Optimizing CuNi catalysts for long-term vapor phase hydrogenation of levulinic acid to γ-valerolactone: Influence of the support on activity and stability

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2025-03-25 Epub Date: 2025-01-27 DOI:10.1016/j.apcata.2025.120140

Eliana Quiroga , Bernay Cifuentes , Santiago Yara , Julia Moltó , Martha Cobo

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Abstract

The conversion of biomass-derived levulinic acid (LA) to γ-valerolactone (GVL) is crucial for sustainable chemical and fuel production. This study evaluates the vapor phase hydrogenation of LA using Cu-Ni bimetallic catalysts supported on various metal oxides and their impact on the pathways of LA conversion. Specifically, we examine the influence of AlO₂, SiO₂, ZrO₂-SiO₂, and CeO₂-SiO₂ on catalyst performance and stability. Cu-Ni catalysts supported on SiO₂ modified with citric acid (SiO_2-CA) exhibited superior stability, while the one supported on Al₂O₃ showed higher activity. The enhanced performance of the SiO_2-CA-supported catalyst is attributed to its moderate acidity (379.3 µmol/g_cat) and resistance to sintering. Stability tests reveal that although both CuNi/Al₂O₃ and CuNi/SiO_2-CA catalysts deactivate over time, the latter demonstrates slower deactivation and better reactivation potential, maintaining conversion close to 80 % for 42 h. The study highlights the role of support in optimizing catalytic performance for LA hydrogenation.

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乙酰丙酸长期气相加氢制γ-戊内酯的CuNi催化剂优化：载体对活性和稳定性的影响

生物质衍生乙酰丙酸（LA）转化为γ-戊内酯（GVL）对可持续化工和燃料生产至关重要。研究了不同金属氧化物负载Cu-Ni双金属催化剂对LA气相加氢反应的影响。具体来说，我们考察了AlO2、SiO2、ZrO2-SiO2和CeO2-SiO2对催化剂性能和稳定性的影响。柠檬酸修饰的SiO2 （SiO2- ca）负载Cu-Ni催化剂表现出较好的稳定性，Al2O3负载Cu-Ni催化剂表现出较高的活性。sio2 - ca负载型催化剂的酸性适中（379.3µmol/gcat），耐烧结性能显著提高。稳定性测试表明，尽管CuNi/Al2O3和CuNi/SiO2-CA催化剂都随着时间的推移而失活，但后者表现出较慢的失活和更好的再活化潜力，在42 h内保持接近80% %的转化率。该研究强调了载体在优化LA加氢催化性能中的作用。

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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.