卟啉
共价有机骨架
电催化剂
共价键
催化作用
电化学
金属有机骨架
热解
材料科学
反应性(心理学)
化学
纳米技术
化学工程
光化学
物理化学
有机化学
吸附
电极
病理
工程类
替代医学
医学
作者
Subhajit Bhunia,Armando Peña,Huifang Li,Hong Li,Mohamed Fathi Sanad,Pranay Saha,Matthew A. Addicoat,Kotaro Sasaki,T. Amanda Strom,Miguel Yacaman,Carlos R. Cabrera,Ram Seshadri,Santanu Bhattacharya,Jean‐Luc Brédas,Luís Echegoyen
出处
期刊:ACS Nano
[American Chemical Society]
日期:2023-02-08
卷期号:17 (4): 3492-3505
被引量:20
标识
DOI:10.1021/acsnano.2c09838
摘要
Designing N-coordinated porous single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) is a promising approach to achieve enhanced energy conversion due to maximized atom utilization and higher activity. Here, we report two Co(II)-porphyrin/ [2,1,3]-benzothiadiazole (BTD)-based covalent organic frameworks (COFs; Co@rhm-PorBTD and Co@sql-PorBTD), which are efficient SAC systems for O2 electrocatalysis (ORR). Experimental results demonstrate that these two COFs outperform the mass activity (at 0.85 V) of commercial Pt/C (20%) by 5.8 times (Co@rhm-PorBTD) and 1.3 times (Co@sql-PorBTD), respectively. The specific activities of Co@rhm-PorBTD and Co@sql-PorBTD were found to be 10 times and 2.5 times larger than that of Pt/C, respectively. These COFs also exhibit larger power density and recycling stability in Zn–air batteries compared with a Pt/C-based air cathode. A theoretical analysis demonstrates that the combination of Co-porphyrin with two different BTD ligands affords two crystalline porous electrocatalysts having different d-band center positions, which leads to reactivity differences toward alkaline ORR. The strategy, design, and electrochemical performance of these two COFs offer a pyrolysis-free bottom-up approach that avoids the creation of random atomic sites, significant metal aggregation, or unpredictable structural features.
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