Fast and stable NH4+ storage in multielectron H-bonding-acceptor organic molecules for aqueous zinc batteries.

IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Qi Huang, Ting Shi, Yang Qin, Yaowei Jin, Lu Huang, Yaojie Sun, Chengmin Hu, Ziyang Song, Fengxian Xie
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引用次数: 0

Abstract

High-capacity small organic compounds are easily dissolved in aqueous electrolytes, resulting in limited cycling stability of Zn-organic batteries (ZOBs). To address this issue, we proposed constructing superstable lock-and-key hydrogen-bonding networks between the 2,7-dinitrophenanthraquinone (DNPQ) cathode and NH4+ charge carriers to achieve ultrastable ZOBs. DNPQ, with its sextuple-active carbonyl/nitro motifs (H-bonding acceptors), was found to be uniquely prone to redox-coupling with tetrahedral NH4+ ions (H-bonding donors) while excluding sluggish Zn2+ ions, owing to a lower activation energy (0.32 vs. 0.43 eV). NH4+-coordinated H-bonding electrochemistry overcame the instability of the DNPQ cathode in aqueous electrolytes and enabled rapid redox kinetics of non-metal NH4+ charge carriers. As a result, a three-step 3e- NH4+ coordination with the DNPQ cathode achieved large-current survivability (50 A g-1) and long-lasting cyclability (80 000 cycles) for ZOBs. This work broadens the potential for developing high-performance H-bonding-stabilized organics for advanced ZOBs.

水溶液锌电池中多电子氢键受体有机分子中NH4+的快速稳定存储。
高容量小有机化合物容易溶解于水溶液中,导致有机锌电池(ZOBs)的循环稳定性有限。为了解决这一问题,我们提出了在2,7-二硝基苯蒽醌(DNPQ)阴极和NH4+电荷载体之间构建超稳定的锁键氢键网络,以实现超稳定的ZOBs。DNPQ具有六活性羰基/硝基基基(h键受体),由于活化能较低(0.32 vs. 0.43 eV), DNPQ易于与四面体NH4+离子(h键供体)氧化还原偶联,而不含惰性Zn2+离子。NH4+配位氢键电化学克服了DNPQ阴极在水溶液中的不稳定性,实现了非金属NH4+电荷载体的快速氧化还原动力学。结果,3e- NH4+与DNPQ阴极的三步配位实现了zob的大电流生存能力(50 a g-1)和持久循环能力(80,000次循环)。这项工作拓宽了开发高性能氢键稳定有机化合物的潜力。
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来源期刊
Materials Horizons
Materials Horizons CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
18.90
自引率
2.30%
发文量
306
审稿时长
1.3 months
期刊介绍: Materials Horizons is a leading journal in materials science that focuses on publishing exceptionally high-quality and innovative research. The journal prioritizes original research that introduces new concepts or ways of thinking, rather than solely reporting technological advancements. However, groundbreaking articles featuring record-breaking material performance may also be published. To be considered for publication, the work must be of significant interest to our community-spanning readership. Starting from 2021, all articles published in Materials Horizons will be indexed in MEDLINE©. The journal publishes various types of articles, including Communications, Reviews, Opinion pieces, Focus articles, and Comments. It serves as a core journal for researchers from academia, government, and industry across all areas of materials research. Materials Horizons is a Transformative Journal and compliant with Plan S. It has an impact factor of 13.3 and is indexed in MEDLINE.
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