重构无定形多金属硫化物实现长寿命快充锌空气电池,Advanced Materials

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重构无定形多金属硫化物实现长寿命快充锌空气电池
Advanced Materials ( IF 27.4 ) Pub Date : 2022-09-30 , DOI: 10.1002/adma.202204247
Ansheng Wang ₁ , Xilin Zhang ₂ , Shan Gao ₁ , Chunning Zhao ₁ , Siyu Kuang ₃ , Shanshan Lu ₃ , Juntao Niu ₄ , Geng Wang ₅ , Weifang Li ₅ , Da Chen ₆ , Haijun Zhang ₆ , Xiaomeng Zhou ₆ , Sheng Zhang ₃ , Bin Zhang ₃ , Weichao Wang ₁

Affiliation

开发快速充电锌空气电池对于扩大其应用至关重要，但由于缓慢的析氧反应 (OER) 动力学和电催化剂活性位点不足的限制，仍然具有挑战性。为了解决这个问题，开发了一种具有高密度有效活性位点的重构非晶 FeCoNiS _x电催化剂，在 10、100 和 500 mA cm -2 下分别产生 202、255 和 323 mV 的低 OER 过电势，用于快速^{-以 100–400 mA cm}⁻²的低充电电压为锌空气电池充电。此外，制造的 3241.8 mAh（20 mA cm ^-2 , 25 °C）准固态锌空气电池在 -10 和 25 °C 下显示出 500 小时的长寿命，在 100 mA 充电下在 40 °C 下显示 150 小时厘米^-2。详细表征结合密度泛函理论计算表明，通过重构非晶多金属硫化物形成富含缺陷的结晶/非晶三元金属（氧）氢氧化物，其中多活性位点之间的电子耦合效应和中间体 O 的迁移* 从 Ni 位点到 Fe 位点打破了比例关系，导致 170 mV 的低理论 OER 过电势，这是出色的快速充电性能的原因。这项工作不仅为通过预催化剂的自重构设计先进的 OER 催化剂提供了见解，而且还为实用的快速充电锌空气电池开辟了一条途径。

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Fast-Charging Zn–Air Batteries with Long Lifetime Enabled by Reconstructed Amorphous Multi-Metallic Sulfide

Developing fast-charging Zn–air batteries is crucial for widening their application but remains challenging owing to the limitation of sluggish oxygen evolution reaction (OER) kinetics and insufficient active sites of electrocatalysts. To solve this issue, a reconstructed amorphous FeCoNiS_x electrocatalyst with high density of efficient active sites, yielding low OER overpotentials of 202, 255, and 323 mV at 10, 100, and 500 mA cm⁻², respectively, is developed for fast-charging Zn–air batteries with low charging voltages at 100–400 mA cm⁻². Furthermore, the fabricated 3241.8 mAh (20 mA cm⁻², 25 °C) quasi-solid Zn–air battery shows long lifetime of 500 h at −10 and 25 °C as well as 150 h at 40 °C under charging 100 mA cm⁻². The detailed characterizations combine with density functional theory calculations indicate that the defect-rich crystalline/amorphous ternary metal (oxy)hydroxide forms by the reconstruction of amorphous multi-metallic sulfide, where the electron coupling effect among multi-active sites and migration of intermediate O* from Ni site to the Fe site breaks the scaling relationship to lead to a low theoretical OER overpotential of 170 mV, accounting for the outstanding fast-charging property. This work not only provides insights into designing advanced OER catalysts by the self-reconstruction of the pre-catalyst but also pioneers a pathway for practical fast-charging Zn–air batteries.

更新日期：2022-09-30

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