低负载Pd(PVA)/沸石催化剂中金属和酸位协同糠醛加氢作用的具体见解

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-09-28 DOI:10.1016/j.apcata.2025.120612

Sara Morandi , Maria Pinto , Ilaria Barlocco , Silvio Bellomi , Alberto Villa , Maela Manzoli

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引用次数: 0

摘要

在糠醛加氢过程中，证实了沸石催化剂负载聚乙烯醇（PVA）与钯胶体中金属和酸位的协同作用。采用PVA溶胶固定化法制备了Pd纳米颗粒，并将其沉积在不同孔径（Y、ZSM-5和FER）和相似Si/Al比的沸石上，研究了可达Brønsted和Lewis酸位点的数量与催化活性和选择性的关系。在50℃条件下的催化实验表明，Pd/Y是最活跃的催化剂，在120 min后转化率达到95.0 %。钯的存在对糠醛转化至关重要，在相同条件下裸沸石表现出最低的活性。产物分布随沸石类型的不同而不同，Pd/Y催化剂在120 min后生成以四氢糠醇（THFA）和乙酰丙酸异丙酯（ILE）为主要产物的复杂混合物，其他催化剂主要生成糠基异丙醚（FIE）。FESEM-EDS， TEM， XPS和FT-IR测试表明，Pd/Y催化剂与其他催化剂最显著的区别是其Lewis酸位点的数量要高得多。这意味着Pd和Lewis酸度之间的协同作用是通过H2分裂和双键活化获得THFA和ILE的关键因素。

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Specific insights on the synergistic role of metal and acid sites of low loading Pd(PVA)/zeolite catalysts for furfural hydrogenation

The synergistic role of metal and acid sites in Pd colloids with polyvinyl alcohol (PVA) supported on zeolite catalysts was proved in furfural hydrogenation. Pd nanoparticles were prepared using PVA sol-immobilization and deposited on zeolites with different pore size (Y, ZSM-5 and FER) and similar Si/Al ratio to correlate the amount of accessible Brønsted and Lewis acid sites with catalytic activity and selectivity. Catalytic tests at 50 °C showed that Pd/Y is the most active catalyst, achieving 95.0 % conversion after 120 min. The presence of Pd is essential for furfural conversion, with bare zeolites showing minimal activity under the same conditions. Product distribution varies with the type of zeolite, with Pd/Y producing a complex mix including tetrahydrofurfuryl alcohol (THFA) and isopropyl levulinate ester (ILE) as the main product after 120 min, while other catalysts mainly form furfuryl isopropyl ether (FIE). FESEM-EDS, TEM, XPS and FT-IR measurements revealed that the most marked difference between Pd/Y and the other catalysts is the much higher amount of Lewis acid sites. This means that the synergistic effect between Pd and Lewis acidity is the key factor for obtaining THFA and ILE through H₂ splitting and double bond activation.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.