Geometric and Electronic Engineering of Atomically Dispersed Copper-Cobalt Diatomic Sites for Synergistic Promotion of Bifunctional Oxygen Electrocatalysis in Zinc–Air Batteries,Advanced Materials

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Geometric and Electronic Engineering of Atomically Dispersed Copper-Cobalt Diatomic Sites for Synergistic Promotion of Bifunctional Oxygen Electrocatalysis in Zinc–Air Batteries
Advanced Materials ( IF 27.4 ) Pub Date : 2023-04-11 , DOI: 10.1002/adma.202300905
Zhijun Li ₁ , Siqi Ji ₁ , Chun Wang ₂ , Hongxue Liu ₁ , Leipeng Leng ₁ , Lei Du ₃ , Jincheng Gao ₁ , Man Qiao ₄ , J Hugh Horton _{1,

5} , Yu Wang ₂

Affiliation

The development of rechargeable zinc–air batteries is heavily dependent on bifunctional oxygen electrocatalysts to offer exceptional oxygen reduction/evolution reaction (ORR/OER) activities. However, the design of such electrocatalysts with high activity and durability is challenging. Herein, a strategy is proposed to create an electrocatalyst comprised of copper-cobalt diatomic sites on a highly porous nitrogen-doped carbon matrix (Cu-Co/NC) with abundantly accessible metal sites and optimal geometric and electronic structures. Experimental findings and theoretical calculations demonstrate that the synergistic effect of Cu-Co dual-metal sites with metal-N₄ coordination induce asymmetric charge distributions with moderate adsorption/desorption behavior with oxygen intermediates. This electrocatalyst exhibits extraordinary bifunctional oxygen electrocatalytic activities in alkaline media, with a half-wave potential of 0.92 V for ORR and a low overpotential of 335 mV at 10 mA cm⁻² for OER. In addition, it demonstrates exceptional ORR activity in acidic (0.85 V) and neutral (0.74 V) media. When applied to a zinc–air battery, it achieves extraordinary operational performance and outstanding durability (510 h), ranking it as one of the most efficient bifunctional electrocatalysts reported to date. This work demonstrates the importance of geometric and electronic engineering of isolated dual-metal sites for boosting bifunctional electrocatalytic activity in electrochemical energy devices.

中文翻译：

原子分散的铜钴双原子位点的几何和电子工程协同促进锌空气电池中双功能氧电催化

可充电锌空气电池的开发在很大程度上依赖于双功能氧电催化剂来提供卓越的氧还原/放出反应（ORR/OER）活性。然而，设计这种具有高活性和耐久性的电催化剂具有挑战性。在此，提出了一种策略，在高度多孔的氮掺杂碳基体（Cu-Co/NC）上创建由铜钴双原子位点组成的电催化剂，具有丰富的可接近金属位点和最佳的几何和电子结构。实验结果和理论计算表明Cu-Co双金属位点与金属-N _{4的协同效应}配位诱导不对称电荷分布，与氧中间体具有适度的吸附/解吸行为。^{这种电催化剂在碱性介质中表现出非凡的双功能氧电催化活性，ORR半波电位为0.92 V，10 mA cm -2}时的过电位为335 mV开放教育资源。此外，它在酸性 (0.85 V) 和中性 (0.74 V) 介质中表现出出色的 ORR 活性。当应用于锌空气电池时，它实现了非凡的运行性能和出色的耐用性（510小时），使其成为迄今为止报道的最高效的双功能电催化剂之一。这项工作证明了孤立双金属位点的几何和电子工程对于提高电化学能源装置中双功能电催化活性的重要性。

更新日期：2023-04-11

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