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
How to go beyond C1 products with electrochemical reduction of CO2
Da Li,Da Li,Hao Zhang,Hang Xiang,Shahid Rasul,Jean-Marie Fontmorin,Jean-Marie Fontmorin,Paniz Izadi,Paniz Izadi,Alberto Roldan,Rebecca S.F. Taylor,Yujie Feng,Liam Banerji,Alexander J. Cowan,Eileen Hao Yu,Eileen Hao Yu,Eileen Hao Yu,Jin Xuan +17 more
TL;DR: In this paper, a review summarises recent development across electro-, photo-electro-and bio-catalyst developments in CO2 electrochemical reduction and explores the role of device design and operating conditions in enabling C-C bond generation.
Journal ArticleDOI
Electrochemistry: Catalysis at the boundaries.
TL;DR: 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, demonstrating that a two-step conversion of CO2 to liquid fuel powered by renewable electricity might be possible.
Journal ArticleDOI
pH-Dependent Reactivity of a Water-Soluble Nickel Complex: Hydrogen Evolution vs Selective Electrochemical Hydride Generation
TL;DR: In this paper, aqueous hydrogen evolution reaction (HER) electrocatalyst [Ni(DHMPE)2]2+ was investigated using 31P{1H} NMR spectroscopy.
Journal ArticleDOI
Evaluation of the Electrochemically Active Surface Area of Microelectrodes by Capacitive and Faradaic Currents
Alina N. Sekretaryova,Alina N. Sekretaryova,Mikhail Vagin,Anton V. Volkov,Igor Zozoulenko,Mats Eriksson +5 more
TL;DR: In this paper, two methods to estimate the electrochemically active surface area (EASA) of microelectrodes were compared, one based on electrocapacitive measurements and the other based on faradaic measuements.
Journal ArticleDOI
Requirements for Beneficial Electrochemical Restructuring: A Model Study on a Cobalt Oxide in Selected Electrolytes
Javier Villalobos,Diego González-Flores,Roberto Urcuyo,Mavis L. Montero,Götz Schuck,Paul Beyer,Marcel Risch +6 more
TL;DR: In this article, Erythrite (Co3(AsO4)2 8H2O) was used as a Co-based OER electrocatalyst to evaluate its catalytic properties during in-situ restructuring into an amorphous Cobased catalyst in four different electrolytes at pH 7.
References
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Journal ArticleDOI
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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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
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