Reversing Zincophobic/Hydrophilic Nature of Metal-N-C via Metal-Coordination Interaction for Dendrite-Free Zn Anode with High Depth-of-Discharge,Advanced Materials

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Reversing Zincophobic/Hydrophilic Nature of Metal-N-C via Metal-Coordination Interaction for Dendrite-Free Zn Anode with High Depth-of-Discharge
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-08 , DOI: 10.1002/adma.202311637
Ziyi Yang ₁ , Fayuan Lai ₁ , Qianjiang Mao ₁ , Chong Liu ₁ , Ruoyu Wang ₁ , Zhihua Lu ₁ , Tianran Zhang _{1,

2} , Xiangfeng Liu ₁

Affiliation

Dendrite-free Zn metal anodes with high depth-of-discharge (DoD) and robust cycle performances are highly desired for the practical application of aqueous Zn-ion batteries. Herein, the zincophobic/hydrophilic nature of Metal-N-C through manipulating the electronic interactions between metal and coordination atoms is successfully reversed, thereby fabricating a zincophilic/hydrophobic asymmetric Zn-N_3Py+1Pr-C (consisting of a Zn center coordinated with 3 pyridinic N atoms and 1 pyrrolic N atom) host, which realizes uniformed Zn deposition and a long lifespan with high DoD. The experimental and theoretical investigations demonstrate weakened interaction between pyrrolic N and metal center in the asymmetric Zn-N_3Py+1Pr-C triggers downshift of the Zn 3d-band-center and a new localization nonbonding state in the N and C 2p-band, resulting in preferred Zn adsorption to water adsorption. Consequently, the asymmetric Zn-N_3Py+1Pr-C host delivers small Zn nucleation overpotential and high Coulombic efficiency of 98.3% over 500 cycles. The symmetric cells with Zn-N_3Py+1Pr-C@Zn anode demonstrate 500 h dendrite-free cycles at DoD up to 50%. The Zn-N_3Py+1Pr-C@Zn/S-PANI full cell also shows a robust long-term cycle performance of 1000 cycles at 10 A g⁻¹. This strategy of constructing zincophilic/hydrophobic Metal-N-C may open up their application for the dendrite-free metal anode.

中文翻译：

通过金属配位相互作用逆转金属NC的疏锌/亲水性质，用于高放电深度的无枝晶锌阳极

水系锌离子电池的实际应用非常需要具有高放电深度（DoD）和强大循环性能的无枝晶锌金属负极。在此，通过操纵金属和配位原子之间的电子相互作用，成功逆转了Metal-NC的疏锌/亲水性质，从而制备了亲锌/疏水的不对称Zn-N _3Py+1Pr -C（由与3个吡啶配位的Zn中心组成） N原子和1个吡咯N原子）主体，实现了均匀的Zn沉积和高DoD的长寿命。实验和理论研究表明，不对称 Zn-N _3Py+1Pr -C 中吡咯 N 与金属中心之间的相互作用减弱，触发了 Zn 3d 能带中心的下移以及 N 和 C 2p 能带中新的局域化非键合态，导致锌的吸附优于水的吸附。因此，不对称 Zn-N _3Py+1Pr -C 主体在 500 次循环中具有较小的 Zn 成核过电势和 98.3% 的高库仑效率。具有 Zn-N _3Py+1Pr -C@Zn 阳极的对称电池在 DoD 下表现出高达 50% 的 500 小时无枝晶循环。 Zn-N _3Py+1Pr -C@Zn/S-PANI全电池还表现出在10 A g ^-1下循环1000次的强大长期循环性能。这种构建亲锌/疏水金属-NC的策略可能会开拓它们在无枝晶金属阳极的应用。

更新日期：2024-01-08

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