Efficient oxygen reduction through metal-free 3D covalent organic frameworks: a novel approach

IF 6.8 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Science China Materials Pub Date : 2024-08-23 DOI:10.1007/s40843-024-3039-8

Shanyue Wei (, ), Xiaowei Wu (, ), Shufei Zhu (, ), Zhiyang Wang (, ), Jiangli Wang (, ), Can-Zhong Lu (, ), Yiming Xie (, )

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引用次数: 0

Abstract

Covalent organic framework (COF) materials have gained significant applications in electrocatalytic systems due to their structural diversity and tunable functionalities. Moreover, three-dimensional (3D) COFs exhibit multistage pore structures, exposing numerous open sites, which facilitate the oxygen reduction reaction (ORR) process. However, the advancement of 3D COFs for ORR has been hindered by challenges, including limited topologies, the scarcity of building blocks with the required reactivity and symmetries, and difficulties in determining crystalline structures. In this work, we utilized an 8-connectivity building unit and successfully constructed two isoreticular 3D COF materials, which exhibited exceptionally high catalytic activity for 2e⁻ oxygen reduction reaction without the addition of any metal or conductive support materials, nor the pyrolyzed process. The electrochemically active surface areas (ECSAs) of the two 3D COFs were found to be 17.19 and 12.18 mF/cm², respectively, which were significantly higher than those reported from other framework materials.

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通过无金属三维共价有机框架实现高效氧还原：一种新方法

共价有机框架（COF）材料因其结构的多样性和可调整的功能性，在电催化系统中获得了重要的应用。此外，三维（3D）COF 显示出多级孔隙结构，暴露出大量开放位点，促进了氧还原反应（ORR）过程。然而，用于 ORR 的三维 COF 的发展一直受到各种挑战的阻碍，包括拓扑结构有限、具有所需反应活性和对称性的构建模块稀缺，以及晶体结构难以确定等。在这项工作中，我们利用 8 连接构建单元，成功构建了两种等轴三维 COF 材料，它们在 2e 氧还原反应中表现出极高的催化活性，无需添加任何金属或导电支撑材料，也无需热解过程。两种三维 COF 的电化学活性表面积（ECSA）分别为 17.19 和 12.18 mF/cm2，明显高于其他框架材料。

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来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.