Tunable activity of electrocatalytic CO dimerization on strained Cu surfaces: Insights from ab initio molecular dynamics simulations

doi:10.1016/S1872-2067(21)64044-5

Abstract

Abstract:

Controlling catalytic activities through surface strain engineering remains a hot topic in electrocatalysis studies. Herein, ab initio molecular dynamics (AIMD) simulation associated with free energy sampling technology were performed to study the energetics of the key step of producing C₂ products in electrocatalytic reduction of CO or CO₂, i.e. CO dimerization, on strained Cu(100) with an explicit aqueous solvent model. It is worth mentioning that when compressive strain reaches a certain extent, the surface of Cu(100) will undergo reconstruction. We showed that, from tensile to compressive strain, the free energy barrier of CO dimerization decreased, suggesting that the activity of CO dimerization increases. It was also found that some of the reconstructed surfaces showing the lowest free energy barriers but might be less stable can be stabilized in the presence of adsorbed O or CO. Upon detailed quantitative analysis on the charges of surface Cu atoms, we found that the free energy barriers were strongly correlated with the charge of Cu atoms where the OCCO intermediate adsorbs. When the surfaces structures of Cu(100) were altered under compressive strain, the electronic structure of surface Cu atoms was monitored and thus the activity of electrocatalytic CO dimerization can be tuned.

Key words: Electrocatalytic CO dimerization, Surface strain, Cu, Surface reconstruction, Ab initio molecular dynamics

Hong Liu, Jian Liu, Bo Yang. Tunable activity of electrocatalytic CO dimerization on strained Cu surfaces: Insights from ab initio molecular dynamics simulations[J]. Chinese Journal of Catalysis, 2022, 43(11): 2898-2905.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64044-5

https://www.cjcatal.com/EN/Y2022/V43/I11/2898

Figures/Tables 7

Fig. 1. Snapshots of the modeling system, which illustrate the CO* dimerization process from the C?C distance of 4.0 to 1.5 Å. Color code: orange, Cu; gray, C; red, O; and white, H.

Fig. 2. The two types of reconstructed Cu(100) surfaces (a,b) and the unreconstructed surface (c). (d) The formation energy of reconstructed surfaces with respect to the energy of the unreconstructed surface at different strains applied.

Fig. 3. (a) Two typical free energy profiles obtained for CO dimerization over the surfaces with maximum compressive strain (δ = +5%) and tensile strain (δ = -4% (100)r-a), with the C-C distance from 4.0 to 1.4 Å. The shaded portion of the line shows the uncertainty of each value. (b) The free energy barriers (Ga) with error bars plotted as a function of strain applied. IS, TS and FS indicate the initial state, transition state and final state of the reaction, respectively.

Fig. 4. The C trajectories of the two CO in the last 2000 steps in the final state (FS), transition state (TS) and initial state (IS) under different strains applied. For intuitional presentation, water, oxygen atom of CO and bulk Cu atom are removed from the Fig., and the green and magenta balls exhibit trajectories of the two C atoms.

Fig. 5. The formation energy for reconstructed surfaces when (a) O or (b) CO are adsorbed at different strain conditions with respect to the energy of corresponding O/CO adsorbed unreconstructed surfaces. The lower value of formation energy indicates that the structure is more stable, and a negative value suggests that the reconstructed surface is more stable.

Fig. 6. Difference charge density plots showing the charge transfer from surface Cu atoms to the adsorbed OCCO moiety. Here the yellow and cyan contour represent charge accumulation and depletion, respectively. The iso-surface level was set to 0.01 e/Å3.

Fig. 7. (a) Net charge of the four Cu atoms at which the OCCO adsorbs in Fig. 4 as a function of strain. (b) Free energy barrier with error bars of CO dimerization as a function of the net charge under different strains applied.

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