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Dithiine Bridged Phthalocyanine-Based Covalent Organic Frameworks for Highly Efficient Oxygen Reduction Reaction
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-02-16 , DOI: 10.1021/acs.jpcc.1c10846
Xueli Li 1 , Yujia Liu 2 , Zhonghua Xiang 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2022-02-16 , DOI: 10.1021/acs.jpcc.1c10846
Xueli Li 1 , Yujia Liu 2 , Zhonghua Xiang 1
Affiliation
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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.
中文翻译：
用于高效氧还原反应的二硫因桥接酞菁基共价有机骨架
过渡金属/氮掺杂碳（M-N-C）的氧还原催化活性的合理调控对于可持续能源转换装置具有重要意义。在这里，我们设计了一系列基于二硫胺桥联酞菁的共价有机骨架（记为COF DTI），并通过密度泛函理论研究了二硫胺的引入对氧还原性能的影响。结果表明，与对应物相比，由于二硫因的吸电子作用，共价骨架中的二硫因将金属原子中的 d 带中心降低到相对于费米能级更负的水平，并削弱了它们与含氧中间体的吸附强度。骨架中没有S原子，即COF BTC，这导致COF DTI -Fe的催化活性从火山图的左支转移到顶点，并超过了Pt（111）的催化活性。这项工作不仅为氧还原反应寻找有希望的候选者，而且通过在 M-N-C 电催化剂中直接引入吸电子功能，为设计高效稳定的正极材料提供了新的视角。
更新日期：2022-02-16
中文翻译：
用于高效氧还原反应的二硫因桥接酞菁基共价有机骨架
过渡金属/氮掺杂碳（M-N-C）的氧还原催化活性的合理调控对于可持续能源转换装置具有重要意义。在这里，我们设计了一系列基于二硫胺桥联酞菁的共价有机骨架（记为COF DTI），并通过密度泛函理论研究了二硫胺的引入对氧还原性能的影响。结果表明，与对应物相比，由于二硫因的吸电子作用，共价骨架中的二硫因将金属原子中的 d 带中心降低到相对于费米能级更负的水平，并削弱了它们与含氧中间体的吸附强度。骨架中没有S原子，即COF BTC，这导致COF DTI -Fe的催化活性从火山图的左支转移到顶点，并超过了Pt（111）的催化活性。这项工作不仅为氧还原反应寻找有希望的候选者，而且通过在 M-N-C 电催化剂中直接引入吸电子功能，为设计高效稳定的正极材料提供了新的视角。
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