Anchoring Pt Single-Atom Sites on Vacancies of MgO(Al) Nanosheets as Bifunctional Catalysts to Accelerate Hydrogenation-Cyclization Cascade Reactions

IF 3.7 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Chemistry - A European Journal Pub Date : 2024-09-06 DOI:10.1002/chem.202402757

Deqiong Xie, Ruifang Xue, Kecan Dou, Yaping Song, Yanghe Fu, Fumin Zhang, De-Li Chen, Weidong Zhu

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Abstract

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 Pt₁/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⁻¹ 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.

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在氧化镁（铝）纳米片空位上锚定铂单原子位点作为双功能催化剂加速氢化-环化级联反应

将 2-硝基苯直接氢化为 2,1-苯并异噁唑是制药和精细化工行业面临的一项重大挑战。本研究采用缺陷工程策略，将铂单原子锚定到氧化镁（铝）纳米片的金属空位上，从而制造出双功能单原子催化剂（SAC）。由此产生的 Pt1/MgO(Al)SAC在 2-硝基酰基苯的氢化-环化反应中表现出了卓越的催化活性和选择性，在温和条件下，完全转化产率达到 97.5%，转化频率达到破纪录的 458.8 h-1。独特的 Pt-O-Mg/Al 分子中完全暴露的单原子铂位点与 MgO(Al) 支持物中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，目前的研究工作为开发可提高有机催化转化效率的双功能或多功能 SAC 铺平了道路。

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来源期刊

Chemistry - A European Journal 化学-化学综合

CiteScore

7.90

自引率

4.70%

发文量

1808

审稿时长

1.8 months

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