For the construction of catalysts for the electrocatalytic carbon dioxide reduction reaction (CO2RR), the class of templates known as covalent organic frameworks (COFs), which feature functionalization with high precision and ordered pores, is regarded as the ideal choice.
Ionic skeletons can facilitate charge transfer, which further enhances conductivity, and C-N bonds have the potential to enhance CO2 adsorption. However, the electrostatic repulsion and weak linkage of direct bottom-up synthesis make it difficult to achieve the coexistence of C-N bonds and ionic frameworks.
a group of researchers led by Prof. Zeng Gaofeng and colleagues A multilevel post-synthetic modification strategy has been proposed by Prof. Xu Qing of the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences to construct high-activity and selectivity catalytic COFs for CO2RR.
Nature Communications published the findings.
The maximum turnover frequency of the post-modified catalytic COFs was 9922.68 h-1 at -1.0 V, and the faradaic efficiency was 97.32% at -0.8 V, both of which were higher than those of the base COF and the single-modified COFs.
Tests and characterizations using electrocatalysis showed that the ionic skeleton and C-N bonds could increase activity and catalytic selectivity.
Moreover, hypothetical estimations outlined that the simpler development of quick CO from COOH was the rate-decided step, and methyl bunches fortified electron thickness.
The role of COFs in the CO2 reduction reaction is clarified by this research. It reveals insight into building staggered post-manufactured alteration COFs towards customized movement and high steadiness.
More information: Minghao Liu et al, Post-synthetic modification of covalent organic frameworks for CO2 electroreduction, Nature Communications (2023). DOI: 10.1038/s41467-023-39544-9
