Abstract The periodic four-layered model of the pure Cu(111) surface has been considered, and the effect of doping with palladium on CH4 dissociation has been investigated. The most stable adsorption geometries of CH x species (x = 1–4) and H atom on the PdCu(111) and pure Cu(111) surfaces have been obtained. Their computed adsorption energy results on the pure Cu(111) surface have been compared with the previously reported studies. Then, transition state geometries of CH4 dehydrogenation steps on both surfaces were calculated by the climbing image nudged elastic band method. Finally, the relative energy diagram for CH4 complete dehydrogenation has been represented. The results show that the PdCu(111) surface is more favorable than the Cu(111) surface in terms of the activation energies. The addition of Pd atoms to the Cu(111) surface significantly improves the catalytic activity. This knowledge can enable an efficient catalyst design at a lower cost using different strategies.

中文翻译：

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Pd/Cu(111) 表面合金上的 CH4 离解：DFT 研究

摘要 考虑了纯Cu(111)表面的周期性四层模型，研究了钯掺杂对CH4解离的影响。已经获得了 PdCu(111) 和纯 Cu(111) 表面上 CH x 物种 (x = 1-4) 和 H 原子最稳定的吸附几何结构。他们在纯 Cu(111) 表面上计算的吸附能结果已与先前报道的研究进行了比较。然后，通过爬升图像轻推松紧带方法计算两个表面上 CH4 脱氢步骤的过渡态几何形状。最后，表示了 CH4 完全脱氢的相对能量图。结果表明，就活化能而言，PdCu(111)表面比Cu(111)表面更有利。在 Cu(111) 表面添加 Pd 原子显着提高了催化活性。这些知识可以使用不同的策略以较低的成本实现有效的催化剂设计。