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Curvature-Engineered Single-Atom Catalysts for Selective Electroreduction of Acetylene to Ethylene: A Systematic Computational Screening
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DOI：10.1021/acs.jpcc.6c01826.png)
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Abstract
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Electrochemical semihydrogenation of acetylene to ethylene is a promising petrochemical process, but catalysts often face issues like overhydrogenation to ethane and insufficient stability. The structural curvature effect of catalysts can effectively tune the electronic structure of active sites, thus suppressing excessive hydrogenation and improving the reaction stability. Herein, we perform a comprehensive computational study to screen high-performance single-atom catalysts (SACs) for electrocatalytic acetylene hydrogenation, constructing a total of 84 SAC models consisting of 14 kinds of metals (Ag, Au, Cu, Co, Fe, Ir, Mn, Ni, Pd, Pt, Ru, Rh, Sn, and Zn) anchored on nitrogen-doped carbon supports with tunable curvatures (graphene, C30, C40, C50, C60, and C70 fullerenes). Results reveal that the curvature of carbon supports modulates the metal–support interaction, tunes the electronic structure of single-atom active sites, and further governs the adsorption strength of reaction intermediates. Notably, Cu-based catalysts have been recognized as the best metal-carrier combination, which exhibits excellent ethylene selectivity and catalytic activity. This is attributed to its moderate stability, activity, and selectivity, which can weaken ethylene adsorption and inhibit excessive hydrogenation. This work establishes a clear structure–activity relationship between support curvature and catalytic performance, providing a theoretical guideline for the rational design of high-efficiency SACs for acetylene-selective hydrogenation.
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