的无金属电催化剂,以加速Li+的运输和LiPSs的转化。密度泛函理论(DFT)计算证明─COOH基团的存在实现了LiPSs的吸附,加速了Li+的输运,而─CONH2基团的存在降低了S8对Li2S的反应能垒。此外,原位UV-vis和Li2S成核/解离实验也验证了g-C3N4-NRs在─COOH和─CONH2官能团的协同作用下实现了对LiPSs的快速吸附和转化。因此,基于g- c3n4 - nrs - pp分离器的硫阴极在0.2℃和0℃下循环70次后,比容量保持在700.3 mAh g−1。本工作为突破高性能锂硫电池无金属催化剂瓶颈提供了新的策略。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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