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
Selective Enhancement of Methane Formation in Electrochemical CO2 Reduction Enabled by a Raman-Inactive Oxygen-Containing Species on Cu
Mingquan He,Xiaoxia Chang,Tzu Hsuan Chao,Chunsong Li,William A. Goddard,Mu Jeng Cheng,Bingjun Xu,Qi Lu +7 more
TL;DR: The role of oxygen-containing species on Cu catalysts in the electrochemical CO2 reduction reaction (CO2RR) remains unclear due to the difficulty in its stabilization under reaction conditions as mentioned in this paper .
Journal ArticleDOI
Reductive and Coordinative Effects of Hydrazine in Structural Transformations of Copper Hydroxide Nanoparticles.
Xenia V. Medvedeva,Aleksandra A. Vidyakina,Feng Li,Andrey S. Mereshchenko,Andrey S. Mereshchenko,Anna Klinkova +5 more
TL;DR: It is shown that hydrazine, while being a common reducing agent in nanochemistry, can not only reduce the metal ions but also coordinate to them as a bidentate ligand and thereby integrate within the lattice of a particle.
Journal ArticleDOI
How computations accelerate electrocatalyst discovery
TL;DR: In this article , the authors introduce and discuss how computations accelerate electrocatalyst discovery from the aspects of providing insights and guidelines, from the typical examples, the advances of theoretical investigations aimed at identifying the active sites and understanding the reaction mechanisms and activity origin, and an overview of the design principles and screening strategies for superior electrocatalysts is highlighted.
Journal ArticleDOI
Progress and Understanding of CO2/CO Electroreduction in Flow Electrolyzers
Donghuan Wu,Feng Jiao,Qi Lu +2 more
TL;DR: In this article , the authors highlight how different flow cell designs impact CO2/CO electroreduction and outline potential strategies that may further improve the cell performance and discuss challenges and opportunities related to fundamental and engineering aspects.
References
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New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces
TL;DR: In this paper, the authors report new insights into the electrochemical reduction of CO2 on a metallic copper surface, enabled by the development of an experimental methodology with unprecedented sensitivity for the identification and quantification of CO 2 electroreduction products.
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TL;DR: This tutorial review will present much of the significant work that has been done in the field of electrocatalytic and homogeneous reduction of carbon dioxide over the past three decades and extend the discussion to the important conclusions from previous work and recommendations for future directions to develop a catalytic system that will convert carbon dioxide to liquid fuels with high efficiencies.
Journal ArticleDOI
Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2 Fixation
Aaron M. Appel,John E. Bercaw,Andrew Bruce Bocarsly,Holger Dobbek,Daniel L. DuBois,Michel Dupuis,James G. Ferry,Etsuko Fujita,Russ Hille,Paul J. A. Kenis,Cheryl A. Kerfeld,Cheryl A. Kerfeld,Robert H. Morris,Charles H. F. Peden,Archie R. Portis,Stephen W. Ragsdale,Thomas B. Rauchfuss,Joost N. H. Reek,Lance C. Seefeldt,Rudolf K. Thauer,Grover L. Waldrop +20 more
TL;DR: Providing a future energy supply that is secure and CO_2-neutral will require switching to nonfossil energy sources such as wind, solar, nuclear, and geothermal energy and developing methods for transforming the energy produced by these new sources into forms that can be stored, transported, and used upon demand.
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