期刊
SMALL
卷 17, 期 22, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202004933
关键词
CO2 electrocatalysis; cobalt; covalent organic frameworks; donor– acceptor; porphyrin
类别
资金
- National Key Research and Development Program of China [2018YFA0208600, 2018YFA0704502]
- NSFC [21871263, 21671188, 21520102001]
- Key Research Program of Frontier Science, CAS [QYZDJ-SSW-SLH045]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- Youth Innovation Promotion Association, CAS [Y201850]
The TT-Por(Co)-COF, containing donor-acceptor heterojunctions, exhibits enhanced performance in electrocatalytic reduction of carbon dioxide to produce CO, thanks to its improved charge transfer capability and large amount of accessible active sites. This study demonstrates that integrating donor-acceptor heterojunctions in COFs can facilitate electron transfer and generate high current densities for CO2RR.
Covalent organic frameworks (COFs) are promising candidates for electrocatalytic reduction of carbon dioxide into valuable chemicals due to their porous crystalline structures and tunable single active sites, but the low conductivity leads to unmet current densities for commercial application. The challenge is to create conductive COFs for highly efficient electrocatalysis of carbon dioxide reduction reaction (CO2RR). Herein, a porphyrin-based COF containing donor-acceptor (D-A) heterojunctions, termed TT-Por(Co)-COF, is constructed from thieno[3,2-b]thiophene-2,5-dicarbaldehyde (TT) and 5,10,15,20-tetrakis(4-aminophenyl)-porphinatocobalt (Co-TAPP) via imine condensation reaction. Compared with COF-366-Co without TT, TT-Por(Co)-COF displays enhanced CO2RR performance to produce CO due to its favorable charge transfer capability from the electron donor TT moieties to the acceptor Co-porphyrin ring active center. The combination of strong charge transfer properties and enormous amount of accessible active sites in the 2D TT-Por(Co)-COF nanosheets results in good catalytic performance with a high Faradaic efficiency of CO (91.4%, -0.6 V vs reversible hydrogen electrode (RHE) and larger partial current density of 7.28 mA cm(-2) at -0.7 V versus RHE in aqueous solution. The results demonstrate that integration of D-A heterojunctions in COF can facilitate the intramolecular electron transfer, and generate high current densities for CO2RR.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据