Issue 13, 2022

Covalent organic frameworks based on tetraphenyl-p-phenylenediamine and metalloporphyrin for electrochemical conversion of CO2 to CO

Abstract

Electrocatalytic CO2 reduction provides a possible method for carbon neutralization. Electrode materials with efficient electron transfer, high selectivity and large current density are highly desirable. Herein, we have developed a couple of tetraphenyl-p-phenylenediamine and metalloporphyrin-based 2D COFs for the electrocatalytic CO2 reduction. TPPDA-MPor-COFs (M = Co and Ni) were obtained by the cross-condensation of tetraphenyl-p-phenylenediamine (TPPDA) and 5,10,15,20-tetrakis(4-formylphenyl)-metalloporphyrin (MPor). The as-prepared TPPDA-CoPor-COF shows high CO faradaic efficiencies of 87–90% from −0.6 to −0.9 V vs. RHE, and the largest CO partial current density (jCO) of TPPDA-CoPor-COF (−22.2 mA cm−2 at −1.0 V vs. RHE) exceeds those of most of the reported COF-based electrocatalysts. Notably, exfoliated TPPDA-CoPor-COF nanosheets (TPPDA-CoPor-COF-NSs) show much better electrocatalytic performance. The CO faradaic efficiencies of TPPDA-CoPor-COF-NSs are over 90% in a wider voltage range (−0.7 to −0.9 V), and the maximum jCO reaches up to −29.2 mA cm−2 at −1.0 V. Density functional theory calculations have been performed to rationalize the improved CO2RR performance of TPPDA-CoPor-COF.

Graphical abstract: Covalent organic frameworks based on tetraphenyl-p-phenylenediamine and metalloporphyrin for electrochemical conversion of CO2 to CO

Supplementary files

Article information

Article type
Research Article
Submitted
14 фев 2022
Accepted
04 май 2022
First published
25 май 2022

Inorg. Chem. Front., 2022,9, 3217-3223

Covalent organic frameworks based on tetraphenyl-p-phenylenediamine and metalloporphyrin for electrochemical conversion of CO2 to CO

L. Gong, B. Chen, Y. Gao, B. Yu, Y. Wang, B. Han, C. Lin, Y. Bian, D. Qi and J. Jiang, Inorg. Chem. Front., 2022, 9, 3217 DOI: 10.1039/D2QI00336H

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