Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review
Author(s)
Detail(s)
Original language | English |
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Pages (from-to) | 75-82 |
Journal / Publication | Nature Catalysis |
Volume | 3 |
Issue number | 1 |
Online published | 16 Dec 2019 |
Publication status | Published - Jan 2020 |
Externally published | Yes |
Link(s)
Abstract
Electrochemical conversion of CO2 into liquid fuels, powered by renewable electricity, offers one means to address the need for the storage of intermittent renewable energy. Here we present a cooperative catalyst design of molecule–metal catalyst interfaces with the goal of producing a reaction-intermediate-rich local environment, which improves the electrosynthesis of ethanol from CO2 and H2O. We implement the strategy by functionalizing the copper surface with a family of porphyrin-based metallic complexes that catalyse CO2 to CO. Using density functional theory calculations, and in situ Raman and operando X-ray absorption spectroscopies, we find that the high concentration of local CO facilitates carbon–carbon coupling and steers the reaction pathway towards ethanol. We report a CO2-to-ethanol Faradaic efficiency of 41% and a partial current density of 124 mA cm−2 at −0.82 V versus the reversible hydrogen electrode. We integrate the catalyst into a membrane electrode assembly-based system and achieve an overall energy efficiency of 13%.
Research Area(s)
Citation Format(s)
Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces. / Li, Fengwang; Li, Yuguang C.; Wang, Ziyun et al.
In: Nature Catalysis, Vol. 3, No. 1, 01.2020, p. 75-82.
In: Nature Catalysis, Vol. 3, No. 1, 01.2020, p. 75-82.
Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review