Designing heterogeneous catalysts with dual-functional sites for hydrogenation reactions holds significant potential for improving activity and selectivity. We present catalysts that incorporate two distinct metal sites onto a MgO support, serving as adsorption sites for reactant and H₂, respectively. From screening 16 candidates using density functional theory calculations, we identified Pt₁Al₁/MgO as a promising catalyst for nitroaromatic hydrogenation. The Al–Mg moiety adsorbs 3-nitrostyrene via its nitro group, while the neighboring Pt–O facilitates H₂ dissociation through transient frustrated Lewis pairs. The synergistic effect of the Al–O–Pt moiety enhances reaction activity, driven by the appropriate adsorption/desorption of *H at the Pt site and a low diffusion barrier. This study offers valuable insights into the design of transient frustrated Lewis pair catalysts and is pivotal for the development of heterogeneous catalysts with dual-sites for hydrogenation reactions.

中文翻译：

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MgO（100） 支持的双金属位点协同作用促进加氢反应的理论见解


设计用于氢化反应的具有双功能位点的非均相催化剂在提高活性和选择性方面具有巨大潜力。我们提出了将两个不同的金属位点掺入 MgO 载体上的催化剂，分别用作反应物和 H₂ 的吸附位点。通过使用密度泛函理论计算筛选 16 个候选催化剂，我们确定了 Pt₁Al₁/MgO 是一种很有前途的硝基芳烃加氢催化剂。Al-Mg 部分通过其硝基吸附 3-硝基苯乙烯，而相邻的 Pt-O 通过瞬时受挫的 Lewis 对促进 H₂ 解离。Al-O-Pt 部分的协同效应增强了反应活性，这是由 *H 在 Pt 位点的适当吸附/解吸和低扩散势垒驱动的。这项研究为瞬态受挫 Lewis 对催化剂的设计提供了有价值的见解，对于开发具有双位点的氢化反应非均相催化剂至关重要。