Construction of imide-linked covalent organic frameworks with palladium nanoparticles for oxygen reduction reaction

EcoEnergy Pub Date : 2024-03-27 DOI:10.1002/ece2.32
Zhuangyan Guo, Shuai Yang, Minghao Liu, Qing Xu, Gaofeng Zeng
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Abstract

Covalent organic frameworks (COFs) have been widely employed as electrocatalysts for oxygen reduction reaction (ORR) due to their diverse and tunable skeletons and pores. However, their electrocatalytic activity was limited due to the lack of highly active catalytic sites. In this work, we have first immobilized palladium nanoparticles (NPs) into the crystal, porous, and stable imide-linked COF for ORR. The newly designed COF had pyridine linkers with imide-linkages in the frameworks serving as the binding sites to anchor Pd sites, and the high surface area and open pore channels provide fast mass transport pathway to the active Pd sites, which contributed highly active performance in ORR. And the designed catalyst delivered onset potential and the half-wave potential of COF-Pd of 0.97 and 0.83 V, with a limited current density of 6.1 mA cm−2, respectively. This work provides us insights into developing high crystalline COFs with metal NPs in electrocatalytic systems.

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用钯纳米粒子构建亚胺链式共价有机框架,用于氧还原反应
共价有机框架(COFs)由于其骨架和孔隙的多样性和可调性,已被广泛用作氧还原反应(ORR)的电催化剂。然而,由于缺乏高活性催化位点,它们的电催化活性受到了限制。在这项工作中,我们首次将钯纳米颗粒(NPs)固定到晶体、多孔和稳定的亚胺连接的 COF 中,用于 ORR。新设计的 COF 框架中的吡啶连接物与亚胺连接物是锚定钯位点的结合位点,而高比表面积和开放的孔道为活性钯位点提供了快速的质量传输途径,从而在 ORR 中发挥了高活性性能。所设计的催化剂的起始电位和 COF-Pd 的半波电位分别为 0.97 V 和 0.83 V,有限电流密度为 6.1 mA cm-2。这项工作为我们在电催化系统中开发含有金属 NPs 的高结晶 COF 提供了启示。
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