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Researchers propose post-synthetic modification of covalent organic frameworks for carbon dioxide electroreduction

July 6, 2023
in Science
Researchers propose post-synthetic modification of covalent organic frameworks for carbon dioxide electroreduction
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Researchers propose post-synthetic modification of covalent organic frameworks for carbon dioxide electroreduction

Schematic illustration of multilevel post-synthetic modification. a Effects of reduction reaction, Menshutkin reaction and multilevel post-synthetic modification on the bond change and charge state. b The synthesis of N+-COF, NH-COF and N+-NH-COF from the base COF (CoTAPP-PATA-COF). Credit: Nature Communications (2023). DOI: 10.1038/s41467-023-39544-9

Covalent organic frameworks (COFs), possessing ordered pores and high-precision functionalization, are regarded as an ideal class of templates to construct catalysts for electrocatalytic carbon dioxide reduction reaction (CO2RR).

C-N bonds can improve adsorption of CO2 and ionic skeletons can promote charge transfer, further enhancing conductivity. However, direct bottom-up synthesis can hardly realize co-existence of C-N bonds and ionic frameworks due to the electrostatic repulsion and weak strength of the linkage.

A research team led by Prof. Zeng Gaofeng and Assoc. Prof. Xu Qing from the Shanghai Advanced Research Institute (SARI) of the Chinese Academy of Sciences has proposed a multilevel post-synthetic modification strategy to construct catalytic COFs towards CO2RR with high activity and selectivity.

The results were published in Nature Communications.

Catalytic COFs synthesized by the post modification showed a maximum turnover frequency value of 9922.68 h–1 at –1.0 V and the highest faradaic efficiency of 97.32% at –0.8 V, which were higher than that of the base COF and the single-modified COFs.

Electrocatalysis tests and characterizations revealed that C-N bonds could improve catalytic selectivity and ionic skeleton contributed to higher activity.

Furthermore, theoretical calculations illustrated that the easier formation of immediate *CO from COOH* was the rate-determined step, and methyl groups strengthened electron density.

This work provides a deeper understanding of COFs in CO2 reduction reaction. It sheds light on constructing multilevel post-synthetic modification COFs towards tailored activity and high stability.

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

Citation:
Researchers propose post-synthetic modification of covalent organic frameworks for carbon dioxide electroreduction (2023, July 6)
retrieved 6 July 2023
from https://phys.org/news/2023-07-post-synthetic-modification-covalent-frameworks-carbon.html

This document is subject to copyright. Apart from any fair dealing for the purpose of private study or research, no
part may be reproduced without the written permission. The content is provided for information purposes only.

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Copyright for syndicated content belongs to the linked Source : Phys.org – https://phys.org/news/2023-07-post-synthetic-modification-covalent-frameworks-carbon.html

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