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
A Disquisition on the Active Sites of Heterogeneous Catalysts for Electrochemical Reduction of CO 2 to Value‐Added Chemicals and Fuel
Rahman Daiyan,Wibawa Hendra Saputera,Wibawa Hendra Saputera,Hassan Masood,Josh Leverett,Xunyu Lu,Rose Amal +6 more
Journal ArticleDOI
Low overpotential and high current CO2 reduction with surface reconstructed Cu foam electrodes
Shixiong Min,Xiulin Yang,Ang-Yu Lu,Chien-Chih Tseng,Mohamed N. Hedhili,Lain-Jong Li,Kuo-Wei Huang +6 more
TL;DR: In this article, the structural integration of Cu foam with open 3D frameworks and the favorable surface structures is a promising strategy to develop an advanced Cu electrocatalyst that can operate at high current density and low overpotential for CO 2 reduction.
Journal ArticleDOI
Black reduced porous SnO2 nanosheets for CO2 electroreduction with high formate selectivity and low overpotential
Guangbo Liu,Guangbo Liu,Zhonghua Li,Jianjian Shi,Jianjian Shi,Kun Sun,Yujin Ji,Zhiguo Wang,Yunfeng Qiu,Yuanyue Liu,Zhijiang Wang,PingAn Hu +11 more
TL;DR: In this paper, a black reduced porous SnO2 nanosheets electrocatalyst was developed that enabled possessing both metallic conductivity and high density of active sites via vacancy engineering, which showed high activity and selectivity for CO2 reduction reaction (CO2RR) electrocatalysts.
Journal ArticleDOI
Identifying Active Sites for CO2 Reduction on Dealloyed Gold Surfaces by Combining Machine Learning with Multiscale Simulations.
TL;DR: This work combines machine learning, multiscale simulations, and QM to predict the performance (a-value) of all 5000-10 000 surface sites on AuNPs and dealloyed Au surfaces and identifies the optimal active sites for CO2RR on de alloyed gold surfaces with dramatically reduced computational effort.
Journal ArticleDOI
Electrochemical CO Reduction: A Property of the Electrochemical Interface.
TL;DR: In this paper, the authors investigate how key CO reduction reaction intermediates are stabilized in different electrolytes and at different pH values, and find that the catalytic trends previously observed experimentally can be explained by the interplay between the metal surface and the electrolyte.
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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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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