Theoretical Studies on the Stability and Reactivity of the Metal-Doped CeO2(100) Surface: Toward H2 Dissociation and Oxygen Vacancy Formation.,Langmuir

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Theoretical Studies on the Stability and Reactivity of the Metal-Doped CeO2(100) Surface: Toward H2 Dissociation and Oxygen Vacancy Formation.
Langmuir ( IF 3.7 ) Pub Date : 2020-05-07 , DOI: 10.1021/acs.langmuir.0c00644
Wei Zhang ₁ , Min Pu ₁ , Ming Lei ₁

Affiliation

Surface doping is a common method to improve the performance of nanostructured materials. Different dopants will affect the structure and catalytic reactivity of the support. For a comprehensive understanding of the doping effects of metals doped into CeO₂, we conducted density functional theory (DFT) studies on the stabilities and geometry structures of transition-metal atoms (M = Fe, Co, Ni, Cu; Ru, Rh, Pd, Ag; Os, Ir, Pt, Au) doped into CeO₂(111), (110), and (100) surfaces. Moreover, the reactivity for H₂ dissociation and oxygen vacancy formation are systematically investigated on M-doped CeO₂(100) surfaces. The greater the binding energies of doped M atoms on the CeO₂ surface, the more difficult the formation of oxygen vacancies. The doped Co and Ir atoms do not directly participate in H₂ activation but serve as a promoter to make the H–H bond to break easily. The Cu, Ru, Pd, Ag, Pt, and Au atoms could act as the catalytically active center for H₂ dissociation and greatly reduce the activation energy barrier. Besides, it is easier to generate H₂O (W^M) and a surface oxygen vacancy from the intermediate H2^M/H4^M than from H3^M/H5^M, which is related to the acid–base interaction between H_Ce/M* and H_O* in H2^M/H4^M. This work could provide theoretical insights into the atomic structure characteristics of the transition-metal-doped CeO₂(100) surface and give ideas for the design of hydrogenation catalysts.

中文翻译：

掺杂金属的CeO2（100）表面的稳定性和反应性的理论研究：H2离解和氧空位的形成。

表面掺杂是提高纳米结构材料性能的常用方法。不同的掺杂剂将影响载体的结构和催化反应性。为了全面了解掺杂到CeO _2中的金属的掺杂效果，我们对过渡金属原子（M = Fe，Co，Ni，Cu，Ru，Rh，将Pd，Ag，Os，Ir，Pt，Au掺杂到CeO ₂（111），（110）和（100）表面中。此外，系统地研究了M掺杂的CeO ₂（100）表面上H ₂离解和氧空位形成的反应性。CeO ₂上掺杂的M原子的结合能越大表面上，氧空位的形成越困难。掺杂的Co和Ir原子不直接参与H ₂活化，但起促进剂的作用，使H–H键容易断裂。Cu，Ru，Pd，Ag，Pt和Au原子可以充当H ₂离解的催化活性中心，并大大降低活化能垒。此外，从中间H2 ^M / H4 ^M生成H ₂ O（W ^M）和表面氧空位比从H3 ^M / H5 ^M生成更容易，这与H _{Ce / M}之间的酸碱相互作用有关。和H_O *在H2 ^M / H4 ^M中。这项工作可以为过渡金属掺杂CeO ₂（100）表面的原子结构特征提供理论见解，并为氢化催化剂的设计提供思路。

更新日期：2020-05-07

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