用于耐用可充电锌空气电池的 Co-CoN4 混合活性位点的稳健电子相关性,Advanced Functional Materials

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用于耐用可充电锌空气电池的 Co-CoN4 混合活性位点的稳健电子相关性
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-10-10 , DOI: 10.1002/adfm.202207331
Kuixing Ding ₁ , Jiugang Hu ₁ , Jia Luo ₁ , Liming Zhao ₂ , Wei Jin ₃ , Yunpeng Liu ₄ , Zhonghua Wu ₄ , Guoqiang Zou ₁ , Hongshuai Hou ₁ , Xiaobo Ji ₁

Affiliation

合理设计对析氧反应 (OER) 和氧还原反应 (ORR) 具有优异活性和稳定性的双功能催化剂对于可充电锌空气电池 (ZAB) 至关重要。在这项研究中，提出了一种简便的协调桥接策略来构建嵌入多孔富氮碳纳米片（表示为 Co- CoN _{4 @NCNs）中的双功能 Co-CoN}₄杂化活性位点，用于 ORR 和 OER。同步加速器 X 射线吸收光谱和密度泛函理论计算表明，增加的固有 ORR/OER 活性可归因于原子 Co 之间的有效界面电荷转移N 位点和金属 Co 位点由于它们强大的电子相关性。原位拉曼光谱证实 OER 活性取决于反应过程中形成的 CoOOH 中间体。Co- CoN ₄ @NCNs对在碱性介质中进行的 ORR（ E _1/2 = 0.83 V）和 OER（η = 310 mV，10 mA cm ^{-2 ）表现出优异的双功能催化性能。}组装的可充电Co- CoN ₄ @NCNs-based ZAB显示开路电压为1.47 V，峰值功率密度为118.8 mW cm ^-2，比容量为776.7 mAh g ^-1，以及超过 1500 次循环的出色循环稳定性。界面电子特性的调节有助于合理设计用于可充电金属-空气电池的双功能电催化剂。

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Robust Electronic Correlation of Co-CoN4 Hybrid Active Sites for Durable Rechargeable Zn-Air Batteries

The rational design of bifunctional catalysts with excellent activity and stability toward the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is essential for rechargeable Zn-air batteries (ZABs). In this study, a facile coordination bridging strategy is proposed to construct bifunctional Co-CoN₄ hybrid active sites embedded in porous N-rich carbon nanolamellas (denoted as Co-CoN₄@NCNs) for both the ORR and OER. Synchrotron X-ray absorption spectroscopy and density functional theory calculations reveal that the increased intrinsic ORR/OER activities can be attributed to the efficient interfacial charge transfer between the atomic CoN sites and metallic Co sites due to their robust electronic correlation. In situ Raman spectroscopy confirms that the OER activity depends on the CoOOH intermediates formed during the reaction. Co-CoN₄@NCNs exhibits superior bifunctional catalytic performance for the ORR (E_1/2 = 0.83 V) and OER (η = 310 mV at 10 mA cm⁻²) conducted in alkaline media. The assembled rechargeable Co-CoN₄@NCNs-based ZAB displays an open-circuit voltage of 1.47 V, peak power density of 118.8 mW cm⁻², specific capacity of 776.7 mAh g⁻¹, and outstanding cycling stability over 1500 cycles. The regulation of the interfacial electronic properties can contribute to the rational design of bifunctional electrocatalysts used in rechargeable metal-air batteries.

更新日期：2022-10-10

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