Halogen-Bond Chemistry-Rectified Hypervalent Tellurium Redox Kinetics towards High-Energy Zn Batteries

IF 32.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Energy & Environmental Science Pub Date : 2024-12-03 DOI:10.1039/d4ee04806g

Jintu Qi, Yongchao Tang, Yue Wei, Guigui Liu, Jianping Yan, ZhenFeng Feng, Zixin Han, Minghui Ye, Wencheng Du, Qi Yang, Yufei Zhang, Zhipeng Wen, Xiaoqing Liu, Cheng Chao Li

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引用次数: 0

Abstract

Hypervalent Te redox (Te0/Te4+) in ionic liquid electrolytes (ILEs) is promising for energetic Zn batteries. However, the energy contribution of Te0/Te4+ is only one-third of the total redox-amphoteric conversion, which entails the contribution maximization for energy upgradation. The underlying kinetics-limited factor is vital but usually overlooked in previous explorations. Herein, we unlock a halogen-bond chemistry-rectified Te0/Te4+ redox with an almost maximized contribution for 700-Wh kgTe-1 Zn batteries. The Zn-X bond barriers in ZnX42- (X = Cl, Br) species from ILEs play crucial roles in rectifying the Te0/Te4+ redox kinetics, especially in localized concentrated ILEs, resulting in sharply different redox conversion depth. When the ZnBr42- with weak Zn-Br bond (34.96 kcal mol-1) as the activator, the Te0/Te4+ redox contribution can be maximized to ~90.0% over 5000 cycles at 5 A g-1, 1.8-fold higher than that with ZnCl42- activator via strong Zn-Cl bond (102.81 kcal mol-1), surpassing those in most aqueous systems (ca. 33.0%). This work decodes halogen-bond chemistry-rectified kinetics to maximize hypervalent redox contribution towards high-energy Zn batteries, which could apply to other chalcogen conversion batteries.

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来源期刊

Energy & Environmental Science 化学-工程：化工

CiteScore

50.50

自引率

2.20%

发文量

349

审稿时长

2.2 months

期刊介绍： Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).