Imparting CO2 Electroreduction Auxiliary for Integrated Morphology Tuning and Performance Boosting in a Porphyrin-based Covalent Organic Framework

Strategies that enable simultaneous morphology-tuning and electroreduction performance boosting are much desired for the exploration of covalent organic frameworks in efficient CO2 electroreduction. Herein, a kind of functionalizing exfoliation agent has been selected to simultaneously modify and exfoliate bulk COFs into functional nanosheas and investigate their CO2 electroreduction performance. The obtained nanosheets (Cu-Tph-COF-Dct) with large-scale (approximate to 1.0 mu m) and ultrathin (approximate to 3.8 nm) morphology enable a superior FECH4 (approximate to 80 %) (almost doubly enhanced than bare COF) with large current-density (-220.0 nzA cm(-2)) at -0.9 V. The boosted performance can be ascribed to the immobilized funakmalizing exfoliation agent (Dct groups) with integrated amino and triazine groups that strengthen CO2 absorption/activation, stabilize intermediates and enrich the CO concentration around the Cu active sites as revealed by AFT calculations. The point-to-point functionalization strategy for modularly assembling Dct-functioruzlized COF catalyst for CO2 electroreduction will open up the attractive possibility of developing COFs as efficient CO2RR electrocatalysts.

Automated summary

This study has successfully prepared COF nanosheets with superior performance using a functionalizing exfoliation agent, providing a new possibility for the development of efficient CO2 electroreduction catalysts.