Theoretical Insight into the Trends that Guide the Electrochemical Reduction of Carbon Dioxide to Formic Acid

Wiley - Tập 9 Số 4 - Trang 358-363 - 2016
Jong Suk Yoo1,2, Rune Christensen3, Tejs Vegge3, Jens K. Nørskov1,2, Felix Studt1,2
1Department of Chemical Engineering, Stanford University, Stanford, CA 94305 USA
2SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA
3Department of Energy Conversion and Storage, Technical University of Denmark, Fysikvej Bldg. 309, 2800 Kgs. Lyngby, Denmark

Tóm tắt

AbstractThe electrochemical reduction (electroreduction) of CO2 to formic acid (HCOOH) and its competing reactions, that is, the electroreduction of CO2 to CO and the hydrogen evolution reaction (HER), on twenty‐seven different metal surfaces have been investigated using density functional theory (DFT) calculations. Owing to a strong linear correlation between the free energies of COOH* and H*, it seems highly unlikely that the electroreduction of CO2 to HCOOH via the COOH* intermediate occurs without a large fraction of the current going to HER. On the other hand, the selective electroreduction of CO2 to HCOOH seems plausible if the reaction occurs via the HCOO* intermediate, as there is little correlation between the free energies of HCOO* and H*. Lead and silver surfaces are found to be the most promising monometallic catalysts showing high faradaic efficiencies for the electroreduction of CO2 to HCOOH with small overpotentials. Our methodology is widely applicable, not only to metal surfaces, but also to other classes of materials enabling the computational search for electrocatalysts for CO2 reduction to HCOOH.

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Wiley

Tập 9 Số 4

358-363

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