On the Real Nature of Rh Single‐Atom Catalysts Dispersed on the ZrO2 Surface,ChemCatChem

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On the Real Nature of Rh Single‐Atom Catalysts Dispersed on the ZrO2 Surface
ChemCatChem ( IF 3.8 ) Pub Date : 2020-03-23 , DOI: 10.1002/cctc.201901878
Ho Viet Thang ₁ , Gianfranco Pacchioni ₂

Affiliation

The nature of a Rh single‐atom catalyst (SAC) stabilized on the surface of tetragonal zirconia, t‐ZrO₂, is investigated here by performing extensive DFT calculations on various possible structural models and comparing the resulting spectral properties with existing data from the literature. The models considered include a Rh atom adsorbed on the clean surface, (Rh)_ads, Rh atoms stabilized by the reaction with surface OH groups to form direct Rh−O bonds, (RhO)_ads, and (RhO₂)_ads, the interaction of a Rh atom with an OH group, (RhOH)_ads, and a Rh atom replacing Zr in the lattice, (Rh)_subZr. Also a t‐ZrO₂ supported Rh₆ cluster has been considered for comparison with Rh single atoms. Surface heterogeneity has been taken into account by computing the various Rh species at terraces and at step sites of the zirconia surface. Based on the calculated adsorption energies, Rh 3d core level binding energies, and stretching frequencies of adsorbed CO and comparison with the experimental data we conclude that the potential candidates for Rh SAC on t‐ZrO₂ are (RhO)_ads and (RhOH)_ads species.

中文翻译：

关于分散在ZrO2表面上的Rh单原子催化剂的真实性质

通过在各种可能的结构模型上进行大量的DFT计算并将所得光谱特性与文献中的现有数据进行比较，在此研究了稳定在四方氧化锆表面上的Rh单原子催化剂（SAC）的性质，即t-ZrO ₂。。考虑的模型包括吸附在干净表面上的Rh原子，（Rh）_ads，通过与表面OH基团反应形成直接Rh-O键而稳定的Rh原子，（RhO）_ads和（RhO ₂）_ads，相互作用带有OH基团的Rh原子的（RhOH）_ads和在晶格中（Rh）_subZr取代Rh的Rh原子。在at-ZrO _2上也支持Rh ₆已经考虑将团簇与Rh单原子进行比较。通过计算氧化锆表面阶地和台阶部位的各种Rh物种，已经考虑到了表面异质性。根据计算得出的吸附能，Rh 3d核心能级结合能，吸附的CO的拉伸频率以及与实验数据的比较，我们得出结论，Rt SAC在t-ZrO ₂上的潜在候选物是（RhO）_ads和（RhOH）_ads种类。

更新日期：2020-03-23

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