期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 126, 期 8, 页码 4008-4014出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c10846
关键词
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资金
- National Key Research and Development Program of China [2019YFA0210300]
- NSF of China [21922802, 22008036]
- Beijing Natural Science Foundation [JQ19007]
- Talent Cultivation of State Key Laboratory of Organic-Inorganic Composites, Double-First-Class Construction Projects [XK180301, XK1804-02]
- Distinguished Scientist Program at BUCT [buctylkxj02]
The rational regulation of the oxygen reduction catalytic activity of transition metal/nitrogen-doped carbon is important for sustainable energy conversion devices. In this study, a series of covalent organic frameworks with dithiine bridges were designed and the effect of dithiine on oxygen reduction was studied. The results showed that the introduction of dithiine can improve the catalytic activity by modifying the electronic structure of the metal atoms.
The rational regulation of oxygen reduction catalytic activity of transition metal/nitrogen-doped carbon (M-N-C) is of great significance for sustainable energy conversion devices. Here, we designed a series of dithiine bridged phthalocyanine-based covalent organic frameworks (denoted as COFDTI) and studied the effect of the introduction of dithiine on the performance of oxygen reduction by density functional theory. The results demonstrate that the dithiine in covalent framework lowers the d-band center in metal atoms toward a more negative level relative to the Fermi level and weakens their adsorption strength with oxygen-containing intermediates owing to the electron-withdrawing effect of dithiine compared with counterparts without S atoms in the skeleton, i.e., COFBTC, which causes the catalytic activities of COFDTI-Fe to shift from the left branch of volcano plot to the apex and exceed that of Pt (111). This work not only seeks a promising candidate for oxygen reduction reaction but also provides a new view for designing efficient and stable cathode materials by directly introducing electron-withdrawing functionality in the M-N-C electrocatalysts.
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