Hydrogenation of nitroarenes to anilines under mild conditions is attractive from both theoretical and practical viewpoints. Here, high-performance catalyst with layered Pd nanoparticles epitaxially growing on ultrathin MoS nanosheets (Pd/MoS) were prepared. It shows surprisingly high catalytic activity, selectivity and stability for hydrogenation of various nitroarenes to corresponding anilines; the turnover frequency is one or two magnitudes higher than conventional Pd-based catalysts. Surface sulfur vacancies are formed on MoS nanosheets with low formation energy barrier. These S vacancies provide efficient positions for adsorbing Pd atoms, which enables facile cleavage of N–O bond as result of strong interfacial electron interaction that decreases activation energy by 0.41 eV in comparison with conventional Pd catalysts. In situ spectroscopy and DFT calculation results reveal a dual-site mechanism, in which surface Pd sites adsorb and dissociate H into active H*, and then readily reacts with nearby activated nitroarene to form aniline on interfacial Pd-MoS sites.

中文翻译：

---

在缺陷 MoS2 纳米片上外延生长 Pd 纳米片，用于增强硝基芳烃氢化为苯胺

从理论和实践的角度来看，在温和条件下硝基芳烃加氢生成苯胺都具有吸引力。在这里，制备了在超薄 MoS2 纳米片（Pd/MoS2）上外延生长的层状 Pd 纳米颗粒的高性能催化剂。它对各种硝基芳烃氢化成相应的苯胺表现出令人惊讶的高催化活性、选择性和稳定性；转换频率比传统的钯基催化剂高一两个数量级。 MoS2纳米片上形成表面硫空位，形成能垒低。这些S空位为吸附Pd原子提供了有效的位置，由于强界面电子相互作用，使得N-O键易于断裂，与传统的Pd催化剂相比，活化能降低了0.41 eV。原位光谱和DFT计算结果揭示了一种双位点机制，其中表面Pd位点吸附H并将H解离成活性H*，然后很容易与附近活化的硝基芳烃反应，在界面Pd-MoS位点上形成苯胺。