Modeling the effect of surface CO coverage on the electrocatalytic reduction of CO2 to CO on Pd surfaces

Literature Information

Publication Date 2019-04-08
DOI 10.1039/C8CP07427E
Impact Factor 3.676
Authors

Jian Liu, Bo Yang


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Abstract

Electrocatalytic reduction of CO2 has attracted considerable attention recently, and it was found experimentally that Pd could show activity for the electroreduction of CO2 to CO. However, theoretical studies showed that the adsorption of CO on Pd surfaces is strong and the coverage of CO is high, indicating that the interactions between the neighboring adsorbed CO and other reaction intermediates on the Pd surfaces cannot be neglected. Here, with density functional theory calculations and utilizing the Sabatier analysis method, we find that an adsorbate–adsorbate interaction is playing a crucial role in the modeling of the electrocatalytic reduction of CO2 to CO on Pd surfaces, whilst the reaction rates obtained by neglecting the interactions between the surface adsorbates are substantially lower than those reported in the experiments. Upon analyzing the interactions quantitatively and using a self-consistent iterative microkinetic modeling method, we find that the active site for CO2 electroreduction is Pd(111) at different potentials applied. Our modeling results provide a reasonable computational interpretation for the electroreduction of CO2 to CO on Pd.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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