Exclusive Co-N4 Sites Confined in Two-dimensional Metal-Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial-Level Current
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review
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Detail(s)
Original language | English |
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Article number | e202219241 |
Journal / Publication | Angewandte Chemie - International Edition |
Volume | 62 |
Issue number | 23 |
Online published | 5 Apr 2023 |
Publication status | Published - 5 Jun 2023 |
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Abstract
Metal-organic framework catalysts bring new opportunities for CO2 electrocatalysis. Herein, we first conduct density-functional theory calculations and predict that Co-based porphyrin porous organic layers (Co-PPOLs) exhibit good activity for CO2 conversion because of the low *CO adsorption energy at Co-N4 sites, which facilitates *CO desorption and CO formation. Then, we prepare two-dimensional Co-PPOLs with exclusive Co-N4 sites through a facile surfactant-assisted bottom-up method. The ultrathin feature ensures the exposure of catalytic centers. Together with large specific area, high electrical conductivity and CO2 adsorption capability, Co-PPOLs achieve a peak faradaic efficiency for CO production (FECO=94.2 %) at a moderate potential in CO2 electroreduction, accompanied with good stability. Moreover, Co-PPOLs reach an industrial-level current above 200 mA in a membrane electrode assembly reactor, and maintain near-unity CO selectivity (FECO>90 %) over 20 h in CO2 electrolysis. © 2023 Wiley-VCH GmbH.
Research Area(s)
- Bottom-up Method, Co-N4 Sites, CO2 Reduction, MEA Device, Porphyrin Porous Organic Layers
Citation Format(s)
Exclusive Co-N4 Sites Confined in Two-dimensional Metal-Organic Layers Enabling Highly Selective CO2 Electroreduction at Industrial-Level Current. / Zhang, Wenjun; Liu, Shanshan; Yang, Yue et al.
In: Angewandte Chemie - International Edition, Vol. 62, No. 23, e202219241, 05.06.2023.
In: Angewandte Chemie - International Edition, Vol. 62, No. 23, e202219241, 05.06.2023.
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review