期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 1, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202114244
关键词
covalent organic frameworks; CO2 reduction; electrocatalysis; phthalocyanine; three-dimensional COFs
资金
- Natural Science Foundation of China [21631003, 21805005]
- Fundamental Research Funds for the Central Universities [FRF-BD-20-14A]
- University of Science and Technology Beijing
Functional 3D COFs with irreversible bond were synthesized successfully, showing a large current density and high Faradaic efficiency, significantly improved compared to excellent 2D COF analogues.
Synthesis of functional 3D COFs with irreversible bond is challenging. Herein, 3D imide-bonded COFs were constructed via the imidization reaction between phthalocyanine-based tetraanhydride and 1,3,5,7-tetra(4-aminophenyl)adamantine. These two 3D COFs are made up of interpenetrated pts networks according to powder X-ray diffraction and gas adsorption analyses. CoPc-PI-COF-3 doped with carbon black has been employed to fabricate the electrocatalytic cathode towards CO2 reduction reaction within KHCO3 aqueous solution, displaying the Faradaic efficiency of 88-96 % for the CO2-to-CO conversion at the voltage range of ca. -0.60 to -1.00 V (vs. RHE). In particular, the 3D porous structure of CoPc-PI-COF-3 enables the active electrocatalytic centers occupying 32.7 % of total cobalt-phthalocyanine subunits, thus giving a large current density (j(CO)) of -31.7 mA cm(-2) at -0.90 V. These two parameters are significantly improved than the excellent 2D COF analogue (CoPc-PI-COF-1, 5.1 % and -21.2 mA cm(-2)).
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