Integration of Strong Electron Transporter Tetrathiafulvalene into Metalloporphyrin-Based Covalent Organic Framework for Highly Efficient Electroreduction of CO2,ACS Energy Letters

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Integration of Strong Electron Transporter Tetrathiafulvalene into Metalloporphyrin-Based Covalent Organic Framework for Highly Efficient Electroreduction of CO2
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-03-05 , DOI: 10.1021/acsenergylett.9b02756
Qiao Wu _{1,

2} , Rui-Kuan Xie _{1,

3} , Min-Jie Mao ₁ , Guo-Liang Chai _{1,

3} , Jun-Dong Yi ₁ , Shao-Shuai Zhao ₁ , Yuan-Biao Huang _{1,

3} , Rong Cao _{1,

2,

3}

Affiliation

Electroreduction of CO₂ (CO₂RR) into value-added fuels is of significant importance but remains a big challenge because of poor selectivity, low current density, and large overpotential. Crystalline porous covalent organic frameworks (COFs) are promising alternative electrode materials for CO₂RR owing to their tunable and accessible single active sites. However, the poor electron-transfer capability of COFs limits their application. Herein, a tetrathiafulvalene (TTF) strut was integrated into a two-dimensional cobalt porphyrin-based COF (TTF-Por(Co)-COF) to enhance its electron-transfer capability from the TTF to the porphyrin ring. Compared with COF-366-Co without TTF, TTF-Por(Co)-COF showed enhanced CO₂RR performance in water with 95% Faradaic efficiency of the CO₂-to-CO conversion at −0.7 V vs RHE and a partial current density of 6.88 mA cm^–2 at −0.9 V vs RHE. This work provides a new insight for the rational design of porous organic framework materials for improving the activity of CO₂RR.

中文翻译：

将强电子转运体四硫富瓦烯整合到金属卟啉基共价有机骨架中，以高效电还原CO ₂

将CO ₂（CO ₂ RR）电还原为增值燃料非常重要，但由于选择性差，电流密度低和超电势大，仍然是一个很大的挑战。结晶多孔共价有机骨架（COF）由于具有可调节和可访问的单个活性位点，因此有望成为CO ₂ RR的替代电极材料。但是，COFs较差的电子转移能力限制了它们的应用。在此，将四硫富瓦烯（TTF）支杆集成到二维基于卟啉钴的COF（TTF-Por（Co）-COF）中，以增强其从TTF到卟啉环的电子转移能力。与没有TTF的COF-366-Co相比，TTF-Por（Co）-COF的CO ₂增强水中的RR性能为-0.7 V vs RHE时，CO ₂到CO转化的法拉第效率为95％，而-0.9 V vs RHE时，部分电流密度为6.88 mA cm ^–2。这项工作为合理设计多孔有机骨架材料以提高CO ₂ RR的活性提供了新的见识。

更新日期：2020-03-05

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