Journal ArticleDOI
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper
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The results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice, demonstrating the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.Abstract:
The electrochemical conversion of CO and H2O into liquid fuel is made feasible at modest potentials with the use of oxide-derived nanocystalline Cu as the catalyst. Renewable electricity is often produced when it is not needed. If the surplus could be harnessed to drive the conversion of CO2 and water into liquid fuel, the energy would not go to waste and a use would be found for CO2 produced by carbon capture. All this requires efficient electrocatalysts that reduce CO2 not only to CO, but also further into fuel chemicals. Copper does this but with low efficiency and selectivity. Christina Li et al. now show that the intrinsic catalytic properties of copper can be improved by producing it from its oxide as interconnected nanocrystallites. Their enhanced catalyst generates primarily ethanol, demonstrating that a two-step conversion of CO2 to liquid fuel powered by renewable electricity might be possible. The electrochemical conversion of CO2 and H2O into liquid fuel is ideal for high-density renewable energy storage and could provide an incentive for CO2 capture. However, efficient electrocatalysts for reducing CO2 and its derivatives into a desirable fuel1,2,3 are not available at present. Although many catalysts4,5,6,7,8,9,10,11 can reduce CO2 to carbon monoxide (CO), liquid fuel synthesis requires that CO is reduced further, using H2O as a H+ source. Copper (Cu) is the only known material with an appreciable CO electroreduction activity, but in bulk form its efficiency and selectivity for liquid fuel are far too low for practical use. In particular, H2O reduction to H2 outcompetes CO reduction on Cu electrodes unless extreme overpotentials are applied, at which point gaseous hydrocarbons are the major CO reduction products12,13. Here we show that nanocrystalline Cu prepared from Cu2O (‘oxide-derived Cu’) produces multi-carbon oxygenates (ethanol, acetate and n-propanol) with up to 57% Faraday efficiency at modest potentials (–0.25 volts to –0.5 volts versus the reversible hydrogen electrode) in CO-saturated alkaline H2O. By comparison, when prepared by traditional vapour condensation, Cu nanoparticles with an average crystallite size similar to that of oxide-derived copper produce nearly exclusive H2 (96% Faraday efficiency) under identical conditions. Our results demonstrate the ability to change the intrinsic catalytic properties of Cu for this notoriously difficult reaction by growing interconnected nanocrystallites from the constrained environment of an oxide lattice. The selectivity for oxygenates, with ethanol as the major product, demonstrates the feasibility of a two-step conversion of CO2 to liquid fuel that could be powered by renewable electricity.read more
Citations
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Journal ArticleDOI
Electrooxidation of saturated C1-C3 primary alcohols on platinum: Potential-resolved product analysis with electrochemical real-time mass spectrometry (EC-RTMS)
Peyman Khanipour,Peyman Khanipour,Sandra Haschke,Julien Bachmann,Karl Johann Jakob Mayrhofer,Karl Johann Jakob Mayrhofer,Ioannis Katsounaros +6 more
TL;DR: In this paper, the authors provide details on the interpretation of data for electrochemical real-time mass spectrometry (EC-RTMS) and on the assignment of mass signals to reaction products by studying three model reactions.
Journal ArticleDOI
CO 2 Valorization Reactions over Cu-Based Catalysts: Characterization and the Nature of Active Sites
TL;DR: In this paper, the structure and nature of active sites of different types of Cu-based catalysts for CO2 valorization in thermo-, photo-, and electro-catalysis are discussed.
Journal ArticleDOI
Accelerated Prediction of Cu-based Single-Atom Alloy Catalysts for CO2 Reduction by Machine Learning
Dashuai Wang,Runfeng Cao,Shaogang Hao,Chen Liang,Guangyong Chen,Pengfei Chen,Yang Li,Xiaolong Zou +7 more
TL;DR: In this article, the authors combine first-principles calculations and machine learning techniques to elucidate critical factors influencing the catalytic properties, taking Cu-based single atom alloys (SAAs) as examples.
Journal ArticleDOI
The influence of oxygen on the surface interaction between CO2 and copper studied by ambient pressure X-ray photoelectron spectroscopy
Anna Regoutz,Gwilherm Kerherve,Ignacio J. Villar-Garcia,Charlotte K. Williams,David J. Payne +4 more
TL;DR: The surface chemistry at the interface between solid Cu and the CO2 containing gas phase lies at the heart of the complex pathways involved in the catalytic interaction, and the precise mechanisms and the oxidation states of Cu involved remain controversial.
Journal ArticleDOI
Reaction mechanism on Ni-C2-NS single-atom catalysis for the efficient CO2 reduction reaction
TL;DR: Ni-based single-atom catalysis (Ni-SAC) has been experimentally reported with superior performance in reducing CO2 to CO. However, due to the ambiguities in its structures, the active sites of Ni-S...
References
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