Reconstructing the Coordination Environment of Fe/Co Dual-atom Sites towards Efficient Oxygen Electrocatalysis for Zn–Air Batteries

IF 19.3 1区材料科学 Q1 CHEMISTRY, PHYSICAL

ACS Energy Letters Pub Date : 2024-11-14 DOI:10.1002/anie.202419595

Hengqi Liu, Jinzhen Huang, Kun Feng, Rui Xiong, Shengyu Ma, Ran Wang, Qiang Fu, Moniba Rafique, Zhiguo Liu, Jiecai Han, Daxing Hua, Jiajie Li, Jun Zhong, Xianjie Wang, Zhonglong Zhao, Tai Yao, Sida Jiang, Ping Xu, Zhihua Zhang, Bo Song

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引用次数: 0

Abstract

Dual-atom catalysts with nitrogen-coordinated metal sites embedded in carbon can drive the oxygen reduction and evolution reactions (ORR/OER) in rechargeable zinc–air batteries (ZABs), and the further improvement is limited by the linear scaling relationship of intermediate binding energies in the absorbate evolution mechanism (AEM). Triggering the lattice oxygen mechanism (LOM) is promising to overcome this challenge, but has yet been verified since the lacking of bridge oxygen (O) in the rigid coordination environment of the metal centers. Here, we demonstrate that suitably tailored dual-atom catalysts of FeCo–N–C can undergo out-plane and in-plane reconstruction to form the both axial O and bridge O at the metal centers, and thus activate the LOM pathway. The tailored FeCo–N–C with shortened Fe–N bonds also favor the ORR process, therefore is a promising dual-atom oxygen catalyst. The assembled rechargeable ZABs demonstrate a peak power density of 332 mW cm−2, and exhibit no notable decline after ~ 720 h of continuous cycling.

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重构铁/钴双原子位的配位环境，实现锌-空气电池的高效氧电催化

嵌入碳中氮配位金属位点的双原子催化剂可以驱动可充电锌-空气电池（ZAB）中的氧还原和进化反应（ORR/OER），但由于吸收剂进化机制（AEM）中中间结合能的线性比例关系，进一步的改进受到了限制。触发晶格氧机制（LOM）有望克服这一挑战，但由于在金属中心的刚性配位环境中缺乏桥氧（O），这一机制尚未得到验证。在此，我们证明了经过适当定制的 FeCo-N-C 双原子催化剂可以进行平面外和平面内重构，在金属中心形成轴向 O 和桥式 O，从而激活 LOM 途径。定制的 FeCo-N-C 具有缩短的 Fe-N 键，也有利于 ORR 过程，因此是一种很有前途的双原子氧催化剂。组装好的可充电 ZAB 显示出 332 mW cm-2 的峰值功率密度，并且在连续循环约 720 小时后没有出现明显下降。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment

CiteScore

31.20

自引率

5.00%

发文量

469

审稿时长

1 months

期刊介绍： ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.