用于喹啉选择性加氢的页硅酸铜纳米催化剂,ACS Applied Nano Materials

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用于喹啉选择性加氢的页硅酸铜纳米催化剂
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-08-10 , DOI: 10.1021/acsanm.3c02180
Xiaodi Ma _{1,

2} , Guan Huang _{1,

2} , Zhichao Sun _{1,

2} , Ying-Ya Liu _{1,

2} , Yao Wang ₁ , Anjie Wang _{1,

2}

Affiliation

1,2,3,4-四氢喹啉（py-THQ）是用于生产医药、农药和其他精细化学品的重要中间体，通过喹啉选择性加氢合成。在这项工作中，页硅酸铜催化剂通过四种不同的合成方法制备：沉积沉淀法、氨蒸发法、尿素辅助凝胶法和水热处理法。研究发现，不同的合成策略导致前体中铜的实际负载量不同。最佳催化剂在100℃和3.0MPa H ₂下2小时内将喹啉完全转化为乙醇时，py-THQ选择性为99.9%。性能的显着提高可能归因于粒径小、Cu ^0的共存和Cu ⁺，以及通过沉积沉淀法制备层状硅酸铜的强相互作用。表征结果表明，Cu ⁰和Cu ⁺是在修复过程中生成的，分别来源于CuO和层状页硅酸盐。另外，Cu ⁺ /(Cu ⁺ + Cu ⁰ )之比随还原温度的变化而变化。这项工作中开发的催化剂设计和合成策略在其他氮杂环加氢反应中具有潜在的应用。

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Nanocatalysts Derived from Copper Phyllosilicate for Selective Hydrogenation of Quinoline

1,2,3,4-Tetrahydroquinoline (py-THQ) is a vital intermediate that is used in the production of medicines, agricultural chemicals, and other fine chemicals and is synthesized through the selective hydrogenation of quinoline. In this work, copper phyllosilicate catalysts were prepared by four different synthesis methods: deposition precipitation, ammonia evaporation, a urea-assisted gel method, and hydrothermal treatment. It was found that the different synthesis strategies led to different actual loadings of copper in the precursors. The optimal catalyst showed a py-THQ selectivity of 99.9% at a full conversion of quinoline in ethanol at 100 °C and 3.0 MPa H₂ for 2 h. The remarkable enhancement of the performance may be attributed to the small particle size, the coexistence of Cu⁰ and Cu⁺, and the strong interaction of copper phyllosilicate by the deposition precipitation preparation method. The characterization results showed that Cu⁰ and Cu⁺ were generated during the restoration process and were derived from CuO and layered copper phyllosilicates, respectively. Additionally, the ratio of Cu⁺/(Cu⁺ + Cu⁰) changed with the reduction temperature. The strategy of the catalyst design and synthesis developed in this work has potential applications in other nitrogen heterocyclic hydrogenation reactions.

更新日期：2023-08-10

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