腺嘌呤改性 Pd/Co-MOFs 催化剂在喹啉加氢反应中实现大幅活性提升

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-11-22 DOI:10.1007/s10562-024-04861-1
Lu Yang, Tao Yuan, Haoyi Xu, Tingling Li, Wei Xiong, Derong Liu
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引用次数: 0

摘要

喹啉的化学选择性氢化反应是一个关键反应,可产生高价值的化学中间体,如药品、杀虫剂和染料。由于喹啉具有稳定的π-共轭结构,用于该反应的传统异相催化剂通常需要更高更严格的反应条件。要实现这种转化,必须开发一些创新策略来增强传统催化剂的催化特性。本研究采用腺嘌呤作为新型结构修饰剂,对 Co-MOFs 材料进行修饰,制备出 Pd/Co-MOFs(A)催化剂。腺嘌呤的引入有效提高了原始钯/Co-MOFs 催化剂的结构稳定性和催化效率。与未改性催化剂相比,催化转化率大幅提高了约 441%。催化性能的大幅提高可归因于传质的增强。N 杂环共轭结构促进了催化剂与喹啉之间的 π-π 堆积相互作用和氢键作用,从而加速了传质,提高了催化效率。在温和的反应条件下,Pd/Co-MOFs(A) 催化剂充分展示了其高催化性能,喹啉转化率达到 99.0%,对 1,2,3,4-四氢喹啉的选择性达到 99.9%。最后,本研究提出的 Pd/Co-MOFs(A)催化剂可以为通过生物碱改性提高传统异相催化剂在喹啉加氢反应中的催化性能铺平道路。 图文摘要
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Achieving a Large Reactivity Activity Improvement in Adenine Modified Pd/Co-MOFs Catalyst for Quinoline Hydrogenation

The chemo-selective hydrogenation of quinoline is a critical reaction, producing high-value chemical intermediates such as pharmaceuticals, pesticides, and dyes. Traditional heterogeneous catalysts for this reaction typically require higher and more stringent reaction conditions due to the stable π-conjugated structure of quinoline. To achieve this transformation, some innovative strategies must be developed to enhance the catalytic properties of conventional catalysts. In this work, adenine was employed as a novel structural modifier to finish Co-MOFs materials and prepare Pd/Co-MOFs(A) catalysts. The introduction of adenine efficiently enhanced structural stability and catalytic efficiency of original Pd/Co-MOFs catalyst. A remarkable increase of approximately 441% in catalytic conversion was obtained compared to the unmodified catalyst. This substantial improvement in catalytic performance could be attributed to mass transfer enhancement. The N-heterocyclic conjugated structure facilitated π–π stacking interactions and hydrogen bonding between the catalyst and quinoline, thereby accelerating mass transfer and improving catalytic efficiency. Under mild reaction conditions, the Pd/Co-MOFs(A) catalyst fully demonstrated its high catalytic performance, achieving a 99.0% quinoline conversion and a 99.9% selectivity toward 1,2,3,4-tetrahydroquinoline. Finally, the Pd/Co-MOFs(A) catalyst presented in this study could pave the way for enhancing the catalytic performance of traditional heterogeneous catalysts through alkaloid modification in quinoline hydrogenation.

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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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