重塑锂镁混合电池:通过晶格匹配策略在 MgMOF 衬底上进行外延电沉积和空间限制

IF 19.5 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Carbon Energy Pub Date : 2024-03-15 DOI:10.1002/cey2.520
Yongqin Wang, Fulin Cheng, Jiawen Ji, Chenyang Cai, Yu Fu
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引用次数: 0

摘要

锂镁混合电池因其电化学动力学性能增强、过电位降低而备受关注。然而,镁电沉积不均匀这一长期存在的难题仍然是其实际集成的重大障碍。在此,我们开发了一种巧妙的方法,该方法以外延电结晶为核心,在专用的 MgMOF 基质上精心控制镁晶体的生长。所选的 MgMOF 衬底对镁具有强大的亲和力,与镁的晶格错位极小,为成功的异质外延电结晶创造了重要的先决条件。此外,在 MgMOF 结构中加入周期性电场和连续的纳米通道创造了一种空间限制环境,大大促进了分子尺度上镁的均匀成核。我们从大数据领域流行的 "区块链 "概念中汲取灵感,无缝集成了导电聚吡咯框架,作为连接 "链",将构成 MgMOF 空腔的 "区块 "相互连接。这种创新设计大大提高了电荷转移效率,从而增强了整体电化学动力学。由此产生的结构(MgMOF@PPy@CC)成为异质外延镁电沉积的特殊宿主,展示了卓越的电沉淀/电镀动力学和出色的循环性能。令人惊讶的是,采用 MgMOF@PPy@CC 电极的对称电池即使在超高电流密度条件下(10 mA cm-2)也表现出了令人印象深刻的稳定性,可维持长达 1200 小时的运行,超过了之前报告的基准。值得注意的是,在将 MgMOF@PPy@CC 阳极与 Mo6S8 阴极耦合后,组装后的电池在 70 C 下的寿命延长了 10,000 次,容量保持率高达 96.23%。这项研究为金属有机框架(MOF)基底驱动的外延电晶化的合理设计提供了一个全新的视角,为尖端电池的发展铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Reshaping Li–Mg hybrid batteries: Epitaxial electrodeposition and spatial confinement on MgMOF substrates via the lattice-matching strategy

Reshaping Li–Mg hybrid batteries: Epitaxial electrodeposition and spatial confinement on MgMOF substrates via the lattice-matching strategy

Reshaping Li–Mg hybrid batteries: Epitaxial electrodeposition and spatial confinement on MgMOF substrates via the lattice-matching strategy

The emergence of Li–Mg hybrid batteries has been receiving attention, owing to their enhanced electrochemical kinetics and reduced overpotential. Nevertheless, the persistent challenge of uneven Mg electrodeposition remains a significant impediment to their practical integration. Herein, we developed an ingenious approach that centered around epitaxial electrocrystallization and meticulously controlled growth of magnesium crystals on a specialized MgMOF substrate. The chosen MgMOF substrate demonstrated a robust affinity for magnesium and showed minimal lattice misfit with Mg, establishing the crucial prerequisites for successful heteroepitaxial electrocrystallization. Moreover, the incorporation of periodic electric fields and successive nanochannels within the MgMOF structure created a spatially confined environment that considerably promoted uniform magnesium nucleation at the molecular scale. Taking inspiration from the “blockchain” concept prevalent in the realm of big data, we seamlessly integrated a conductive polypyrrole framework, acting as a connecting “chain,” to interlink the “blocks” comprising the MgMOF cavities. This innovative design significantly amplified charge-transfer efficiency, thereby increasing overall electrochemical kinetics. The resulting architecture (MgMOF@PPy@CC) served as an exceptional host for heteroepitaxial Mg electrodeposition, showcasing remarkable electrostripping/plating kinetics and excellent cycling performance. Surprisingly, a symmetrical cell incorporating the MgMOF@PPy@CC electrode demonstrated impressive stability even under ultrahigh current density conditions (10 mA cm–2), maintaining operation for an extended 1200 h, surpassing previously reported benchmarks. Significantly, on coupling the MgMOF@PPy@CC anode with a Mo6S8 cathode, the assembled battery showed an extended lifespan of 10,000 cycles at 70 C, with an outstanding capacity retention of 96.23%. This study provides a fresh perspective on the rational design of epitaxial electrocrystallization driven by metal–organic framework (MOF) substrates, paving the way toward the advancement of cutting-edge batteries.

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来源期刊
Carbon Energy
Carbon Energy Multiple-
CiteScore
25.70
自引率
10.70%
发文量
116
审稿时长
4 weeks
期刊介绍: Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.
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