<br>通过构建基于双（2-氨基乙基）胺的内亥姆霍兹平面来维持质子和氢氧根离子的浓度平衡，以实现长寿命的锌金属阳极,Chemical Engineering Journal

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通过构建基于双（2-氨基乙基）胺的内亥姆霍兹平面来维持质子和氢氧根离子的浓度平衡，以实现长寿命的锌金属阳极
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-01-04 , DOI: 10.1016/j.cej.2023.148511
Zhijian Wang , Zuyang Hu , Minghui Ye , Jiachi Chen , Yifa Chen , Zhipeng Wen , Yufei Zhang , Yongchao Tang , Xiaoqing Liu , Cheng Chao Li

尽管具有高安全性和低成本的优点，但由于析氢反应（HER）和不可逆Zn4SO4(OH)6·的形成，锌金属负极的循环寿命短，阻碍了可充电水系金属锌电池的发展。 nH2O 是由吸附在 Zn 金属阳极内亥姆霍兹平面 (IHP) 上的 H2O 分子分解引起的。为了解决这个问题，我们使用双（2-氨基乙基）胺（B2AA）有机分子作为添加剂，通过重构IHP并维持质子和氢氧根离子的浓度平衡来抑制Zn腐蚀和HER，从而实现长期且高度的腐蚀。可逆锌金属电池。密度泛函理论计算和分子动力学模拟表明，由于高吸附能，B2AA优先吸附在Zn阳极界面上，通过排斥约19%的H2O分子形成缺水的IHP。此外，B2AA的-NH2/-NH-基团可以可逆地捕获H2O分解产生的H+并动态中和OH-，从而抑制腐蚀反应。使用包含 B2AA 的水性电解质，对称 Zn//Zn 电池在 10 mA cm−2 下表现出 2400 小时的长循环寿命。与NH4V4O10（NVO）正极匹配，Zn//NVO全电池在10 A/g电流下具有147.24 mAh/g的高初始容量，并在3000次循环后保持66%的高容量保持率。

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Maintaining the concentration equilibrium of proton and hydroxide ions by construction of bis(2-aminoethyl)amine-based inner helmholtz plane toward long-life zinc metal anodes

Despite the merits of high safety and low cost, the development of rechargeable aqueous Zn metal batteries is oppressed by the short cycling life of Zn metal anodes, due to the hydrogen evolution reaction (HER) and the formation of irreversible Zn4SO4(OH)6·nH2O that are caused by the decomposition of H2O molecules adsorbed in the inner Helmholtz plane (IHP) of Zn metal anodes. To solve this issue, we herein use bis(2-aminoethyl)amine (B2AA) organic molecules as additives to suppress Zn corrosion and HER via reconstructing the IHP and maintaining the concentration equilibrium of protons and hydroxide ions, thus achieving long-term and highly reversible Zn metal batteries. Density functional theory calculations and molecule dynamics simulations reveal that B2AA are preferentially adsorbed on the interface of Zn anode owing to the high adsorption energy, forming a water-deficient IHP via repelling ≈19% of H2O molecules. Additionally, the −NH2/−NH− groups of B2AA can reversibly capture H+ derived from the decomposition of H2O and dynamically neutralize OH−, thus suppressing the corrosion reaction. Using an aqueous electrolyte involving B2AA, symmetric Zn//Zn cells exhibit a long cycling life of 2400 h at 10 mA cm−2. Matched with a NH4V4O10 (NVO) cathode, the Zn//NVO full cell delivers a high initial capacity of 147.24 mAh/g at 10 A/g, and maintains a high capacity retention of 66% after 3000 cycles.

更新日期：2024-01-04

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