Journal
SMALL
Volume 18, Issue 51, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202204615
Keywords
3D N-doped vertical graphene; electrochemical CO; (2) reduction reaction; electronic structure; heterogeneous molecular catalysts
Categories
Funding
- National Natural Science Foundation of China [52002015, 22275010, 51872249]
- General Research Fund [CityU 11308120, CityU 11308321]
- Fundamental Research Funds for the Central Universities [buctrc202006]
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This study reports the development of an integrated molecular catalyst for CO2 reduction reaction by anchoring metal phthalocyanines on three-dimensional graphene arrays. The catalyst exhibits superior performance and stability, attributed to the efficient electron transfer channels and strong coupling effect between graphene and metal phthalocyanines.
Metallic phthalocyanines (MePcs) have shown their potential as catalysts for CO2 reduction reactions (CO2RR). However, their low conductivity, easy agglomeration, and poor stability enslave the further progress of their CO2RR applications. Herein, an integrated heterogeneous molecular catalyst through anchoring CoPc molecules on 3D nitrogen-doped vertical graphene arrays (NVG) on carbon cloth (CC) is reported. The CoPc-NVG/CC electrodes exhibit superior performance for reducing CO2 to CO with a Faradic efficiency of above 97.5% over a wide potential range (99% at an optimal potential), a very high turnover frequency of 35800 h(-1), and decent stability. It is revealed that NVG interacts with CoPc to form highly efficient channels for electron transfer from NVG to CoPc, facilitating the Co(II)/Co(I) redox of CO2 reduction. The strong coupling effect between NVG and CoPc molecules not only endows CoPc with high intrinsic activity for CO2RR, but also enhances the stability of electrocatalysts under high potentials. This work paves an efficient approach for developing high-performance heterogeneous catalysts by using rationally designed 3D integrated graphene arrays to host molecular metallic phthalocyanines so as to ameliorate their electronic structures and engineer stable active sites.
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