Catalytic activity of 1D chains of gold oxide on a stepped gold surface from density functional theory,Physical Chemistry Chemical Physics

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Catalytic activity of 1D chains of gold oxide on a stepped gold surface from density functional theory
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-11-15 , DOI: 10.1039/d2cp03524c
Shikun Li ₁ , Okikiola Olaniyan ₂ , Lenard L Carroll ₂ , Marcus Bäumer ₁ , Lyudmila V Moskaleva ₂

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The rich surface chemistry of gold at the nanoscale has made it an important catalyst for low-temperature applications. Recent studies point to the possible role of self-organized structures formed by chemisorbed O atoms on the surface of gold catalysts for their catalytic activity and/or deactivation. In this study, we investigate the reactivity of a double O chain running along a step on a Au(221) surface with oxygen vacancies as a prototypical model of a 1D surface gold oxide. We compare CO and O₂ adsorption on such a chain with the oxygen-free Au(221) surface model. A systematic study of the reactivity of the double chain with O vacancies was done with respect to the regular Au(221) surface using CO as a probe. The CO oxidation was investigated assuming dissociative and associative mechanisms. Remarkably, O₂ adsorbs stronger on the double oxygen vacancy than on the regular Au(221) surface, and its dissociation barrier reduces significantly from 1.84 eV to 0.87 eV, whereas the CO adsorption energy is similar on these surfaces. Calculations suggest that CO oxidation should occur more efficiently on the double O vacancy than on the regular Au(221) surface due to stronger adsorption of O₂ and a low activation barrier for O₂ + CO surface reaction.

中文翻译：

密度泛函理论对阶梯金表面一维金氧化物链的催化活性

纳米级金的丰富表面化学使其成为低温应用的重要催化剂。最近的研究指出了金催化剂表面化学吸附的 O 原子形成的自组织结构对其催化活性和/或失活的可能作用。在这项研究中，我们研究了在具有氧空位的 Au(221) 表面上沿着台阶运行的双 O 链的反应性，作为一维表面氧化金的原型模型。我们比较 CO 和 O ₂用无氧 Au(221) 表面模型吸附在这样的链上。使用 CO 作为探针，对规则 Au(221) 表面的双链与 O 空位的反应性进行了系统研究。假设解离和缔合机制研究了 CO 氧化。值得注意的是，O ₂在双氧空位上的吸附比在常规 Au(221) 表面上的吸附更强，其解离势垒从 1.84 eV 显着降低至 0.87 eV，而这些表面上的 CO 吸附能相似。_{计算表明，由于 O 2更强的吸附和 O}₂ + CO 表面反应的低活化势垒，CO 氧化在双 O 空位上比在常规 Au(221) 表面上更有效。

更新日期：2022-11-15

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