Covalent organic frameworks based on tetraphenyl-p-phenylenediamine and metalloporphyrin for electrochemical conversion of CO2 to CO. Issue 13 (25th May 2022)

• Record Type: Journal Article
• Authors: Gong, Lei; Chen, Baotong; Gao, Ying; Yu, Baoqiu; Wang, Yinhai; Han, Bin; Lin, Chenxiang; Bian, Yongzhong; Qi, Dongdong; Jiang, Jianzhuang
• Is Part Of: Inorganic chemistry frontiers. Volume 9:Issue 13(2022)
• Page Start: 3217
• Page End: 3223
• Publication Date: 2022-05-25
• Subjects: Chemistry, Inorganic -- Periodicals; 546.05
• DOI: 10.1039/d2qi00336h
• Languages: English
• ISSNs: 2052-1553

Abstract

Abstract : The as-prepared TPPDA-CoPor-COF shows high CO faradic efficiencies of 87–90% from −0.6 to −0.9 V vs. RHE, and the largest CO partial current density of TPPDA-CoPor-COF exceeds most of reported COF-based electrocatalysts. 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 ( j CO ) 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 j CO reaches up to −29.2 mA cm −2 at −1.0 V. Density functional theory calculations have been performed to rationalize the improved CO2 RR performance of TPPDA-CoPor-COF.