Theoretical study of structure sensitivity on ceria‐supported single platinum atoms and its influence on carbon monoxide adsorption,Journal of Computational Chemistry

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Theoretical study of structure sensitivity on ceria‐supported single platinum atoms and its influence on carbon monoxide adsorption
Journal of Computational Chemistry ( IF 3.4 ) Pub Date : 2024-05-25 , DOI: 10.1002/jcc.27393
Antoine Salichon ₁ , Agustin Salcedo ₁ , Carine Michel ₁ , David Loffreda ₁

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Density functional theory (DFT) calculations explore the stability of a single platinum atom on various flat, stepped, and defective ceria surfaces, in the context of single‐atom catalysts (SACs) for the water–gas shift (WGS) reaction. The adsorption properties and diffusion kinetics of the metal strongly depend on the support termination with large stability on metastable and stepped CeO2(100) and (210) surfaces where the diffusion of the platinum atom is hindered. At the opposite, the more stable CeO2(111) and (110) terminations weakly bind the platinum atom and can promote the growth of metallic clusters thanks to fast diffusion kinetics. The adsorption of carbon monoxide on the single platinum atom supported on the various ceria terminations is also sensitive to the surface structure. Carbon monoxide weakly binds to the single platinum atom supported on reduced CeO2(111) and (211) terminations. The desorption of the CO2 formed during the WGS reaction is thus facilitated on the latter terminations. A vibrational analysis underlines the significant changes in the calculated scaled anharmonic CO stretching frequency on these catalysts.

中文翻译：

二氧化铈负载单铂原子结构敏感性及其对一氧化碳吸附影响的理论研究

密度泛函理论 (DFT) 计算探讨了在水煤气变换 (WGS) 反应的单原子催化剂 (SAC) 的背景下，单个铂原子在各种平坦、阶梯和有缺陷的氧化铈表面上的稳定性。金属的吸附性能和扩散动力学强烈依赖于亚稳态和阶梯状 CeO 上具有高稳定性的支撑终止2 (100)和(210)表面，铂原子的扩散受到阻碍。相反，CeO 更稳定2 (111) 和 (110) 末端与铂原子的结合较弱，并且由于快速扩散动力学可以促进金属簇的生长。一氧化碳在各种二氧化铈末端负载的单个铂原子上的吸附也对表面结构敏感。一氧化碳与还原 CeO 上负载的单个铂原子微弱结合2 (111)和(211)终止。 CO的解吸2因此，在 WGS 反应过程中形成的酶在后者的终止过程中得到促进。振动分析强调了这些催化剂上计算的缩放非简谐 CO 伸缩频率的显着变化。

更新日期：2024-05-25

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