MIL-47 (V)中的硫醇中心酶模拟催化加速硫氧化还原,提高贫电解质锂硫电池的稳定性

IF 9.4 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Yangyang Dong, Dong Cai, Honglong Ning, Meiling Shu, Shuo Yang, Xuemei Zhou, Huagui Nie, Xingqiao Wu, Zhanshuang Jin, Zhi Yang
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引用次数: 0

摘要

然而,为了实现高能量密度的锂硫电池,设计定制的多功能催化剂来提高贫电解质硫氧化还原动力学是至关重要的。受天然酶活性位点结构保护的激励,我们将天然谷胱甘肽(GSH)植入金属-有机框架MIL-47 (V)腔中,用于GSH@MIL-47 (V)仿生催化剂,从而稳定和激活其硫醇功能。使用DTNB作为探针的定量证实了GSH的成功结合,表明GSH@MIL-47 (V)能够实现连续稳定的催化反应循环。此外,原位和原位光谱表明,硫醇驱动的S-S键断裂降低了反应能垒,同时促进了LiTFSI的分解。因此,GSH@MIL-47 (V)电池在6℃的倍率下,放电容量为733.1 mAh g-1,并在750次循环后保持573.0 mAh g-1。即使在5.5 μL mg-1的电解硫比下,它在0.5 c的高倍率下也能保持867.2 mAh g-1。这一策略突出了酶激发催化剂在增强锂硫电池方面的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Thiol centric enzyme mimetic catalysis within MIL-47 (V) accelerates sulfur redox and enhances stability for lean electrolyte lithium–sulfur batteries
Designing tailored multifunctional catalysts that enhance lean-electrolyte sulfur redox kinetics is crucial for achieving high-energy-density lithium-sulfur batteries, however, still remains challenge. Motivated by the structural protection of active sites in natural enzymes, we implant natural glutathione (GSH) within the metal-organic framework MIL-47 (V) cavity for GSH@MIL-47 (V) biomimetic catalysts, thereby stabilizing and activating its thiol functionality. Quantification using DTNB as a probe confirmed successful GSH incorporation, revealing that GSH@MIL-47 (V) enables a continuous and stable catalytic reaction cycle. Moreover, in-situ and ex-situ spectroscopies indicate thiol-driven S-S bond breakage that lowers the reaction energy barrier and concurrently promote LiTFSI decomposition. As a result, GSH@MIL-47 (V) cells, at 6 C rate, deliver a discharge capacity of 733.1 mAh g-1 and maintain 573.0 mAh g-1 after 750 cycles. Even under an electrolyte-to-sulfur ratio of 5.5 μL mg-1, it maintains 867.2 mAh g-1 at a high-rate of 0.5 C. This strategy highlights the potential of enzyme-inspired catalysts for enhancing lithium-sulfur batteries.
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来源期刊
Nano Research
Nano Research 化学-材料科学:综合
CiteScore
14.30
自引率
11.10%
发文量
2574
审稿时长
1.7 months
期刊介绍: Nano Research is a peer-reviewed, international and interdisciplinary research journal that focuses on all aspects of nanoscience and nanotechnology. It solicits submissions in various topical areas, from basic aspects of nanoscale materials to practical applications. The journal publishes articles on synthesis, characterization, and manipulation of nanomaterials; nanoscale physics, electrical transport, and quantum physics; scanning probe microscopy and spectroscopy; nanofluidics; nanosensors; nanoelectronics and molecular electronics; nano-optics, nano-optoelectronics, and nano-photonics; nanomagnetics; nanobiotechnology and nanomedicine; and nanoscale modeling and simulations. Nano Research offers readers a combination of authoritative and comprehensive Reviews, original cutting-edge research in Communication and Full Paper formats. The journal also prioritizes rapid review to ensure prompt publication.
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