Xie Deqiong, Xue Ruifang, Dou Kecan, Song Yaping, Fu Yanghe, Zhang Fumin, Chen De-Li, Zhu Weidong
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua, 321004, People's Republic of China.
Chemistry. 2024 Dec 10;30(69):e202402757. doi: 10.1002/chem.202402757. Epub 2024 Oct 26.
The direct hydrogenation of 2-nitroacylbenzene to 2,1-benzisoxazole presents a significant challenge in the pharmaceutical and fine chemicals industries. In this study, a defect engineering strategy is employed to create bifunctional single-atom catalysts (SACs) by anchoring Pt single atoms onto metal vacancies within MgO(Al) nanosheets. The resultant Pt/MgO(Al) SAC displays an exceptional catalytic activity and selectivity in the hydrogenation-cyclization of 2-nitroacylbenzene, achieving a 97.5 % yield at complete conversion and a record-breaking turnover frequency of 458.8 h under the mild conditions. The synergistic catalysis between the fully exposed single-atom Pt sites within a unique Pt-O-Mg/Al moiety and the abundant basic sites of the MgO(Al) support is responsible for this outstanding catalytic performance. The current work, therefore, paves the way for developing bifunctional or multifunctional SACs that can enhance efficient organocatalytic conversions.
将2-硝基酰基苯直接氢化为2,1-苯并异恶唑在制药和精细化工行业中是一项重大挑战。在本研究中，采用缺陷工程策略，通过将铂单原子锚定在MgO(Al)纳米片内的金属空位上，制备双功能单原子催化剂（SACs）。所得的Pt/MgO(Al) SAC在2-硝基酰基苯的氢化环化反应中表现出优异的催化活性和选择性，在温和条件下完全转化时产率达到97.5%，周转频率高达458.8 h，创历史记录。独特的Pt-O-Mg/Al部分中完全暴露的单原子铂位点与MgO(Al)载体丰富的碱性位点之间的协同催化作用是这种出色催化性能的原因。因此，目前的工作为开发能够提高有机催化转化效率的双功能或多功能SACs铺平了道路。
