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Effect of Halide Anions on the Electroreduction of CO 2  to C 2 H 4 : A Density Functional Theory Study

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The halide anions present in the electrolyte improves the Faradaic efficiencies (FEs) of the multi-hydrocarbon (C 2+ ) products for the electrochemical reduction of CO 2  over copper (Cu) catalysts. However, the mechanism behinds the increased yield of C 2+  products with the addition of halide anions still remains indistinct. In this study, we analysed the mechanism by investigating the electronic structures and computing the relative free energies of intermediates formed from CO 2  to C 2 H 4  on the Cu (100) facet based on density functional theory (DFT) calculations. The results show that formyl *CHO species from the hydrogenation reaction of the adsorbed *CO acts as the key intermediate, and the C-C coupling reaction occurs preferentially between the *CHO and *CO with the formation of a *CHO-CO intermediate. Subsequently, the free-energy pathway of C 2 H 4  formation has been proposed, and we found that the presence of halide anions significantly decreases the free energy of the *CHOCH intermediate, and enhances desorption of C 2 H 4  in the order of I -  > Cl -  > Br -  > F - . Lastly, the obtained results are rationalized by the Bader charge analysis.

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